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Marvin S. ANTELMAN
TetraSilver-TetraOxide vs. Cancer
Compassion-response.net Articles
Marantech: Technical Explanation of "Electron
Jumping Compounds" (EJC)
Marvin S. Antelman: US Patent # 5,336,499 ~ "Molecular
Crystal Device for Pharmaceuticals"
M. Antelman: US Patent # 5,676,977 ~ "Method
of Curing AIDS with Tetrasilver Tetroxide Molecular Crystal Devices"
M. Antelman: US Patent # 5,571,520 ~ "Molecular
Crystal Redox Device for Pharmaceuticals"
M. Antelman: US Patent # 5,223,149 ~ "Trivalent
Silver Water Treatment Compositions"
M. Antelman: US Patent # 5,211,855 ~ "Method
of Treating Water Employing Tetrasilver Tetroxide Crystals"
M. Antelman: US Patent # 6,485,755 ~ "Methods
of Using Electron Active Compounds for Managing Cancer"
M. Antelman: US Patent # 5,098,582 ~ "Divalent
Silver Oxide Bactericides" (Abstract)
M. Antelman: US Patent # 5,571,520 ~ "Molecular
Crystal Redox Device for Pharmaceuticals" (Abstract)
M. Antelman: US Patent # 6,258,385 ~ "Tetrasilver
Tetroxide Treatment for Skin Conditions" (Abstract)
M. Antelman: US Patent # 5,089,275 ~ "Stabilized
Divalent Silver Bactericides" (Abstract)
M. Antelman: US Patent # 5,078,902 ~ "Divalent
Silver Halide Bactericide" (Abstract)
M. Antelman: US Patent # 5,073,382 ~ "Divalent
Silver Alkaline Bactericide Compositions" (Abstract)
Robert Hammer/Jacob Kleinberg: Inorganic
Syntheses IV: 12 ~ Preparation of Silver (II) Oxide
Marantech website: http://www.Marantech.com
Compassion-Response.net ~ http://www.compassion-response.net/08Treatments/05Imusil.htm
"US Patent Claiming CURE for AIDS (USP # 5,676,977)"
In October 1977, the United States patented a "method for curing AIDS',
US Patent # 5,676,977. The product is called TETRASIL/IMUSIL and is a one-time
injection/infusion that eliminates bacterial pathogens in the blood system
of an individual. It is this cheap and effective cure for AIDS that is
the subject of my presentation.
As a 29-month recipient of this one time injection, I further submit
that we have an effective and cheap remedy for AIDS that is ready now.
Our goal in bringing this information to the international community is
to serve as aconduit for the necessary global "double blind" efficacy clinical
trials of this U.S. patented CURE for AIDS.
...Marantech has identified a number of Electron Jumping Compounds (EJCs)
that have been found in independent laboratory testing to exhibit
antimicrobial activity. However, to date the bulk of Company testing
of EJCs for pharmacological safety and efficacy has centred on tetrasilver
tetroxide, a multivalent metal oxide also known as Tetrasil..
Independent laboratory and clinical testing indicates that Tetrasil
molecules selectively target and kill rapidly proliferating organisms (e.g.,
cancer cells and pathogenic micro-organisms) through a multitude of nano-level
electrical discharges followed by physical combination (chelation), while
leaving normal tissues generally unaffected. The unusual suspected kill
method may thwart the development of pathogens resistant to Tetrasil therapy.
Antimicrobial Activity: It has been known for several years that Tetrasil
is a potent antimicrobial agent that kills a broad spectrum of viruses,
fungi, algae and bacteria (including drug resistant strains) in vitro at
concentrations that have been certified safe by the EPA for usage in swimming
pools ("EPA Levels").
Recent clinical studies commissioned by Marantech and conducted by Exetec
Labs in Honduras, indicate that topically applied Tetrasil can
lead to dramatic improvements in such infection-caused skin conditions
as acne, cold sores, herpes lesions, conjunctivitis, chickenpox,
shingles, dermal tuberculosis and ringworm.
Moreover, building on earlier informal testing against systemic infections
(including Candida albicans, dysentery and AIDS), Exetec has
been commissioned to conduct clinical studies of Tetrasil as an intravenous
treatment for AIDS and tuberculosis.
One may contact Dr. Antelman through the Weizmann Institute in Israel
or through Antelman Technologies, POB 382, Rehovat, Israel. Email contact:
impy@netvision.net.il
For information about Tetrasil and Imusil, you are invited to look up
the Marantech website at http://www.Marantech.com
Marantech is the company presently supplying Imusil.
Marantech contact information:
Marantech Holding, LLC, One Turks Head Place Suite 810, Providence,
RI 02903, USA. Tel: (401) 223-3000 Fax: (401) 223-7000
http://www.compassion-response.net/15Promotional%20Articles/Magazine%20article%203pp.htm
Compassion Response Network developed action projects in both Kinshasa
and Harare. In all, once adequately funded, the projects would treat 43
advanced AIDS patients over six months, each patient being on one of
nine alternative treatments for HIV/AIDS;
Zapper + colloidal silver + ozonated water, Dr Bob Beck treatment, Tetrasil/Imusil,
Essiac formula, Flor Essence, Aurea Cento Spice Oils, Glyco-nutritional
supplements, Absolutely pure colloidal silver + Oxyrich, Sutherlandia herb.
Each of these treatments has impressive claims for treating HIV/AIDS,
but we remain impartial and detached from those claims.
Our task is to provide an independent comparative assessment of many
alternative treatments for HIV/AIDS, something we believe had never been
done before. A daily nutritious meal would be provided to each of the
patients (for otherwise many were so poor that once they were half better
they would need to go and look for work simply to eat.)
The treatments were donated or provided for free, and the networking
facilitators within Compassion Response Network serve on a voluntary
basis. However conditions in Africa are difficult and to do things
properly various expenses would arise, food, transport, wages for cooks
and staff to provide treatments, comprehensive blood testing every
two months of treatment and miscellaneous costs.
Blood tests would involve state of the art medical tests; bDNA viral
load, CD4 immunity tests, full blood count and several other tests
pre-treatment and at every 2-month stage of the 6 months of treatment.
Marantech: Technical Description of "Electron Jumping
Compounds" (EJC)
http://www.Marantech.com
Electron-Jumping Compounds® (EJCs) represent
a class of multivalent metallic oxides that function as electron-firing
molecular-scale nano devices.
To date, the company has identified eight EJCs and widely
patented their potential market applications. Each EJC is based on a different
metallic oxide, including silver, iron, manganese, cobalt, praseodymium,
terbium, copper and bismuth.
EJCs have a natural attraction to specific biochemical
functional groups of the elements sulfur, nitrogen and phosphorous, one
of which is expressed by certain proteins on the membrane surface of cancer
cells and all rapidly proliferating pathogens (bacteria, fungi, viruses,
and protozoa).
Upon contact, a multi-stage chemical reaction is triggered:
Covalent bonding with the target
Release of electrical energy (nano-electrocution) through
a reduction/oxidation process
Release of highly active singlet oxygen.
This action effectively ensures the target’s death. No
other drug or anti-microbial functions in this way. The unique method of
action of the Company’s compounds has the potential to establish a new
class of medicine.
US Patent # 5,336,499
August 9, 1994 ~ Cl. 424/618
Molecular Crystal Device for Pharmaceuticals
Marvin S. Antelman
Abstract ~
A novel molecular scale device is described which is bactericidal, fungicidal,
viricidal and algicidal. The anti-pathogenic properties of the device are
attributed to electron activity indigenous to diamagnetic semiconducting
crystals of tetrasilver tetroxide ( Ag4O4 ) which
contains two monovalent and two trivalent silver ions in each molecular
crystal. When the crystals are activated with an oxidizing agent, they
release electrons equivalent to 6.4 x 10-19 watts per molecule
which in effect electrocute pathogens. A multitude of these devices are
effective at such low concentrations as 0.3 PPM used as preservatives in
a variety of formulations ranging from cosmetics to pharmaceuticals. Indeed,
they are intended as active ingredients for pharmaceuticals formulated
to destroy such pathogens as Staphylococcus aureus, and epidermidis, the
latter of which it completely destroys in a nutrient broth culture of about
1 million organisms at 0.6 PPM, or Candida albercans, the vaginal yeast
infection at 2.5 PPM, and the AIDS virus at 18 PPM.
References Cited ~
U.S. Patent Documents:
4695353
~
Sep., 1987 ~ Jansen, et al. ~ 423/604
4717562~
Jan., 1988~ Jansen, et al. ~ 423/604
4835077~
May, 1989~ Megahed et al. ~ 423/604
5017295~
May, 1991~ Antelman ~ 424/618
5073382~
Dec., 1991~ Antelman ~ 424/601
5078902~
Jan., 1992~ Antelman ~ 424/601
5089248~
Feb., 1992~ Akhtar ~ 423/604
5089275~
Feb., 1992~ Antelman ~ 424/601
Primary Examiner: Page; Thurman K. ~ Assistant Examiner:
Hulina; Amy
Attorney, Agent or Firm: Salter & Michaelson
Claims ~
What is claimed is:
1. A method of inhibiting the growth of pathogens in pharmaceutical
and cosmetic products, said pathogens selected from the group consisting
of E. coli, Micrococcus Luteus, Staphylococcus aureus, Staphylococcus epidermidis,
Pseudomonas aeruginosa, Streptococcus pyogenes, Candida Albicans, and Saccharomycetpideae,
which comprises introducing molecular semiconductor crystal devices of
the molecule tetrasilver tetroxide ( Ag4O4 ) in the
presence of an oxidizing agent comprising a persulfate.
Description ~
BACKGROUND OF THE INVENTION
The present invention relates to the employment of molecular crystals
as bactericidal, viricidal and algicidal devices, but more particularly
to the molecular semiconductor crystal tetrasilver tetroxide Ag.sub.4 O.sub.4
which has two trivalent and two monovalent silver atoms per molecule, and
which through this structural configuration enables electronic activity
on a molecular scale capable of killing algae and bacteria via the same
mechanism as macroscale electron generators. The concept of molecular scale
semiconductor devices for the storage of information has been the subject
of much activity in recent years so that the concept of a molecular scale
device performing such functions as storing information or acting as resistors,
capacitors or photovoltaic devices is well accepted. The molecular device
of this invention is a multivalent silver diamagnetic semiconductor. Now
the bactericidal activity of soluble divalent silver (Ag II) complex bactericides
is the subject of U.S. Pat. No. 5,017,285 of the present inventor. The
inventor has also been granted U.S. Pat. Nos. 5,078,902, USP # 5,073,382,
USP # 5,089,275, and USP # 5,098,582, which all deal with Ag II bactericides
but more particularly with (respectively) halides, alkaline pH, stabilized
complexes and the divalent oxide. It is the last patent, i.e., U.S. Pat.
No. 5,098,582, and its perfection that has led to my original concept of
the molecular device of the present invention. Now said patent designated
AgO as divalent silver oxide, the popular name of the compound. Indeed,
the Merck Index (11th Edition) designates the oxide as silver(II) oxide
(AgO) (entry 8469). However, it also states that it is actually a silver(I)-silver(III)
oxide with a molecular weight of 123.88. Said oxide is actually on a molecular
level Ag4O4 where one pair of silver ions in the
molecule is trivalent and another pair is monovalent.
While the formula AgO accurately designates the silver:oxygen ratio,
the molecular weight of the compound is actually 495.52. Further elucidation
of the molecule's electromagnetic properties reveals that it is a diamagnetic
semiconductor. The structure is electronically active because of the trivalent
sp.sup.2 electron configuration disparity of the electrons within the crystal.
Further testing of the unique oxide was continued on various types of
bacteria, molds, yeasts and algae, beyond the water treatment applications
claimed in my previous patents. The phenomenal efficacy of said oxide against
pathogens while they were in constant contact with their nutrient source
in contradistinction to its efficacy with these same organisms in water,
where the pathogen is separated from a constant nutrient source, could
only be accounted for by considering each molecule of oxide as a "device".
This in turn has led to the final development of this invention, namely,
a molecular device for killing viruses, fungi, algae and bacteria, which
can be utilized as the active component of pharmaceuticals and as a preservative
against said pathogens in pharmaceutical and other products.
OBJECTS OF THE INVENTION
The main object of this invention is to provide for a molecular scale
device of a single tetrasilver tetroxide semiconductor crystal capable
of killing viruses, bacteria, fungi and algae when operating in conjunction
with other such devices.
Another object of the invention is to provide for a molecular device
which can be utilized in pharmaceuticals formulated to destroy pathogens.
Still another object of the invention is as a preservative in pharmaceutical,
cosmetic, and related chemical specialty products against said pathogens.
Other objects and features of the present invention will become apparent
to those skilled in the art when the present invention is considered in
view of the accompanying examples. It should, of course, be recognized
that the accompanying examples illustrate preferred embodiments of the
present invention and are not intended as a means of defining the limits
and scope of the present invention.
SUMMARY OF THE INVENTION
This invention relates to a molecular scale device capable of destroying
gram positive and gram negative bacteria as well as fungi, viruses and
algae. Said molecular scale device consists of a single crystal of tetrasilver
tetroxide. Several hundred thousand trillion of these devices may be employed
in concert for their bactericidal, fungicidal, and algicidal properties
and applied to industrial cooling towers, swimming pools, hot tubs, municipal
water supplies and various pharmaceutical formulations.
The molecular crystals which are the subject of this invention are commercially
available and can be prepared by reacting silver nitrate with sodium or
potassium peroxydisulfate according to the following equation: 4AgNO3
+2Na2S2O8 + 8NaOH = Ag4O4
+ 4Na2SO4 + 4NaNO3 + 4H2O The
oxide lattice represented by the formula Ag4O4 is
depicted in the Drawing FIG. 1. It is a semiconducting electron active
diamagnetic crystal containing two monovalent and two trivalent silver
ions in combination with four oxygen atoms. The distance between the Ag(III)-O
Ag(I)O units equals 2.1 A. Ag(III)-Ag(III) = Ag(I)-Ag(I) = 3.28A and Ag(I)-Ag(III)
= 3.39 A. Each trivalent silver ion is coordinated via dsp2
electron bonds to 4 oxygen atoms. The depiction of this lattice is based
on several literature references relating to crystallographic studies.
Exemplary of this literature are J. A. McMillan's studies appearing in
Inorganic
Chemistry 13,28 (1960); Nature vol. 195 No. 4841 (1962), and
Chemical
Reviews 1962, 62, 65. Alvin J. Salkind elucidated studies involving
neutron diffraction with his coworkers (J. Ricerca Sci. 30, 1034
1960) proving the Ag(III)/Ag(I) nature of this molecule and states in his
classic entitled Alkaline Storage Batteries (Wiley 1969), coauthored
with S. Uno Falk, that the formula is depicted by Ag4O4
(page 156).
That same year a scientific communication appeared in Inorganic Nuclear
Chemistry Letters (5,337) authored by J. Servian and H. Buenafama which
maintained that their neutron diffraction studies also confirmed the tetroxide
lattice and the presence of Ag(III) and Ag(I) bonds in the lattice, a conclusion
also reported previously by Naray-Szahn and Argay as a result of their
x-ray diffraction studies (Acta Cryst. 1965, 19,180). Thus the effects
of this invention can be explained in terms of these structural elucidations,
namely, that the single molecular semiconductor crystal which inevitably
must be electronically active exchanging two electrons per crystals between
its mono and trivalent bonds is in reality a device which kills pathogens
in the same manner as electrically active large-scale devices utilized
in water supplies.
When the tetroxide crystals are utilized to destroy pathogens, they
will not do so unless activated by an oxidizing agent. This is analogous
to the behavior of single semiconducting photovoltaic molecular devices
such as copper indium selenide whose surfaces must be "etched" in order
to activate the photovoltaic activity, i.e., for light to facilitate the
release of electrons from the molecule. The tetroxide was activated by
persulfates. It was found that when the persulfates were tested as a control
by themselves, they failed to exhibit any unilateral antipathogenic activity
at the optimum level selected of 10 PPM. The persulfates evaluated varied
from Oxone (Registered Trademark Du Pont Company) brand potassium monopersulfate
to alkali peroxydisulfates.
DESCRIPTION OF THE DRAWING
In the drawing which illustrates the best mode presently contemplated
for carrying out the present invention:
FIG. 1 is a diagrammatic view showing the crystal lattice of Ag4O4
attacking a pathogenic bacillus.
DESCRIPTION OF THE INVENTION
Turning now to Drawing FIG. 1 depicting the crystal lattice of Ag4O4,
the device operates by transferring electrons from the monovalent silver
ions 10 to the trivalent silver ions 11 in the crystal 20 through the aqueous
media in which it is immersed and which conducts electrons depicted by
the path 12, contributing to the death of pathogen 13 with electrons 14,
traversing the cell membrane surface 15, said pathogen being "electrocuted"
by not only these electrons but by others: 16 and 17 following paths 18,
and 19 emanating from other molecular devices in the vicinity of the pathogen.
The device is attracted to the cell membrane surface 15 by powerful covalent
bonding forces 21 caused by the well-known affinity of silver to certain
elements present in the membrane, such as sulfur and nitrogen. Drawing
FIG. 1 exaggerates the size of the silver oxide molecular device with respect
to that of a microorganism for depiction purposes only.
The electron transfer can be depicted by the following half reactions
in which the monovalent silver ion loses an electron and the trivalent
silver gains one as follows:
Ag+ -e = Ag+2
Ag+3 +e = Ag+2
The molecular crystal then will become stabilized with each silver ion
having a divalent charge.
Stringent testing was performed in which cultures were actually placed
in trypticase soy nutrient broth, which allowed the pathogens being tested
to replicate without being detached from its own food supply. Under these
conditions the devices were able to kill two strains of E. Coli at 2.5
PPM; Micrococcus Luteus at 1.25 PPM; Staphylococcus aureus at 2.5 PPM;
Staphylococcus epidermidis at 0.6 PPM; Pseudomonas aeruginosa at 1.25 PPM;
and Streptococcus pyogenes at 2.5 PPM.
The devices were then evaluated in analogous nutrient used for yeasts,
algae and molds utilizing Sabouraud dextrose broth. The infectious yeast
pathogen Candida ALBICANS was totally killed at 2.5 PPM and that of the
Saccharomycetpideae variety at 1.25 PPM.
If we are to consider one molecular device in operation, then each molecule
would release two electrons having each a charge of 4.8 x 10-10
e.s.u. equivalent to approximately 1.6 x 10-19 coulombs. The
EMF given in my Encyclopedia of Chemical Electrode Potentials (Plenum
1982), page 88, for the oxidation of Ag(I) to Ag(II) is 1.98 volts which
approximates 2.0 V. The total power output per device can be calculated
in watts by multiplying the power output for each electron by 2. Since
power is the product of the potential times the charge, P = EI; for each
electron it would be
2.0 x 1.6 x 10-19 = 3.2 x 10-19 watts
From this, and using Avogadro's number, we can calculate that the power
flux of one liter of solution containing 0.5 PPM of devices would be 0.064
watts. Since the electronic charges of the devices are directly proportional
to the number of devices in solution, i.e., the concentration of the oxide
in the solution, we can arbitrarily assign our own device power flux constant
which can be used to gauge the concentrations of the devices required in
order to kill particular organisms in specific environments. I have found
the following formula useful for this purpose: Power Flux = EMF generated
per molecule x Concentration x 5 (the EMF being 4.0 volts per molecular
device; and the concentration is in PPM). Utilizing this formula, the power
flux to effectuate 100% kills for the following organisms is given in Table
I which follows.
TABLE I
______________________________________
Organism Name Power
Flux
______________________________________
Escherichia coli 50.0
Staphylococcus aureus
50.0
Streptococcus faecalis
50.0
Streptococcus pyogenes
50.0
Candida albicans 50.0
Pseudomonas aeruginosa
25.0
Micrococcus luteus 25.0
Staphylococcus epidermidis
12.5
______________________________________
EXAMPLE 1
The molecular crystal devices were tested as to whether they could kill
pathogenic microorganisms with the intent of utilizing them in pharmaceutical
applications. Once it could be determined that the devices inhibited a
particular microorganism, the minimal concentration required of the Ag.sub.4
O.sub.4 molecular crystal devices was determined to inhibit the microorganism
in nutrient broth. One family of pathogens that are known for their deleterious
effects on humans are popularly called "staph" infections. These infections
are commonly contracted in hospitals having lax infectious screening procedures.
Accordingly, three staph strains were selected as follows for evaluation:
Staphylococcus aureus 9027, 27543 and Staphylococcus epidermidis 12228.
The inoculum nutrient broth was prepared according to AOAC specifications
so as to contain 0.6-1 million organisms per drop of inoculum, each drop
being equal to 0.05 ml. The broth itself was trypticase soy broth BBL 11766
prepared according to label instructions. Accordingly, the broth was prestandardized
for the microorganisms in question in order to assure that the number of
organisms remained constant within the margins of statistical allowance
during the test period. Having carried out the procedures with 0.05 ml.
of inoculum and having incubated the organisms for 24 hours at 34.degree.-35.degree.
C., it was found that staph organism 9027 was inhibited at 2.5 PPM; number
27543 at 5.0 PPM; and the 12228 organism at 0.625 PPM all in the presence
of 10 PPM sodium persulfate. This data was utilized to formulate a dermatological
cream which would contain 100 PPM sodium persulfate and 10 PPM of device
crystals to inhibit staph infections. The data was also utilized to formulate
a surgical instrument sterilization formulation and a surgical scrub soap.
EXAMPLE 2
The procedures described in Example 1 were analogously followed for
the yeast pathogen Candida ALBICANS using strain 16464 excepting that the
nutrient broth was changed to accommodate this yeast pathogen to Sabouraud
dextrose broth (Difco 038217-9). It was found that 2.5 PPM of molecular
crystal devices completely inhibited the growth of this gynecological yeast
infection. A gynecological cream and a douche were formulated against yeasts
based on the results, as well as a cosmetic preservative.
EXAMPLE 3
The devices were tested against AIDS virus. The protocol used was that
of the Ministry of Health of the State of Israel at their Virology Laboratory
located at Tel HaShomer, Israel. AIDS viruses which had been grown in vitro
in a tissue culture were isolated and exposed to the devices at device
concentrations of 0.05, 1.0, 2.0, 3.0, 5.0 and 10.0 PPM. There was no evidence
of AIDS suppression at all until the concentrations reached 5.0 and 10.0
PPM. At 5.0 PPM, 60% of the viruses were killed. AT 10.0 PPM, 75% of the
viruses were killed. Extrapolation of this data reveals that at 18.0 PPM
there would be total suppression of the virus. These test results indicate
that the devices are capable of being used to destroy viruses in applications
involving the proliferation and transmittal of the AIDS virus outside of,
or for external application on, the human body as in cold sterilization,
or the active component of chemical specialty lubricants used in condoms.
While there is shown and described herein certain specific examples
embodying the invention, it will be manifest to those skilled in the art
that various modifications and rearrangements of the invention may be made
without departing from the spirit and scope of the underlying inventive
concept and that the same is not limited to the particular forms herein
shown and described except insofar as indicated by the scope of the appended
claims.
United States Patent 5,676,977
October 14, 1997 ~ Cl. 424/618
Method of Curing AIDS with Tetrasilver Tetroxide Molecular
Crystal Devices
Marvin S. Antelman
Abstract ~
The diamagnetic semiconducting molecular crystal tetrasilver tetroxide
( Ag4O4 ) is utilized for destroying the AIDS virus,
destroying AIDS synergistic pathogens and immunity suppressing moieties
(ISM) in humans. A single intravenous injection of the devices is all that
is required for efficacy at levels of about 40 PPM of human blood. The
device molecular crystal contains two mono and two trivalent silver ions
capable of "firing" electrons capable of electrocuting the AIDS virus,
pathogens and ISM. When administered into the bloodstream, the device electrons
will be triggered by pathogens, a proliferating virus and ISM, and when
fired will simultaneously trigger a redox chelation mechanism resulting
in divalent silver moieties which chelate and bind active sites of the
entities destroying them. The devices are completely non-toxic. However,
they put stress on the liver causing hepatomegaly, but there is no loss
of liver function.
References Cited ~
U.S. Patent Documents:
4415565
~ Nov., 1983 ~ Wysor ~ 424/618
4915955
~ Apr., 1990 ~ Gomori~ 424/618
4952411
~ Aug., 1990 ~ Fox, Jr. et al.~ 424/618
5073382
~ Dec., 1991 ~ Antelman~ 424/618
5078902
~ Jan., 1992 ~ Antelman ~ 424/618
5089275
~ Feb., 1992 ~ Antelman ~ 424/618
5211855
~ May, 1993 ~ Antelman ~ 424/618
5223149
~ Jun., 1993 ~ Antelman ~ 424/618
5336499
~ Aug., 1994 ~ Antelman ~ 424/618
5571520
~ Nov., 1996 ~ Antelman ~ 424/618
Other References ~
"Is The AIDS Virus A Science Fiction?" by Peter H. Duesberg and Bryan
J. Ellison: Policy Review (Summer 1990), pp. 40-51.
Claims ~
What is claimed is:
1. A method of treating AIDS-afflicted humans comprising injecting a
multitude of tetrasilver tetroxide molecular crystals into the bloodstream
of the human subject.
2. A method for increasing white blood cell counts in AIDS-afflicted
humans comprising injecting a multitude of tetrasilver tetroxide molecular
crystals into the bloodstream of the human subject.
3. Methods of treating AIDS-affilicted humans according to claims 1-2
where the concentration of said molecular crystals is approximately 40
PPM of the total blood weight of the human subject.
Description ~
BACKGROUND OF THE INVENTION
The present invention relates to the employment of molecular crystals
as anti-AIDS devices, but more particularly to the molecular crystal semiconductor
tetrasilver tetroxide Ag4O4 which has two monovalent
and two trivalent silver ions per molecule, and which through this structural
configuration enables intermolecular electron transfer capable of killing
viruses and binding them to the resulting silver entity so that a single
intravenous injection will completely obliterate acquired immune deficiency
syndrome (AIDS) in humans. Furthermore, said devices are capable of killing
pathogens and purging the bloodstream of immune suppressing moieties (ISM)
whether or not created by the AIDS virus (HIV); so as to restore the immune
system.
The present invention is based on concepts previously elucidated in
applicant's U.S. Pat. No. 5,336,499 which discloses the destruction and
inhibition of bacteria, algae and the AIDS virus in nutrient life supporting
systems by using said silver oxide devices. Example 3 of said patent discloses
that 18 PPM of said crystal devices could totally suppress the AIDS virus
(page 6, line 5). Subsequent to the filing of the aforementioned patent,
further testing revealed complete 100% destruction of the AIDS virus in
vitro at 20 PPM, and the fact that said devices were harmless when ingested
and inhaled, being non-toxic.
Encouraged by these evaluations and successes, applicant obtained permission
to evaluate the crystals in vitro against murine acquired immune deficiency
syndrome (MAIDS). Only one facility in the State of Israel is licensed
for these evaluations, namely, the Kaplan Hospital in Rehovot, Israel,
which is affiliated with the Hebrew University-Hadassah Medical School
where said evaluations were done.
The initial evaluations entailed experimenting with various silver moieties
cited in applicant's aforementioned patent, concentrations, non-reactive
buffers and modes of administration. After about 18 months of judicious
efforts and initial failures, success was finally achieved in destroying
the MAIDS virus in C57BL mice with a single intravenous injection. The
results of this test program comprise Example 5 of U.S. Pat. No. 5,336,499.
After success with mice, the inventor was able to test the efficacy of
said devices on two select etiological groups of terminal AIDS patients
in a clinic in Tegucigalpa, Honduras, Central America.
The AIDS patients comprised the etiological subgroups, Candidiasis and
Wasting Syndrome. Current indicator diseases for diagnosing AIDS which
have been expanded by the CDC, fall into the following five major categories
with the approximate percent distribution among AIDS patients:
______________________________________
1. P. carinii pneumonia
51%
2. Wasting syndrome
19%
3. Candidiasis 13%
4. Kaposi's sarcoma
11%
5. Dementia
6%
______________________________________
This invention concerns itself with the treatment and cure of candidiasis
and wasting syndrome AIDS patients with Tetrasil*. These two groups account
for approximately one third of AIDS cases.
*Trademark of Holipharm Corporation (of Israel) for Ag.sub.4 O.sub.4
Stedman's Medical Dictionary (Williams & Wilken's 26th Ed.,
1995) defines wasting syndrome "as a condition of 10% weight loss in conjunction
with diarrhea or fever . . . Associated with AIDS (p. 1744)."
OBJECTS OF THE INVENTION
The main object of the invention is to provide for a molecular scale
device of a single tetrasilver tetroxide crystalline molecule capable of
restoring the immunity of AIDS afflicted humans of the two AIDS etiological
subgroups, candidiasis and wasting syndrome.
Another object of the invention is to provide for immunity restoration
in said AIDS afflicted humans through a single injection.
Another object of this invention is to destroy ISM in humans manifesting
AIDS diseases of said AIDS etiological subgroups irrespective as to whether
said ISM was HIV induced, since it is known that humans may manifest AIDS
and still be HIV negative, and thus restore the immune system in said humans.
Another object of this invention is to destroy the AIDS virus when present
in the systems of said AIDS afflicted humans.
SUMMARY OF THE INVENTION
This invention relates to a molecular scale device not only capable
of destroying the AIDS virus, but of purging the human bloodstream of pathogens
and restoring immunity to AIDS patients of the candidiasis and wasting
syndrome categories. Said molecular device consists of a single crystal
of tetrasilver tetroxide (Ag4O4). The crystal lattice
of this molecule has a unique structure since it is a diamagnetic semiconducting
crystal containing two mono and two trivalent silver ions, which in effect
are capable of "firing" electrons under certain conditions which will destroy
AIDS viruses, other pathogens and immune suppressing moieties (ISM), not
only through the electrocution mode, but also by a binding process which
occurs simultaneously with electron firing, namely, binding and chelation
of divalent silver, i.e., the resulting product of the electron transfer
redox that occur when the monovalent silver ions are oxidized and the trivalent
ions are reduced in the crystal. The binding/chelation effect occurs at
active sites of the AIDS virus, pathogens and ISM. Because of the extremely
minute size of a single molecule of this crystal, several million of these
devices may be employed in concert to destroy a virus colony to purge a
life support system of ISM and pathogens with the consumption of only parts
per trillion of the crystal devices. Thus an optimum of 40 PPM of the devices
by weight of human blood was found to be sufficient to completely obliterate
AIDS. This concentration is slightly over double of the optimum concentration
recommended in applicant's aforementioned U.S. patent for the destruction
of the human AIDS virus in vitro. Other details concerning the structure
of the crystal and its mechanism against pathogens, the AIDS virus and
ISM would analogously hold here, and have already been further elucidated
in said patent.
The actual destruction of pathogens, ISM and the AIDS virus is effectuated
by injection of a suspension of these devices in distilled or deionized
water with a non-reacting electrolyte directly, i.e. intravenously, into
the bloodstream. A single injection is all that is required under these
conditions. Accordingly, humans injected in this manner, upon being inspected
after three weeks or more had elapsed and compared with similar humans
that had been given placebos, were completely cured of AIDS. The control
group still manifested AIDS. Accordingly, the tetrasilver tetroxide device
performed in concert with and in full conformity with the ultimate objects
of this invention. Furthermore, three out of four wasting syndrome terminal
patients and four out of the five candidiasis terminal patients were still
alive in 1995 after a year and a half had elapsed from their initial injection.
By that time all the AIDS patients had been released from the clinic and
allowed to return home.
Other objects and features of the present invention shall become apparent
to those skilled in the art when the present invention is considered in
view of the accompanying examples. It should, of course, be recognized
that the accompanying examples illustrate preferred embodiments of the
present invention and are not intended as a means of defining the limits
and scope of the present invention.
EXAMPLE 1
Five patients afflicted with AIDS of the candidiasis etiological category
were segregated for Tetrasil treatment. The rationale for selecting them
was based on facts presented in an article by Peter H. Duesberg and Brian
J. Ellison entitled "Is The AIDS Virus A Science Fiction?" (Policy Review,
Summer 1990 pp. 40-51). Only the factual presentations of the article were
utilized and the hypothesis of the authors was ignored. The facts presented
in the article related to the method of selecting AIDS patients based on
the five aforementioned etiological subgroups targeted by the CDC, and
the evidence presented, that there is AIDS without HIV as well as with
it so that an anti-viral agent in most instances will not necessarily restore
the immunity system.
Evaluations with Tetrasil were conducted on AIDS patients at Lucha Contra
el Sida, Comayaguela, Honduras. The patients two weeks prior to inoculation
were removed from their AZT, AIDS therapy. Tetrasil was administered at
approximately 40 PPM of blood volume per patient as a suspension in a proprietary
buffer solution (pH = 6.5), supplied by Holipharm Corporation.
The results of evaluations with candidiasis are tabulated in Table I
under its disease category. All patients evaluated were terminal. Some,
however, were in moderate (m) condition and others in poor (p) as designated
in the Table. The I and F designations refer to initial and final values
as shown. WBC indicates white cell blood count. The H column, following
CD 8, indicates whether hepatomegaly occurred. This was an unfortunate
consequence of the treatment which resulted in enlarged livers in all patients
except the second one. Despite hepatomegaly, there was no interference
with liver function.
The onset of hepatomegaly was not spontaneous and varied from patient
to patient, being in the range of 4-16 days.
It should also be noted that shortly after injection of Tetrasil there
were indications of fever (symbolized by T in the Ag4O4
column), sometimes accompanied by fatigue (F). The body temperature was
invariably 38.5.degree. C. (101.3.degree. F.). This was indicative of restoration
of the immune response of the body, since normally the body will destroy
pathogens when the immune system is functional by raising the temperature.
The patient who died; first responded favorably to Diflucan, which previously
gave no response. He was cured of his candidiasis, but unfortunately succumbed
to his previous body damage. All the other candidiasis syndrome people
who previously did not respond to the indicated medications subsequently
responded after the Tetrasil treatment. Further evidence of the recovery
of the AIDS patients manifested itself 30 days after the initial injection
when white blood cell counts were taken. They are shown in Table I under
the WBC column, which gives the initial and final WBC. All candidiasis
patients showed a dramatic increase in their white blood cell counts, indicative
of the restoration of their immunity systems.
EXAMPLE 2
The above protocol of Example 1 was repeated with AIDS patients exhibiting
wasting syndrome. The results of their treatment are tabulated in Table
I under the disease category of said syndrome. It should be noted that
two of the four wasting syndrome patients showed improved white blood counts.
The female patient, whose condition improved from poor and terminal to
be among the living, showed a decrease in the WBC. However, she showed
an increase in body temperature which was indicative of immune response.
The test results indicate that one cannot rely on a single factor to indicate
the demise of AIDS. The usual HIV marker CD 4 initial and final are irrelevant.
ISM suppression appears to be more critical than the destruction of HIV.
AIDS was suppressed, any permanent damage that had been done to the patients
in the course of their succumbing to AIDS was not obviously cured or corrected
by said crystal device treatment, rather said injury persisted and the
patient was improved with respect to AIDS but still suffered from said
permanent injury or impairment previously inflicted.
TABLE I
__________________________________________________________________________
Response of AIDS Patients to Single 40 PPM Ag4O4
Inoculation
Date
Weight
DISEASE
PATIENT
Inoc.
WBC CD 4 DEATH
Lbs.
Group Sex
Age
Medictn
1994
I F I F CD 8
H 1944
I F Ag4O4
__________________________________________________________________________
Candidiasis
M p
28 Diflucan
5/5
1,200
4,200
41
-- 221
+ 6/11
82 76
T
F m
33 " 5/5
6,000
6,700
554
872
394
- 98 98
T
F m
33 Ketaconzl
5/27
2,600
3,850
248
181
951
+ 123 123
T
M p
62 " 6/2
3,300
3,700
89
237
59
+ 105 92
F
F m
31 Pentamidn
6/2
2,400
3,050
9 181
65
+ 121 118
Pain
Wasting
M m
27 5/27
3,600
4,600
39
14
709
+ 119 120
T
Syndrome
M m
28 5/27
2,750
-- 10
-- 60
+ 7/19
121 119
T, F
F p
43 5/27
3,600
2,700
68
246
248
+ 101 98
T, F
M m
19 5/10
3,850
5,400
137
36
48
+ 103 106
T, F
_________________________________________________________________________
As this invention may be embodied in several forms without departing
from the spirit or essential characteristics thereof, the present embodiments
are therefore illustrative and not restrictive, since the scope of the
invention is defined by the appended claims rather than by the description
preceding them, and all changes that fall within the metes and bounds of
the claims or that form their functional as well as conjointly cooperative
equivalents, are therefore intended to be embraced by these claims.
US Patent # 5,571,520
Molecular Crystal Redox Device for Pharmaceuticals
( November 5, 1996 ~ Cl. 424/618 )
Marvin S. Antelman
Abstract ~
The employment of molecular crystals as bactericidal, viricidal and
algicidal devices, and specifically the molecular semiconductor crystal
tetrasilver tetroxide Ag4O4 which has two trivalent
and two monovalent silver atoms per molecule, and which through this structural
configuration generates electronic activity on a molecular scale capable
of killing algae and bacteria via the same mechanism as macroscale electron
generators.
References Cited ~
U.S. Patent Documents
4055655
~ Oct., 1977 ~ Maurer et al ~ 514/495
4695353
~ Sep., 1987 ~ Jansen et al. ~ 423/604
4717562
~ Jan., 1988 ~ Jansen et al.~ 423/604
4784991
~ Nov., 1988 ~ Nimrod et al. ~ 514/495
4835077
~ May., 1989 ~ Megahed et al. ~ 423/604
4915955
~ Apr., 1990 ~ Gomori ~ 424/618
4952411
~ Aug., 1990 ~ Fox, Jr. et al. ~ 424/618
5017295~
May., 1991 ~ Antelman ~ 210/764
5073382
~ Dec., 1991 ~ Antelman ~ 210/764
5078902
~ Jan., 1992 ~ Antelman ~ 210/764
5089248
~ Feb., 1992 ~ Akhtar ~ 423/604
5089275
~ Feb., 1992 ~ Antelman ~ 424/602
5098582
~ Mar., 1992 ~ Antelman ~ 210/759
5211855
~ May., 1993 ~ Antelman ~ 424/618
5223149
~ Jun., 1993 ~ Antelman ~ 424/618
5336508
~ Aug., 1994 ~ Marty ~ 424/618
5362735
~ Nov., 1994 ~ Luengo ~ 514/291
5444052
~ Aug., 1995 ~ Pieringer et al. ~ 514/738
Claims ~
What is claimed is:
1. A method for curing amoebic dysentery comprising, administering crystals
of tetrasilver tetroxide intravenously so as to give a concentration of
crystals of 40 PPM in the bloodstream.
2. A method for treating systemic Candida albicans; comprising injecting
tetrasilver tetroxide crystals into the blood of humans so as to give a
concentration of approximately 40 PPM in the bloodstream.
3. A method for treating Candida albicans according to claim 2 comprising
only one single administered injection.
Description ~
BACKGROUND OF THE INVENTION
The present invention relates to the employment of molecular crystals
as bactericidal, viricidal and algicidal devices, but more particularly
to the molecular semiconductor crystal tetrasilver tetroxide Ag4O4
which has two trivalent and two monovalent silver atoms per molecule, and
which through this structural configuration enables electronic activity
on a molecular scale capable of killing algae and bacteria via the same
mechanism as macroscale electron generators.
The molecular device of this invention is a multivalent silver diamagnetic
semiconductor as previously described in my aforesaid pending U.S. application
Ser. No. 07/971,933, now U.S. Pat. No. 5,336,499.
OBJECTS OF THE INVENTION
The main object of this invention is to provide a molecular scale redox
device of a single tetrasilver tetroxide semiconductor crystal capable
of killing viruses, bacteria, fungi and algae when operating in conjunction
with other such devices.
Another object of the invention is to provide a molecular device which
can be utilized in pharmaceuticals formulated to destroy pathogens.
Other objects and features of the present invention will become apparent
to those skilled in the art when the present invention is considered in
view of the accompanying examples. It should, of course, be recognized
that the accompanying examples illustrate preferred embodiments of the
present invention and are not intended as a means of defining the limits
and scope of the present invention.
SUMMARY OF THE INVENTION
This invention relates to a molecular scale device capable of destroying
gram positive and gram negative bacteria as well as fungi, viruses and
algae. Said molecular scale device consists of a single crystal of tetrasilver
tetroxide. Several hundred thousand trillion of these devices may be employed
in concert for their bactericidal, fungicidal, and algicidal properties
and in various pharmaceutical formulations and therapies. The physical
chemistry of said tetroxide devices has already been described in my aforesaid
pending application Ser. No. 07/971,933, now U.S. Pat. No. 5,336,499 and
is incorporated herein by reference.
DESCRIPTION OF THE INVENTION
The crystal lattice of the Ag4O4 device operates
by transferring electrons from its two monovalent silver ions to the two
trivalent silver ions in the crystal in aqueous media in which it is immersed,
and which conducts electrons, contributing to the death of pathogens by
traversing the cell membrane surface of the pathogens being "electrocuted",
not only by these electrons but also by others emanating from other molecular
devices in the vicinity of the pathogen. The device is attracted to the
cell membrane surface by powerful covalent bonding forces caused by the
well-known affinity of silver to certain elements present in the membrane,
such as sulfur and nitrogen.
The electron transfer can be depicted by the following redox half reactions
in which the monovalent silver ion loses an electron and the trivalent
silver gains one as follows:
Ag+ -e = Ag+2
Ag+3 +e = Ag+2
The molecular crystal then will become stabilized with each silver ion
having a divalent charge.
Stringent testing was performed in which cultures were actually placed
in trypticase soy nutrient broth, which allowed the pathogens being tested
to replicate without being detached from its own food supply. Under these
conditions the devices were able to kill two strains of E. coli at 2.5
PPM; Micrococcus luteus at 1.25 PPM; Staphylococcus aureus at 2.5 PPM;
Staphylococcus epidermidis at 0.6 PPM; Pseudomonas aeruginosa at 1.25 PPM;
and Streptococcus pyogenes at 2.5 PPM.
The devices were then evaluated in analogous nutrient used for yeasts,
algae and molds utilizing Sabouraud dextrose broth. The infectious yeast
pathogen Candida albicans was totally killed at 2.5 PPM and that of the
Saccharomycetpideae variety at 1.25 PPM. These were also evaluated successfully
in mice against murine aids, and in humans against Candida albicans both
as a douche and intravenously. The devices also were successful externally
in humans against Staphylcoccus epidermidis, nail fungus and athlete's
foot. Intravenous injections completely cured subjects who were suffering
from acute diarrhea of ameobic dysentery.
It was found that oxidizing agents, particularly persulfates, enhance
the efficacy of said devices.
EXAMPLE 1
The molecular crystal devices were tested as to whether they could kill
pathogenic microorganisms with the intent of utilizing them in pharmaceutical
applications. Once it could be determined that the devices inhibited a
particular microorganism, the minimal concentration required of the Ag4O4
molecular crystal devices was determined to inhibit the microorganism in
nutrient broth. One family of pathogens that are known for their deleterious
effects on humans are popularly called "staph" infections. These infections
are commonly contracted in hospitals having lax infectious screening procedures.
Accordingly, three staph strains were selected as follows for evaluation:
Staphylococcus aureus 9027, 27543 and Staphylococcus epidermidis 12228.
The inoculum nutrient broth was prepared according to AOAC specifications
so as to contain 0.6-1 million organisms per drop of inoculum, each drop
being equal to 0.05 ml. The broth itself was trypticase soy broth BBL 11766
prepared according to label instructions. Accordingly, the broth was prestandardized
for the microorganisms in question in order to assure that the number of
organisms remained constant within the margins of statistical allowance
during the test period. Having carried out the procedures with 0.05 ml.
of inoculum and having incubated the organisms for 24 hours at 34.degree.-35.degree.
C., it was found that staph organism 9027 was inhibited at 2.5 PPM; number
27543 at 5.0 PPM; and the 2228 organism at 0.625 PPM all in the presence
of 10 PPM sodium persulfate. This data was utilized to formulate a dermatological
cream which would contain 100 PPM sodium persulfate and 10 PPM of device
crystals to inhibit staph infections. The cream was applied to a "staph"
infection. The infection disappeared overnight. The subject was a 24-year
old female.
EXAMPLE 2
The procedures described in Example 1 were analogously followed for
the yeast pathogen Candida albicans using strain 16464 excepting that the
nutrient broth was changed to accommodate this yeast pathogen to Sabouraud
dextrose broth (Difco 038217-9). It was found that 2.5 PPM of molecular
crystal devices completely inhibited the growth of this gynecological yeast
infection. A gynecological cream and a douche were formulated against yeasts
based on the results. The douche which contained 10 PPM of crystals and
40 PPM sodium persulfate was self-administered by a woman in her thirties
who had suffered an entire year from the infection and who had taken virtually
every prescription medicine for the infection to no avail. After taking
two 2-quart douches within 24 hours, all signs of the candida infection
had disappeared and her doctor pronounced her completely cured.
EXAMPLE 3
Device crystals were administered intravenously into a person in such
a manner as to give a concentration of said tetroxide crystals of 40 PPM
in the bloodstream. The person was chronically ill from Candida albicans.
The subject, a citizen and resident of Honduras, was a 33-year old female.
She was completely cured within a month of taking the crystals intravenously.
It should be noted that the subject was close to death as a consequence
of exposure to the disease prior to the aforesaid treatment.
EXAMPLE 4
Two patients at the same clinic where Example 3 patient was treated,
in San Pedro Sultas, Honduras, were suffering from acute ameobic dysentery
with diarrhea and dehydration. They were similarly intravenously treated
to a level of 40 PPM of the crystals. Both patients, one a 19-year old
male, and the other a 62-year old male, after being given one injection
started to show slight improvement after one week. After one month had
elapsed, they were completely cured from their condition.
The human dosages of this and the previous example were known to be
safe as they were pretested in mice by injecting them with said crystal
devices.
EXAMPLE 5
Six C57BL mice were selected that were six months old. One mouse was
untreated as a control. Another control mouse was treated with an intravenous
injection via its tail with 0.1 ml. of tetrasilver tetroxide devices calculated
to contain 40 PPM in the bloodstream of the mouse. Two more control mice
were now infected with MAIDS virus designated culture LP-BM5. Two test
mice were then infected with culture LP-BM5. The LP-BM5 culture infection
was achieved with intra-peritoneal injections of 0.4 ml. of said viral
suspension. Subsequent to these vital injections the test mice were injected
intravenously with 0.1 ml. (through the tail) of the 40 PPM (0.08 mg.)
tetrasilver tetroxide devices. The devices in each case were suspended
in distilled water for 3 days prior to injection and conditioned with sodium
acetate as the electrolyte of choice. After 4 weeks had elapsed, the untreated
and device treated control mice were killed. The untreated control mouse
had a spleen weight of 90 mg., and the device treated mouse that of 89
mg. Both mice were seen to be in perfect health. After 3.5 weeks had elapsed,
one of the infected control mice was killed and showed signs of MAIDS infection
with a spleen weight of 138 mg. After 4 weeks had elapsed, the second infected
control mouse was killed. It too showed signs of MAIDS infection with a
spleen weight of 158 mg. As for the test mice, the vital suspension injection
was injected immediately prior to the silver device treatment. They were
then killed after 4 weeks. Both mice showed no signs of MAIDS infection,
and their spleens weighed 103 and 95 mg., respectively, which are normal
weights for these mice, whose body weight varies between 15-30 g. and whose
blood volume is approximately 2.0 ml.
EXAMPLE 6
A 29-year old male suffering from athlete's foot soaked his feet in
a solution containing 100 PPM of the crystal devices. The subject was completely
cured within 24 hours.
EXAMPLE 7
A 61-year old male who suffered from a toenail fungus was treated with
a 25% suspension of said crystal devices. The nail fungus, which had bothered
the subject for three years, was gone after a week.
While there is shown and described herein certain specific examples
embodying the invention, it will be manifest to those skilled in the art
that various modifications and rearrangements of the invention may be made
without departing from the spirit and scope of the underlying inventive
concept and that the same is not limited to the particular forms herein
shown and described except insofar as indicated by the scope of the appended
claims.
US Patent # 5,223,149
( June 29, 1993 ~ Cl. 210/764 )
Trivalent Silver Water Treatment Compositions
Marvin Antelman
Abstract ~
A method for controlling the growth of bacteria and algae in utilitarian
bodies of water such as industrial cooling towers, swimming pools and hot
tubs is described. The method comprises adding to the water novel trivalent
silver compounds. Said compounds are light stable and can be supplied as
liquid concentrates which will not precipitate any silver whatsoever from
saline waters nor will the concentrates stain skin or discolor surfaces.
Said compounds meet the rigid EPA standards of killing 100% of select coliforms
within ten minutes and are efficacious at concentrations as low as 1-2
PPM.
References Cited ~
U.S. Patent Documents
5073382
~ Dec., 1991 ~ Antelman ~ 210/764
5078902
~ Jan., 1992 ~ Antelman ~ 210/764
5089275
~ Feb., 1992 ~ Antelman ~ 210/764
5098582
~ Mar., 1992 ~ Antelman ~ 210/759
Claims ~
What is claimed is:
1. A method for limiting the growth of bacteria and algae in the water
of swimming pools, industrial cooling towers, hot tubs and reservoirs which
comprises adding to the water a stable trivalent silver compound.
2. The method as claimed in claim 1 wherein the trivalent silver compound
is a periodate.
3. The method as claimed in claim 1 wherein the said water is salt water,
and wherein no silver halide is caused to precipitate.
4. The method as claimed in claim 2 wherein the said water is salt water,
and wherein no silver halide is caused to precipitate.
5. The method as claimed in claim 1 wherein said trivalent silver compound
is supplied as a liquid concentrate.
6. The method as claimed in claim 2 where said trivalent silver periodate
is supplied as a liquid concentrate.
7. The method as claimed in claim 1 wherein said trivalent silver compound
is employed without adding an oxidizing agent.
8. The method as claimed in claim 2 wherein said trivalent silver periodate
is employed without adding an oxidizing agent.
9. The method as claimed in claim 1 where said trivalent silver compound
concentrate will not stain skin or surfaces with which it is in contact.
10. The method as claimed in claim 2 where said trivalent silver periodate
concentrate will not stain skin or surfaces with which it is in contact.
11. The method as claimed in claim 1 where said trivalent silver compound
is light stable so as not to discolor or leave black silver films on the
inner surface of vessels containing the water to be treated.
12. The method as claimed in claim 2 where said trivalent silver periodate
is light stable so as not to discolor or leave black silver films on the
inner surface of vessels containing the water to be treated.
Description ~
BACKGROUND OF THE INVENTION
The present invention relates to the employment of trivalent silver
(Ag[III]) compounds as bactericidal and algicidal agents in water treatment.
Water soluble trivalent silver compounds are part of the class of multivalent
silver compounds which have been the subject of patents granted to the
instant inventor for water treatment. To date five such patents have been
granted, namely, U.S. Pat. # 5,017,295; USP # 5,073,382; USP # 5,078,902;
USP # 5,089,275; and USP # 5,098,582. These patents all deal with divalent
silver compounds and compositions that are anti-pathogenic but more particularly
with (respectively) soluble complexes, alkaline pH stable compositions,
halides, solid stabilized complexes and solid black oxide. All of said
compounds more particularly related to treating utilitarian bodies of water
defined as bodies of water having an ultimate use such as swimming pools,
hot tubs, industrial cooling towers and municipal reservoirs where pathogens
are known to proliferate. While all of the cited patents describe multivalent
silver compounds which have many novel advantages in treating said bodies
of water and while they all conform to regulatory requirements for treating
said bodies of water, such as the rules and regulations of the Environmental
Protection Agency for treating swimming pools, none of the above inventions
provides for an antipathogenic composition which embodies all of the following
characteristics:
1. A liquid composition;
2. Not precipitated out by halides present in the water treated;
3. Non-staining in concentrated form to human skin and to the surfaces
of the containing vessel of said bodies of water.
None of the previously patented compounds or compositions met all of
these three criteria, despite the fact that each invention embodied unique
compositions of Ag(II) moieties. The first patent, for example, in its
preferred embodiments dealing with Ag(II) complexes, though of liquid composition,
stained the skin in concentrated form and precipitated cupious white material
when introduced into saline bodies of water. While of all the previous
patents the silver halides were free of this nuisance and were nonstaining,
they all were solid compositions which were totally insoluble in water.
Accordingly, a composition meeting these three criteria was sought. Therefore,
attempts were made to synthesize water soluble Ag(III) compounds, and testing
and evaluation of their efficacy to see whether they met all the aforementioned
criteria. The Ag(II) compositions were all light stable and it was verified
as anticipated for Ag(III) as well. Accordingly, the tests and evaluations
proved successful which has led to the final development of this invention,
namely, trivalent silver compositions capable of killing and/or preventing
the replication of gram positive and gram negative bacteria, as well as
algae in utilitarian water bodies, such as swimming pools, which can be
supplied in liquid concentrate form which will not stain the skin nor precipitate
in the presence of halides.
In the course of the testing of the compositions of this invention,
another previously unanticipated advantage of these compositions became
evident. Whereas all the previous Ag(II) compositions required additions
of oxidizing agents, such as alkali metal persulfates, to synergize their
efficacy, these compositions required no such additions and were efficacious
in themselves.
OBJECTS OF THE INVENTION
The main object of this invention is to provide compositions embodying
trivalent silver compounds capable of killing and/or inhibiting the growth
of bacteria and algae, particularly in utilitarian bodies of water when
said compositions are added to said water supply.
Another object of the invention is to provide a source of trivalent
silver ions capable of meeting the regular EPA standards for swimming pools
and hot tubs, mainly, a bactericide capable of achieving 100% kills within
ten minutes.
Still another object of the invention is to provide for a trivalent
silver composition which will perform the aforementioned anti-pathogenic
functions and will not be subject to the formation of a precipitate in
the presence of halides.
Still another object of the invention is to provide a trivalent silver
composition having all of the aforementioned functions and characteristics,
but which will not stain the skin nor discolor surfaces with which it is
in contact in its concentrated liquid form.
Still another object of the invention is to provide a trivalent silver
composition having all of the aforementioned functions, but which can be
formulated into a marketable concentrated liquid product for utilization
in utilitarian bodies of water.
Still another object of the invention is to provide a trivalent silver
composition having all of the aforementioned functions and characteristics,
but which can perform its anti-pathogenic functions without the need of
adding an oxidizing agent to the composition.
A final object of the invention is to provide a trivalent silver composition
having all of the aforementioned functions and characteristics, but which
is also light stable, unlike monovalent silver compounds.
Other objects, features, functions and characteristics of the present
invention will become apparent to those skilled in the art when the present
invention is considered in view of the accompanying examples. It should,
of course, be recognized that the accompanying examples illustrate preferred
embodiments of the present invention and are not intended as a means of
defining the limits and scope of the present invention.
SUMMARY OF THE INVENTION
This invention relates to the utilization of trivalent silver compounds
for bactericidal and algicidal applications in utilitarian bodies of water,
such as swimming pools, hot tubs, municipal and industrial water supplies,
as for example, cooling towers.
More particularly, this invention concerns stable Ag(III) complexes
designated by the principal quantum number, n = 4, and the second quantum
number l = 2, delineating sublevel d having eight electrons, the accepted
conventional expression being d8 complexes in contradistinction
to the d9 divalent complexes and d10 monovalent complexes
of silver.
Trivalent silver complexes were prepared by either reacting Ag(I-III)
tetrasilver tetroxide with a ligand bearing compound capable of forming
Ag(III) complexes or reacting an Ag(I) salt in the presence of said ligand
with an oxidizing agent, such as alkali persulfate, or in the alternative,
by reacting Ag(III) hydroxide complex formed electrolytically by the anodic
oxidation of silver in an alkali solution.
Said trivalent silver complexes were subsequently evaluated as to their
efficacy in killing gram positive and gram negative bacteria in algae in
accordance with the EPA protocols for swimming pools, which require 100%
kills of bacteria within ten minutes. The compounds far exceeded the bacteria
requirements at concentrations of one PPM or less of silver. They were
evaluated with and without persulfate salts at 10 PPM and were effective
without persulfates as bactericides.
The complexes were then evaluated with salt concentrations as high as
10% without precipitating halide.
The complexes, which were colored from deep orange to brown and maroon,
were left exposed in clear glass bottles for three months with constant
exposure to daylight. The complexes were stable and did not decompose to
silver.
Ag(III) complexes were applied to human skin in concentrated form containing
as much as 5,000 PPM silver without any silver staining of the skin whatsoever.
Of all the Ag(III) complexes prepared, the easiest to prepare were periodate
complexes. Accordingly, a particular Ag(III) periodate complex was selected
for evaluation against algae and it proved effective.
The particular Ag(III) periodate selected was prepared by the action
of potassium hydroxide on tetrasilver tetroxide (Ag4O4)
and is depicted by the following reaction:
Ag4O4 + 6KOH + 4KIO4 = 2K5H2
[Ag(IO6)2 ] + Ag2O + H2O
The Ag(III) periodate complexes can be depicted by the following structure:
[ ##STR1## ] Several Ag(III) periodates have been identified
which conform to this structure, in addition to the aforementioned one,
which was designated by Servian, J. and Buenafama, H.D., Inorganic Nuclear
Chemistry Letters. 1969, 5, 337-8. Another formula is:
K3H4 [Ag(IO6)2 ]
(Cohen, G. and Atkinson, G., Inorganic Chemistry 1964, 3, 2,
1741-2.)
DESCRIPTION OF THE PREFERRED EMBODIMENTS
As illustrative of the preferred embodiments of this invention are the
following examples.
EXAMPLE 1
An Ag(III) periodate was prepared by calculating the amounts of reactant
necessary to form the periodate complex according to the aforementioned
reaction equation involving KOH, 0.15 grams; tetrasilver tetroxide 1.0
gram and potassium periodate 2.0 grams. The KOH was first dissolved in
20 ml. of distilled water and the subsequent ingredients were added, and
the entire mixture was heated and kept at 65 degrees C. for two hours.
At the end of that time, the supernatant liquid, which had a rich orange-maroon
color, was separated and was filtered and submitted for analysis to an
independent laboratory, after it was diluted to a total volume of 100 ml.
in a volumetric flask. The resulting solution assayed 3290 mg./L Ag and
represented a 76% yield of Ag(III) periodate based on the aforementioned
reaction stoichiometry. Having evaluated the silver concentration via an
independent EPA certified laboratory, Ag(III) periodate aliquots were submitted
to another EPA certified laboratory for bactericidal evaluation of the
Ag(III) complex. Accordingly, good laboratory practice was followed in
accordance with FIFRA and ffdca/40 CFR 160, May 2, 1984. The bacteria employed
were E. coli, a gram negative pathogenic bacillus. The protocol employed
for the evaluations was that as set forth in AOAC (15th) 1990:965:13 at
colony densities of 100K/cc.,utilizing two exposure times, i.e., five and
ten minutes. Concentrations of Ag(III) evaluated were 0.5, 1.0 and 3.0
PPM. The evaluation pH was 7.5. Testing was done with controls and with
and without potassium persulfate at a concentration of 10 PPM. There was
100% inhibition of the colonies after ten minutes at all concentrations
and after five minutes except for the 0.5 PPM solution.
Having completed the aforementioned evaluations, another EPA certified
laboratory was chosen for more comprehensive testing according to the aforementioned
protocols excepting that sodium persulfate at 10 PPM was added to the Ag(III)
periodate and tested against said periodate at zero persulfate and testing
was also done on cultures of Streptococcus faecalis.
Here is a summary of the results in terms of the time required to give
100% kills of bacteria.
______________________________________
PERS Ag TIME
BACTERIA STRAIN (PPM)
(PPM) (MIN)
______________________________________
Strep. 6569
0.0 2.0 4.0
faecalis
10.0 2.0 0.5
0.0 1.0 5.0
10.0 1.0 2.0
E. coli 11229
0.0 2.0 2.0
10.0 2.0 0.5
0.0 1.0 5.0
10.0 1.0 2.0
______________________________________
EXAMPLE 2
An ATTC strain of Chorella was grown in nutrient Medium 866 broth under
the required lighting. When optimal growth was reached, the number of organisms
per ml. were determined by microscopic count and then subcultured. The
first Ag(III) periodate complex was applied to the algae at concentrations
of 2 PPM and 4 PPM. The algae were left in contact for one hour, one day
and ten days. The protocol for these tests involved procedures described
in the Water and Waste Water Manual of the United States Public Health
Service. The exposure tests involved post inoculation in order to determine
whether the compound was algicidal or algistatic. The Ag(III) periodate
complex was found to be algistatic at 2 PPM and algicidal at 4 PPM after
one hour's exposure. After one day and ten days, there were no positive
flasks at all. Ten flasks of subculture were utilized for each test.
EXAMPLE 3
Trivalent silver biguanide (Ag[III] bg) was prepared by modifying the
procedure of D. Sen described in the Journal of the Chemical Society
(A) 1969, p. 1304. Biguanide sulfate was stirred in suspension in distilled
water using 6 g./100 cc. of the compound (pH = 2.8-3.0). 5 g. of sodium
bicarbonate were added slowly to adjust the pH. The final pH was 7.7. Accordingly,
the pH adjustment resulted in a clear solution. 5 cc. of 10% silver nitrate
were then added to the clear solution followed by 20 cc. of a 5% sodium
persulfate solution. At the end of two hours, a beautiful precipitate of
maroon colored Ag(III) bg was obtained, which was decanted, purified and
separated. The resulting compound was then suspended in distilled water
and serially diluted with distilled water so as to give a resulting solution
which was 3 PPM in Ag(III). Sodium persulfate was then added to this solution
to give a final concentration of 10 PPM of persulfate. The resulting solution
was submitted to the same testing laboratory for the same type of E. coli
efficacy as described in Example 1. There was 100% inhibition of E. coli
within five minutes.
While there is shown and described herein certain specific examples
embodying the invention, it will be manifest to those skilled in the art
that various modifications and rearrangements of the invention may be made
without departing from the spirit and scope of the underlying inventive
concept and that the same is not limited to the particular forms herein
shown and described except insofar as indicated by the scope of the appended
claims.
US Patent # 5,211,855
Method of Treating Water Employing Tetrasilver Tetroxide
Crystals
May 18, 1993 ~ Cl. 210/758
Marvin Antelman
Abstract ~
A novel molecular scale device is described which is bactericidal, fungicidal
and algicidal. The antipathogenic properties of the device are attributed
to electron activity indigenous to diamagnetic semiconducting crystals
of tetrasilver tetroxide (Ag4O4) which contains two
monovalent and two trivalent silver ions in each molecular crystal. When
the crystals are activated with an oxidizing agent, they release electrons
equivalent to 6.4 x 10-19 watts per molecule which in effect
electrocute pathogens. A multitude of these devices are effective at such
low concentrations as 0.3 PPM where they can kill 100% of 100 K/cc Streptococcus
faecalis, and E. coli colonies in three minutes meeting the ten-minute
EPA criteria of 100% kills within ten minutes for swimming pool and hot-tub
applications. The devices can be used in utilitarian bodies of water, such
as municipal and industrial water reservoirs.
References Cited ~
U.S. Patent Documents:
4055655
~ Oct., 1977 ~ Maurer et al. ~ 514/495
4092245
~ May., 1978 ~ Franks et al.. ~ 210/169
4492618
~ Jan., 1985. ~ Eder. ~ 210/764
5017295
~ May., 1991. ~ Antelman. ~ 210/764
5073382
~ Dec., 1991. ~ Antelman. ~ 210/169
5078902
~ Jan., 1992. ~ Antelman. ~ 210/764
5089275
~ Feb., 1992. ~ Antelman. ~ 210/169
5098582
~ Mar., 1992. ~ Antelman. ~ 210/764
Other References
Hawley's Condensed Chemical Dictionary, 11th ed, p. 699 (definition
of Ligand).
Hammer & Kleinberg: Inorganic Synthesis vol. IV, p. 12.
J. Servian & H. Buenafama, Inorg. NUC. Letters 5, 337
Claims ~
What is claimed is:
1. A method for killing pathogens including bacteria, viruses and algae
in utilitarian water bodies including the water of swimming pools, industrial
cooling towers, hot tubs and drinking supply reservoirs, which comprises
adding to the water a multitude of tetrasilver tetroxide molecular crystals
which are capable of electrocuting said pathogens via an electron transfer
mechanism involving their molecular structure in the presence of oxidizing
agents.
2. A method as claimed in claim 1 where the oxidizing agent is a persulfate.
3. A method as claimed in claim 1 where the concentration of the molecular
crystals in the water is a maximum of one part per million.
4. A method as claimed in claim 2 where the concentration of the molecular
crystals in the water is a maximum of one part per million.
Description ~
BACKGROUND OF THE INVENTION
The present invention relates to the employment of molecular crystals
as bactericidal, viricidal and algicidal devices, but more particularly
to the molecular crystal semiconductor tetrasilver tetroxide Ag4O4
which has two trivalent and two monovalent silver atoms per molecule, and
which through this structural configuration enables electronic activity
on a molecular scale capable of killing algae and bacteria via the same
mechanism as macroscale electron generators. The concept of molecular scale
semiconductor devices for the storage of information has been the subject
of much activity in recent years so that the concept of a molecular scale
device performing such functions as storing information or acting as resistors,
capacitors or photovoltaic devices is well accepted. The molecular device
of this invention is a multivalent silver diamagnetic semiconductor. The
bactericidal activity of soluble divalent silver (Ag II) complex bactericides
is the subject of U.S. Pat. No. 5,017,295 of the present inventor. The
inventor has also been granted U.S. Pat. Nos. 5,078,902, USP # 5,073,382,
USP # 5,089,275, and USP # 5,098,582, which all deal with Ag II bactericides
but more particularly with (respectively) halides, alkaline pH, stabilized
complexes and the divalent oxide. It is U.S. Pat. No. 5,098,582, and its
perfection that has led to the present invention. This patent designated
AgO as divalent silver oxide, the popular name of the compound. Indeed,
the Merck Index (11th Edition) designates the oxide as silver(II) oxide
(AgO) (entry 8469). However, it also states that it is actually a silver(I)-silver(III)
oxide with a molecular weight of 123.88. After filing my patent application,
a comprehensive examination was begun of information relating to the structure
of this oxide. Further investigation of the scientific literature revealed
that said oxide was actually on a molecular level Ag4O4
where one pair of silver ions in the molecule was trivalent and another
pair was monovalent. Said oxide is actually on a molecular level Ag4O4
where one pair of silver ions in the molecule is trivalent and another
pair is monovalent.
While the formula AgO accurately designates the silver:oxygen ratio,
the molecular weight of the compound is actually 495.52. Further elucidation
of the molecule's electromagnetic properties revealed that it is a diamagnetic
semiconductor. The structure is electronically active because of the trivalent
sp2 electron configuration disparity of the electrons within
the crystal. The oxide as presented in my patent was actually capable of
killing 100% of standardized E. coli and Strep. faecalis colonies in less
than five minutes at concentratiors of 0.5 PPM. My independent evaluations
of this oxide in areas unrelated to water treatment resulted in the "molecular
device" concept which was substantiated by submission of the oxide for
testing with a preferred embodiment of the invention (10 PPM of sodium
persulfate) at an Environmental Protection Agency (EPA) certified laboratory
which revealed that 0.5 PPM of oxide only yielded 0.003 PPM of silver in
solution, a silver concentration entirely too low to cause this level of
bactericidal activity. Indeed, the killing of the bacteria was analogous
to that obtained by electron generating devices utilized in swimming pools
or water towers for killing bacteria. It was therefore postulated that
the oxide efficacy at low concentrations could only be attributed to regarding
each oxide molecule as a device. Further testing was continued on algae
and viruses. The accumulated data of efficacy at low concentrations, coupled
together with a reinterpretation of silver oxide efficacy, has led to the
final development of this invention, namely, a molecular device for killing
algae, bacteria and viruses in utilitarian water bodies, such as swimming
pools.
OBJECTS OF THE INVENTION
The main object of this invention is to provide for a molecular scale
device of a single tetrasilver tetroxide semiconductor crystal capable
of killing viruses, bacteria, and algae when operating in conjunction with
other such devices.
Another object of the invention is to provide for a device which is
so small that several thousand trillion can be added to a water supply
to perform their effective functions and still be effective at concentrations
of the devices in said supply not exceeding one part per million.
Still another object of the invention is to provide for a device which
will perform the aforementioned anti-pathogenic functions without polluting
the water supplies it is intended to purify, such as swimming pools, industrial
cooling towers, hot tubs and municipal water supplies.
Still another object of the invention is to provide for a device which
can be employed in swimming pools, hot tubs and other environments for
these aforementioned functions in the presence of humans, without causing
them respiratory and eye irritations and other nuisance effects characteristic
of active sanitizers based on halogens such as chlorine, one such nuisance
affect being the deterioration of bathing suits.
Other objects and features of the present invention will become apparent
to those skilled in the art when the present invention is considered in
view of the accompanying examples. It should, of course, be recognized
that the accompanying examples illustrate preferred embodiments of the
present invention and are not intended as a means of defining the limits
and scope of the present invention.
SUMMARY OF THE INVENTION
This invention relates to a molecular scale device capable of destroying
gram positive and gram negative bacteria as well as viruses and algae.
Said molecular scale device consists of a single crystal of tetrasilver
tetroxide. Several hundred thousand trillion of these devices may be employed
in concert for their bactericidal, viricidal, and algicidal properties
and applied to industrial cooling towers, swimming pools, hot tubs, and
municipal water supplies.
The molecular crystals which are the subject of this invention are commercially
available and can be prepared by reacting silver nitrate with sodium or
potassium peroxydisulfate according to the following equation:
4AgNO3 + 2Na2 S2 O8 + 8NaOH
= Ag4O4 + 4Na2SO4 + 4NaNO3
+ 4H2O
The oxide lattice represented by the formula Ag4O4
is depicted in the Drawing FIG. 1. It is a semiconducting electron active
diamagnetic crystal containing two monovalent and two trivalent silver
ions in combination with four oxygen atoms. The distance between the Ag(III)-O
Ag(I)O units equals 2.1 A. Ag(III)-Ag(III) = Ag(I)-Ag(I) = 3.28A and Ag(I)-Ag(III)
= 3.19 A. Each trivalent silver ion is coordinated via dsp2
electron bonds to 4 oxygen atoms. The depiction of this lattice is based
on several literature references relating to crystallographic studies.
Exemplary of this literature are J. A. McMillan's studies appearing in
Inorganic
Chemistry 13,28 (1960); Nature vol. 195 No. 4841 (1962), and
Chemical
Reviews 1962, 62,65. Alvin J. Salkind elucidated studies involving
neutron diffraction with his coworkers (J. Ricerca Sci. 30, 1034
1960) proving the Ag(III)/Ag(I) nature of this molecule and states in his
classic entitled Alkaline Storage Batteries (Wiley 1969), coauthored with
S. Uno Falk, that the formula is depicted by Ag4O4
(page 156).
That same year a scientific communication appeared in Inorganic Nuclear
Chemistry Letters (5,337) authored by J. Servian and H. Buenafama which
maintained that their neutron diffraction studies also confirmed the tetroxide
lattice and the presence cf Ag(III) and Ag(I) bonds in the lattice, a conclusion
also reported previously by Naray-Szahn and Argay as a result of their
x-ray diffraction studies (Acta Cryst. 1965, 19,180). Thus the effects
of this invention can be explained in terms of these structural elucidations,
namely, that the single molecular semiconductor crystal which inevitably
must be electronically active exchanging two electrons per crystals between
its mono and trivalent bonds is in reality a device which kills pathogens
in the same manner as electrically active large-scale devices utilized
in water supplies.
When the tetroxide crystals are utilized to destroy pathogens, they
will not do so unless activated by an oxidizing agent. This is analogous
to the behavior of single semiconducting photovoltaic molecular devices
such as copper indium selenide whose surfaces must be "etched" in order
to activate the photovoltaic activity, i.e., for light to facilitate the
release of electrons from the molecule. The tetroxide was activated by
persulfates. It was found that when the persulfates were tested as a control
by themselves, they failed to exhibit any unilateral antipathogenic activity
at the optimum level selected of 10 PPM. The persulfates evaluated varied
from OXONE (Registered Trademark Du Pont Company) brand potassium monopersulfate
to alkali peroxydisulfates.
DESCRIPTION OF THE DRAWING
In the drawing which illustrates the best mode presently contemplated
for carrying out the present invention:
FIG. 1 is a diagrammatic view showing the molecular crystal Ag4O4
attacking a pathogenic bacillus.
DESCRIPTION OF THE INVENTION
Turning now to Drawing FIG. 1 depicting the crystal lattice of Ag4O4
, the device operates by transferring electrons from the monovalent silver
ions 10 to the trivalent silver ions 11 in the crystal 20 through the aqueous
media in which it is immersed and which conducts electrons depicted by
the path 12, contributing to the death of pathogen 13 with electrons 14,
traversing the cell membrane surface 15, said pathogen being "electrocuted"
by not only these electrons but by others: 16 and 17 following paths 18,
and 19 emanating from other molecular devices in the vicinity of the pathogen.
Drawing FIG. 1 exaggerates the size of the silver oxide molecular device
with respect to that of a microorganism for depiction purposes only. The
device is attracted to the cell membrane surface 15 by powerful covalent
bonding forces 21 caused by the well-known affinity of silver to certain
elements present in the membrane, such as sulfur and nitrogen.
The electron transfer can be depicted by the following half reactions
in which the monovalent silver ion loses an electron and the trivalent
silver gains one as follows:
Ag + -e = Ag+2
Ag+3 + e = Ag+2
The molecular crystal then will become stabilized with each silver ion
having a divalent charge.
The molecular device was evaluated in concentrations ranging from 0.5
to 5.0 PPM on mixed gram positive and gram negative cultures and mixed
coliforms for evaluation in conjunction with EPA protocols for swimming
pools in the presence of 10 PPM sodium persulfate. It killed 100% of colonies
of Streptococcus faecalis and E. coli within three minutes at 0.5 PPM.
The EPA requirement is within ten minutes. The colony concentrations were
100,000/cc.
In order to consider the possibility that silver ions escaping the crystal
device may have had an influence on the bactericidal properties of the
device especially if those silver ions were of a higher valence state facilitated
by the persulfate according to the reaction:
AgO + H2O = Ag+2 + 2OH-
Ag4O4 crystals were sent to an independent
EPA certified testing laboratory together with sodium persulfate with specific
instructions to prepare Ag4O4 suspensions in
10 PPM persulfate at various concentrations. The preparations were made
in one-liter volumetric flasks utilizing 0.5 mg and other concentrations
/L of Ag4O4 , where the concentration of mg. per
liter equals parts per million of the oxide. After vigorous mixing of the
oxide crystals in the flasks, the solutions were allowed to remain undisturbed
for 24 hours. After that time period the supernatant liquid was analyzed
for silver utilizing atomic absorption spectroscopy with inductively coupled
plasma. At 0.5 PPM Ag4O4 there was only silver found
equivalent to 0.003 PPM. This concentration is so low that even if it were
speculated that the ions were in a higher valence state, they could never
even then be considered bactericidal. Indeed, the inventor's U.S. Pat.
No. 5,017,295 involving divalent silver bactericides claims these compounds
at the lowest silver ion concentration of 0.5 PPM.
If we are to consider one molecular device in operation, then each molecule
would release two electrons having each a charge of 4.8 x 10-10
e.s.u. equivalent to approximately 1.6 x 10-19 coulombs. The
EMF given in my Encyclopedia of Chemical Electrode Potentials (Plenum
1982), page 88, for the oxidation of Ag(I) to Ag(II) is 1.98 volts which
approximates 2.0 V. The total power output per device can be calculated
in watts by multiplying the power output for each electron by 2. Since
power is the product of the potential times the charge, P = EI; for each
electron it would be
2.0 x 1.6 x 10-19 = 3.2 x 10-19 watts
From this, and using Avogadro's number, we can calculate that the power
flux of one liter of solution containing 0.5 PPM of devices would be 0.064
watts. Since the electronic charges of the devices are directly proportional
to the number of devices in solution, i.e., the concentration of the oxide
in the solution, we can arbitrarily assign our own device power flux constant
which can be used to gauge the concentrations of the devices required in
order to kill particular organisms in specific environments. I have found
the following formula useful for this purpose:
Power Flux = EMF generated per molecule x Concentration x 5
(the EMF being 4.0 volts per molecular device times the concentration
in PPM). Utilizing this formula, the power flux to effectuate 100% kills
for E. coli and Streptococcus faecalis is equal to 6.0.
Tests were conducted to see whether the molecular crystals posed any
harm to the human body. Accordingly, a 3% concentrate of the crystals was
prepared for a series of evaluations.
The first evaluation met the requirements of Code of Federal Regulations
(CFR) 40 part 160 which consisted of determining the single dose toxicity
in rats or LD50. All the animals survived so that the LD50
was greater than 5.0 g./Kg. This was true for concentrations of crystals
of a magnitude of 6-60,000 times the actual concentrations that would be
used in its utilization. This test classified the device as a category
IV substance according to EPA protocols.
The second evaluation was for acute dermal toxicity in rabbits. The
protocol, 40 CFR 158.135, 81-2, was to determine the LD50 for
dermal application. All animals survived the maximum dose 2.0 g/Kg., classifying
the
crystals as category III with a dermal LD50 greater than
2000 mg/Kg.
The third evaluation, entitled "Primary Dermal Irritation in Albino
Rabbits", conformed to 40 CFR 160. It consisted of exposing the rabbits
for prolonged periods of time and observing edema, erythema, ulceration,
necrosis and any other evidence of dermal reactions or tissue destruction.
There were none, classifying the crystal concentrate as a category IV dermal
agent by EPA criteria.
The fourth evaluation dealt with primary eye irritation. This also was
in conformity with 40 CFR part 160. There was absolutely no eye irritation
when the crystal concentrate was applied, classifying it as a category
IV substance with regard to eye effects according to EPA criteria.
The concentrate submitted for these evaluations, i.e., the 3% suspension
of crystals, represented a concentration 1.50% times as great as the end
product intended for commercialization, namely, a 2% suspersion of silver
oxide crystals.
The crystals were also evaluated by monitoring their performance over
a period cf time at various concentrations. Periodically, water samples
were taken and shipped in a refrigerated state for bacterial counts. Accordingly,
the device performed in concert with its attendant devices in full conformity
with the ultimate objects of this invention.
Other objects and features of the present invention will become apparent
to those skilled in the art when the present invention is considered in
view of the accompanying examples. It should, of course, be recognized
that the accompanying examples illustrate preferred embodiments of the
present invention and are not intended as a means of defining the limits
and scope of the present invention.
EXAMPLE 1
Tetrasilver tetroxide (Ag4O4 ) crystals were prepared
by modifying the procedure described by Hammer and Kleinberg in Inorganic
Syntheses (IV,12). A stock solution was prepared by dissolving 24.0
grams of potassium peroxydisulfate in distilled water and subsequently
adding to this 24.0 of sodium hydroxide and then diluting the entire solution
with said water to a final volume of 500 ml. Into 20 ml. vials were weighed
aliquots of silver nitrate containing 1.0 g. of silver. Now 50 ml. of the
aforementioned stock solution were heated in a 100 ml. beaker, and the
contents of one of the vials was added to the solution upon attaining a
temperature of 85.degree. C. The beaker was then maintained at 90.degree.
C. for 15 minutes. The resulting deep black oxide obtained consisting of
molecular crystal devices was washed and decanted four times with distilled
water in order to remove impurities. The purified material was collected
for further evaluation and comparison with commercial material. The commercial
material was purchased from Johnson Matthey's Catalog Chemicals Division
of the Aesar Group of Ward Hill, Massachusetts, under product code 11607
and generically listed in its materials Safety Data Sheet as both silver
peroxide and silver suboxide, having a purity of 99.9%.
Both the prepared and commercial device crystals were submitted for
bactericidal evaluation following "good laboratory practice" regulations
as set forth in Federal Regulations (FIFRA and ffdca/40 CFR 160, May 2,
1984). The protocols consisted of exposures to Streptococcus faecalis,
a gram positive pathogenic bacillus utilizing AOAC (15th) 1990:965:13:
at colony densities of 100 000 colonies/cc. and two exposure times of five
and ten minutes. The devices were tested at concentrations of 0.3, 0.5
and 1.0 PPM in distilled water adjusted to pH = 7.5 and containing Oxone
(Registered Trademark Du Pont Company), which is potassium monopersulfate
at a level of 10 PPM. The evaluations were repeated at the same persulfate
concentration utilizing commercial grade sodium persulfate manufactured
by FMC. 100% kills were actually obtained after three minutes at all the
aforementioned device concentrations, there being actually zero colonies
at the 0.5 and 1.0 PPM levels after five minutes and at the 0.3 PPM level
after ten minutes. Analogous testing employing the same colony density
of the gram negative bacillus E. coli were carried out. The same results
were obtained. EPA criteria require that 100% kills be obtained within
ten minutes for a substance to meet EPA criteria for swimming pool utilizatior.
In this case, the devices at 0.3 PPM, equivalent to approximately 360,000
trillion devices, were able to far exceed EPA criteria for sanitizing a
swimming pool.
EXAMPLE 2
Commercial grade silver oxide prepared according to the method of Example
1, but which is actually the tetrasilver tetroxide molecular devices were
tested in a swimming pool under actual-use conditions. The swimming pool
contained approximately 27,000 gallons of water. The level of the device
crystal concentration was maintained at 1.0-1.5 PPM. The swimming pool
was periodically monitored by removing water samples for pH, silver calcium,
algae and bacteria. The swimming pool was utilized on a daily basis over
a period of six weeks by an average number of four people per day. The
pool was made up fresh with a fresh coating of plaster. The initial pH
was 9.7. By the end of the first week, the pH dropped to 8.2. Thereafter
the average daily pH of the pool was 7.8. The calcium level of the pool
was allowed to rise slowly from an initial 100 PPM to 220-240 PPM. Without
any new additions of silver to the solution of the initial 1.5 PPM molecular
crystal concentration, the pool had zero bacteria and zero algae. Other
extraneous factors were also monitored, such as copper (0.1-0.2 PPM) and
iron (initial .0 average .05 PPM), which did not affect the results.
EXAMPLE 3
Tests were performed on residual silver concentration of device crystals
in water to see whether the devices could be used to treat municipal drinking
water supplies since the devices had proven to be antipathogenic at 0.3
PPM according to Example 1. Now there is no adverse health effect for silver
at the present time according to the EPA, and it has been dropped from
the 1991 pollutants list according to 56 FR 1470 p.7. A secondary maximum
contaminant level for drinking water involving silver was proposed in 1989
(54 FR 22062), May 22, 1989) of 0.1 PPM. The oxidizing agent to activate
the crystals for water supplies would be OXONE (Registered Trademark Du
Pont Company) or hydrogen peroxide. Accordingly, brand potassium monopersulfate
samples of commercial oxide devices of Aesar origin as heretofore described
were sent to an EPA certified laboratory for evaluation. The laboratory
prepared samples of the devices at concentrations of 0.5, 1.0, 2.0, 5.0
and 10.0 PPM in 10 PPM sodium persulfate solution. The solutions were allowed
to stand for 24 hours, after which the supernatant liquid was tested for
residual silver content by atomic absorption spectroscopy using inductively
coupled plasma as the excitation source. The respective amounts of silver
found in the supernatant liquid were respectively 0.003, 0.13, 0.52 and
0.94 PPM. This means that at a concentration of nearly double the pathogenic
inhibition requirement level that the secondary silver allowance of 0.1
PPM was hardly reached, which qualifies the devices for drinking water.
EXAMPLE 4
The devices were tested against AIDS virus. The protocol used was that
of the Ministry of Health of the State of Israel at their Virology Laboratory
located at Tel HaShomer, Israel. AIDS viruses which had been grown in vitro
in a tissue culture were isolated and exposed to the devices at device
concentrations of 0.05, 1.0, 2.0, 3.0, 5.0 and 10.0 PPM. There was no evidence
of AIDS suppression at all until the concentrations reached 5.0 and 10.0
PPM. At 5.0 PPM, 60% of the viruses were killed. AT 10.0 PPM, 75% of the
viruses were killed. Extrapolation of this data reveals that at 18.0 PPM
there would be total suppression of the virus. These test results indicate
that the devices are capable of being used to destroy viruses in applications
involving the proliferation and transmittal of the AIDS virus outside of
the human body as in cold sterilization.
EXAMPLE 5
An ATTC strain of Chorella was grown in nutrient Medium 866 broth under
the required lighting. When optimal growth was reached, the number of organisms
per ml. were determined by microscopic count and then subcultured. The
molecular crystal devices were applied to the algae at concentrations of
1 and 2 PPM. The algae were left in contact for one hour, one day and ten
days. The protocol for these tests involved procedures described in the
Water and Waste Water Manual of the United States Public Health Service.
The exposure tests involved post inoculation in order to determine whether
the devices were algicidal or algistatic. The oxidizing agent for activation
was sodium persulfate at a concentration of 10 PPM. The devices were found
to be algistatic at 1 PPM and algicidal at 2 PPM after one hour's exposure.
After one day and ten days, there were no positive flasks at all. Ten flasks
of subculture were utilized for each test, and only one flask was positive
out of ten after one hour at 1 PPM.
While there is shown and described herein certain specific examples
embodying the invention, it will be manifest to those skilled in the art
that various modifications and rearrangements of &he invention may
be made without departing from the spirit and scope of the underlying inventive
concept and that the same is not limited to the particular forms herein
shown and described except insofar as indicated by the scope of the appended
claims.
US Patent # 6,485,755
Methods of Using Electron Active Compounds for Managing
Cancer
( US Cl. 424/618 ~ November 26, 2002 )
Marvin S. Antelman
Abstract ~
The present invention provides methods for preventing, treating, and/or
managing one or more cancerous conditions in a patient, such as a human.
A multivalent metal oxide, such as Ag(I,III), Cu(I,III), Pr(III,IV), and
Bi(III,V) oxides or a pharmaceutically acceptable derivative thereof, may
be administered to the patient in an amount and for a period of time which
is therapeutically effe