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Патент USA US3046197

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Untied SW8 Pets?“ Office.
3,645,188
‘Patented July
1
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-\
.7.
The ' patents; further n'ogtes j that' when other‘
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FUNGICIDAL COMPOSITION.
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- com;
pounds :such'ajs ‘zinc carbonate, zines-names; "gincottala'tc
were used plac'eof iinc'iotiide, tho result-s ,w'pré‘tnerciy
additive’andno synergistic effe'c'tfcoiu'ld‘befound. ,._' 11,]:
.
Bsmltarti ?autliana flotsam .8}?! ~ liitshwert Ontario,
Canada, and Gunter Goezc, Koin-Bayenthal, Gcrtnapy
(% ,Fahlherg-Lint G.:t1.b.!-l. ,Chemischc Fahrilt, G?llldt‘
In stillanqther. US. Patent 2,540,209itfisstafeditl'iai
_l’lat1.'_1],Pos?aehlltfl, Wolfenbu'tttgl, Germany) ,
,zirtc' sluifitejis .theponly 'zinc ‘salt 'whiehliglivelis' the desired
protection-‘against copper injury in coppcrfuogicidesn
'
ins =1,$,b¥lf5¢fi?t§ mat-“hi5.
"No‘prayvi’ng'. ‘Filed July 27,1959, seam). 829,505 '
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“If-Claims. "(Gl.’167--14)‘
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i
~-'»"I?h'isinvention-relates to improvements'in the"composi~
tion'of- -'fungicidal'1preparations ‘effective in protecting
10
tions in which the constituents imparting, fungicidal prop
erties are copper compounds supplemented by specific
over the improvements previously reported is‘obtained'by
the resulting composition-possesses fungicidal properties
the use of zinc chromate and/or zincsulphidehin, adnti>t7
greatly in excess of those attributable to the use of simi-'
lar amounts of copper compounds and zinc compound sep‘
tut'e \vithtungicide copper compounds.
duced by as much as 75%. whcn'uscd with the {proper
Thus in the prior art above noted, the besureported re
sults amounted to a saving of 50%_of copper w,hc_n,a_-c_om;
bination of a basic copper-zinc .sulphate is. uscd,,when
compared with the action of_a qoppcr-sul-phate-limemlu
tion. Howevcr,,wo have found that with agsttitttblejww
stance, in actual'pra'cticc‘it‘has been found that the amount
per compound used ‘in combination with zinc sulphide or
zinc chromate, an unexpectedly high saving with respect
to the copper compound is obtained and that only about
'
' It is ‘well ‘known that ‘ziin'c cor'n'pounds do not possess
any noticeable fungicide properties in thetnirelves? How
one-fourth of the amount of copper compound heretofore
deemed necessary need actually be used to effectively
ever, prior efforts to dimnish the amount of copper com
control the diseases mentioned.
pounds necessary to effectively protect the plants from
diseases mentioned above have included proposals to use
duce a saving of copper up to 50%.
However various patents relating to this subject mat
ter indicate that any such‘synergistic effect is not the
general -rule,,but rather the exception, notod only with
specific combinationsof zinc and copper compounds, and
not with most combinations.
_' For‘instance, in US. Patent 1,905,532 it is stated that
soluble‘ zin'c compounds damage the foliage of solanace
ous plants andthe use .of basiccopper and zinc sulphate
is proposed as‘ a fungi'eide,‘hydratcd lime being added
toreduc'e' the damage to the foliage. There is no men
tiot't'of a synergistic effect and _the mixture is proposed
,
_-
.- ,
free of Phytophthora, it is necessary. according to'the ‘
One such, proposal has been to dissolve copper and zinc "
salts in water and to produce by means of alkaline ma
copper and zinc sulphate. This composition, according to
its 'author is said to have a synergistic effect and to pro—
..
For instance, if a copper sulphate solution with 0.75%
of copper sulphate is used ‘in order to keep potato ?elds
acombination of zinc or zinc compounds with copper
compounds. in" order to produce effective parasiticidcs.
stance is formed which consists of a combination of basic
_,
proportions of the zinc compounds speci?ed.v . ._ ; t;
of afo'pper ‘compound necessary to keep a potato field
free of"‘Phytophthora,"‘spraycd only once is between
2.5 and ‘5.0 kg.of cupric oxychloride or l.2‘and ‘2.4 kg.
of'cup'rousioxide for'an acreage of one hectare (2.417
tetials precipitates‘which are soluble to a small extent
: ;_
chloride, basic copper carbonate, and ,the,_lik_e may be re;
tect‘ion of ?elds of‘some acreage is prodigious.v ‘For in-~
only._ According to this proposition, a protective sub
,
per compounds, .such as cuprous. oxide,' copper-oxy
It is well known that protection against diseases of the
groups listed above may be obtained by using copper com
pounds; When, howeven'this method is used the quan
tity'of copper‘compounds' necessary for an effective pro
"
,
Speci?cally it has been found that the amount of-cop:
arately.
'
. z .
ment in the effectiveness offungicidcscopper compounds
zinc compounds ‘which‘p'roduce a synergistic effect so that
"
-, ~
ing view is that .a huge number OfliItC compounds can
only be used if‘they canbe converted to basiccornpounds.
According to the present invcntiotra marked improve;
ticularly it relates-to-improvements in “fttgicidai composi'
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~.
bination, ‘produce synergistic effects, and lhatone prevailj
diumwOercospora, Perono'spor'a and the‘ like. More par
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per and “zinccompounds .irt general,1 when _usedi;in.-com<
plants-"agat't'tstvv diseus'es‘such - as ‘Phytophlhora, Fu'sicla
acres).
..
_ In summary then,.>prior patents in'this?e'ldfwould’iteind
to indicate that it is by no‘ means recognized-that cop;
accepted practice, to use about-600 liters for treutingnne
hectare (2.417 acres) in order to treat .the plants. uni
formly. it is therefore. necessary to expend- for each hccp
tare, 4.5 kg. of copper sulphate, a ?gure which corre
sponds to 1.8 kg. of metallic copper.
,
.,
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However, if according to the invention-n-cotnbination
of for instance, copper oxychloride and zinc sulphide is
used, actual ?eld tests have proved that/for each hectare
only 600 goof copper oxychloride must be used which con‘
tains 350 g._of metallic copper, Thisis clettrlyan effect
which could not have been-foreseen.’ The savings thus
obtained are about fottr times the savings obtainable by
the best method of saving so far mentioned in the litera
ture above quoted. The savings are still greater if com
pared with those plant protection compoundsand. mix
turcs_wbich are now used and which hnvcbcon endorsed
officially by Governmentuuthoritics. One of these-reci
ognizcd spraying means containing copperguses’ 2.5 ‘kg.
of copper oxychloride witlna content of 1445 kg. of’cop
por metal-for each hectare sprayed.v This/is-the bcst'coml
to prevent‘ ihe'damaging effect of zinc sulphate. per so.
pound_now known which‘hasfound general rocogx'ttn'om
on the plants.
Therefore, when compared with the most modernzooppot
.
1
Another proposal is'set forth in US. Patent 2.051910
wherein 'the physicahpropertie‘s of copper silicate fungi~
cides, are said to beeimprovcd ‘by replacing a portion ‘of
thezcopperwith zine; ' Lower damage to’ the foliage was
noted without a noticeable impairment in toxicity.
spraying fungicide the combination according tozthc in'v'en
tion has the advarnage that -it uses..only-oheifourtht-of
the copper or, otherwise stated, ‘that a quantity equal to
three times the quantity actually used can be considered
as having been saved.
I
2-.lnrUIS.’ Patent'2;225,867 a speci?c ‘synergistic effect is
‘ A further advantage. of -thb tnvention'consists inllhe
noted when zine oxide'is used in ‘combination with cop
per oxide; which is not evident in the case of'othcr com
pounds, according to the patcntee. indeed in other com
binations, the patentee reported that the use of zinc com
and
fact that
zinc the-rather
compoundscumbersome?convcrsioh
into their basic stilts of
by ‘the’
im'eans of
substances
of
alkaline
reaction
can
be
dispensed
with.’ '_ j
70
A further advantage of the combination‘ consists in the
pottnds-actuallydocrcased the effectiveness of the product.
fact that no damage to the foliage results, even if the
aces, 188
La
'33.
4
dosage should for some reason or other be excessive.
are again the quantity sprayed for each hectare of a
While applicants do not want to advance any theory for
this increasedielfectiveness, they assume that zinc chro
potato ?eld.
Example 4.-—Spraying Paste
mate as well as Zinc sulphide activate the copper com
[Proportions in grams]
pounds to a high degree. This has been deduced from
experiments with other zinc compounds (e.g. with zinc
carbonate) which do not produce any increase in the
30 g. copper oxychloride, 5 g. zinc sulphide, are mixed
intimately and thoroughly with 25 g. of a water disper
effectiveness of the copper salts as a fungicide.
sion of polyvinylacetate, 0.5 g. of animal glue and 39.5‘
pronounced improvement were zinc sulphide and zinc
chromate.
(2) The copper fungicides to which the invention is
ple 1 were made on two adjacent ground parcels planted
with hops. The hops on one ground parcel-was sprayed
and the other left unsprayed. The hops in the untreated
g. of water.
Before illustrating this invention in the speci?c exam
In order to prevent Peronospora on hops, the hops are
ples which follow, certain limiting and critical features 10
sprayed with a 0.5% suspension of the paste in water.
of the invention should be noted as follows:
Experimental tests similar to those described in Exam
(1) The only zinc compounds found to produce the
ground parcel were severely attacked by Peronospora
applicable are those copper compounds which are in
while the hops which were sprayed did not show any
soluble or difficulty soluble in water. Speci?c members
Peronospora attack and remained healthy.
of this class include: cuprous oxide, copper oxychloride,
copper hydroxide and basic copper carbonate.
Example 5 .—-Spraying Paste
(3) The amount of zinc compound to be used may 20
The spray prepared according to Example 4 was tested
vary considerably. It depends upon the nature of inert
on beets attacked by Cercospora. A test was made ex
diluents in the mixture, and upon the plant to which the
actly as described in Example 4 with the same results.
dust or spray is to be applied.
The relative proportions -
Example 6.—-Spraying Powder
of zinc compound: copper compound in the mixture
should preferably be between 1:4 and 1:8; that is, for
every ?ve parts by weight of zinc compound, between
20 and 40 parts by weight of a suitable copper fungicide
should be present.
25
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(4) Other ingredients which may be present in the
composition include diluents commonly used in the
preparation of sprays, pastes or dusts. -
The examples which follow are intended to be taken
as illustrative of the invention and not as limitative.
Example 1.—Spraying Powder
[Proportions in grams]
[Proportions in grams]
20 g. of copper oxychloride, 5 g. zinc sulphide are
mixed with 60 g. kaolin. Into this mix 5 g. of a higher
molecular weight aromatic sulfonic acid, acting as a wet~
ting and dispersion agent and 10 g. of powder acting as
an adhesive agent were worked, until complete homw
geneity was obtained. A 0.30% suspension of this spray
ing powder in water was sprayed on apple trees during
the pre-blossoming period to prevent infestation with
Fusicladium. The effect when compared with trees
35 which had not been sprayed was very marked.
25 g. copper oxychloride, and 5 g. zinc chromate are
intimately mixed with 55 g. kaolin. In this mixture 5 g.
of a higher molecular weight aliphatic sulfonic acid
acting as a wetting agent and as an emulsi?er such as 40
sodium sulforicinate and 10 g. of an adhesive known as
To this spray insecticides were added, especially
gamma hexachlorocyclophexane and dichlordiphenyltri
chlorethane.
Example 7.—-Spraying Powder
[Proportions in grams] ..
“cell powder” are worked.
A suspension of 3 kg. of a mixture, prepared with the
above proportions indicated in grams, in 600 liters of
30 g. cuprous oxide, 5 g. zinc sulphide are mixed with
45 g. of kaolin. Into this mix 5 g. of high molecular
weight aliphatic sulfonic acid such as sodium sulforicinate
water is prepared. This quantity is sprayed uniformly 45 and 10 g. of an adhesive known as “cell powder” and 5
on each hectare of a potato ?eld.
g. hexachlorocyclohexane are worked.
In an experimental test the potato plants on a ground
2 kg. of this spraying powder are suspended in 600
parcel Were treated and those on an adjacent ground par
liters of water and are sprayed over 1 hectare of ground
cel were not treated by spraying. On the non-treated
with potato plants. Infection with Phytophthora was
section the plants on account of infestation with Phytoph
completely prevented. The Colorado potato beetle and
thora died, on the sprayed section the plants remained
its larvae were completely killed‘ by the spraying.
healthy and completely free of Phytophthora.
Example 2.——Spraying Paste
[Proportions in grams]
30 g. copper oxychloride and 5 g. zinc sulphide are
stirred and intimately and thoroughly mixed by agitation
‘Example '8.-—Spray Powder
35 g. basic copper carbonate and 4 g. zinc sulphide are
mixed with 46 g. kaolin, 5 g. of a high molecular weight
aliphatic sulfonic acid, as wetting and emulsifying agent,
and 10 g. cellulose powder, as binding agent, are worked
with 25 g. of a watery dispersion of polyvinylacetate, 0.5
into the mixture.
g. animal glue powder, the latter acting as a stabilizer,
3 kg. of the powder was dispersed in 600 liters of water
and 39.5 g. of water.
60 and uniformly sprayed over one hectare of potato plants.
The mix has the consistency of a paste and 3 kg. of
Lots not sprayed developed a Phytophthora infection.
this paste are suspended in 600 liters of water. This
'Il‘lhe
sprayed lots remained healthy and free of Phytoph~
quantity is sprayed on one hectare (2.417 acres) of
t ora.
potato plants.
The experiment mentioned in Example 1, was also
made with this mixture of Example 2.
Example 3.——Spraying Paste
[Proportions in grams]
The same effect as that described in Examples 1 and 2
is obtained with a mix of 22 g. cuprous oxide, 5 g. zinc
sulphide, 25 g. of a watery dispersion of polyvinyl pro
pionate, 0.5 g. of animal glue serving as a stabilizer, and
47.5 g. of water which are intimately mixed to form a
paste. 3 kg. of the paste suspended in 600 liters of water 75
Example 9.—Spray Paste
30 g. basic copper carbonate and 5 g. zinc chromate
are stirred with 25 g. of an aqueous dispersion of poly
vinyl acetate, 0.5 g. lime powder as stabilizer and 39.5 g.
water.
3 kg. of this pasty mass was disposed in 600 liters of
water and sprayed over one hectare of potato plants.
The effectiveness against Phytophthora was the same as in
Example 8.
Example 10.—Spray Powder
v
25 g. copper hydroxide and 5 g. zinc sulphide are mixed
3,046,188
6
with 55 g. kaolin, 5 g. of a high molecular weight aliphatic
sulfonic acid, as wetting and emulsifying agent, and 10
5. A fungicidal mixture consisting essentially of zinc
sulphide and copper hydroxide in the relative proportions
g. cellulose powder, as binding agent, are worked into
the mixture.
of about 1 part of zinc sul?de to between about 4 and 9
parts of copper hydroxide, by ‘weight.
Field experimentation, employing 3-6 kg. of this spray
6. The process of controlling fungus growth of a fungus
selected from the group consisting of Phytophthora,
powder dispersed in 600 liters of water as a spray over one
hectare of beets, produced inhibition of infection by
Fusicladium, Cercospora, and Peronospora on living plants
Example JL-Spray Paste
which comprises applying to the plant a fungicidal com
position having as an active ingredient a mixture consist~
ing of a zinc compound selected from the group consist
ing of zinc sulphide and Zinc chromate and a copper com
pound selected from the group consisting of cuprous oxide,
copper hydroxide, copper oxychloride and basic copper
Cercospora.
PFpi
30 g. copper hydroxide and 5 g. zinc chromate are
stirred with 25 g. of an aqueous dispersion of polyvinyl
acetate, 0.5 g. lime powder as stabilizer and 39.5 g. water.
3 kg. of this pasty mass is dispersed in 600‘ liters of
water and sprayed over one hectare of beets. The ef~
fectiveness against Cercospora was the same as in Ex
carbonate the relative proportions of said Zinc compound
and said copper compound being between about 4 and 9
parts by weight of copper compound for each part of
weight of zinc compound.
7. The method of claim 6, wherein the mixture contains
between 20 and 45 parts by weight of copper compound
for each 5 parts by weight of zinc compound.
8. The method of claim 6 wherein the zinc compound
is zinc chromate and the copper compound is copper oxy
chloride.
9. The method of claim 6 wherein the zinc compound
is zinc sulphide and the copper compound is copper oxy
chloride.
10. The method of claim 6 wherein the zinc compound
is Zinc sulphide and the copper compound is basic copper
carbonate.
11. The method of claim 6 wherein the zinc compound
is zinc sulphide and the copper compound is copper hy
droxide.
ample 10.
This application is a continuation-in-part of Serial No.
547,303, ?led November 16, 1955, now abandoned in
favor of the present application.
What is claimed as new is as follows:
1. A mixture for protecting plants against fungicidal
diseases such as Phytophthora, Fusicladium, Cercospora,
and Peronospora comprising for each 5 parts in weight
of a zinc compound of the group consisting of zinc
sulphide and zinc chromate, between 20* and 45 parts by
Weight of an insoluble fungicidal copper compound of the
group consisting of cuprous oxide, copper hydroxide,
copper oxychloride and basic copper carbonate; and from
3 to 12 parts by weight of kaolin.
2. A fungicidal mixture consisting essentially of 5 parts
by weight of Zinc chromate and 25 parts by Weight of
copper oxychloride.
3. A fungicidal mixture consisting essentially of be
tween 20 and 40 parts by weight of copper oxychloride
and about 5 parts by weight of Zinc sulphide.
4. A fungicidal mixture consisting essentially of zinc
sulphide and basic copper carbonate in the relative pro~
References Cited in the ?le of this patent
UNITED STATES PATENTS
2,602,727
portions of about 1 part of zinc sul?de to between 4 and
9 parts of basic copper carbonate, by weight.
6
Warinner ____________ _- July 8, 1952
OTHER REFERENCES
Frear: A Catalogue of Insecticides and Fungicides
(1948), vol. 1, page 173; vol. 2, pages 51, 52, 56.
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