Acyclic and cyclic guanidine-and acetamidine derivatives,...

Drug – bio-affecting and body treating compositions – Designated organic active ingredient containing – Having -c- – wherein x is chalcogen – bonded directly to...

Reexamination Certificate

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C546S332000

Reexamination Certificate

active

06538013

ABSTRACT:

The present invention relates to novel pesticides of the formula (I) below having improved action against parasites; to compositions suitable for use as parasiticides comprising those compounds as active ingredient and to methods of controlling parasites that are based on the administration of those compounds or compositions, and to the use of the said compounds and compositions in a method of controlling parasites and in the manufacture of pesticides for use against parasites. Also described are intermediates of formula (XX) which themselves have parasiticidal activity and are excellently suitable for the preparation of compounds of formula (I).
Numerous pesticides are known that can be used in controlling parasites on warm-blooded animals. The control is effected principally by two different methods; either by way of contact action by topical and therefore external treatment of the host animal or systemically, that is to say by oral, transdermal or percutaneous administration to the host animal and ingestion of the active ingredient by the parasites via the blood of the host animal.
Far fewer substances are available for systemic use than for topical application, because only substances that have a systemic action and are well tolerated by the host animal can be used.
Compounds having as characteristic structural element the sub-structure of formula (II)
wherein R
1
, X, Y, T and U are as defined for formula (I) hereinbelow, form a very interesting class of substances on account of their pronounced topical and systemic action.
A prominent individual example is nitenpyram, a compound of formula (III)
Nitenpyram and other examples of this class of substances are disclosed, together with their preparation, in EP 0 302 389. Those compounds are described as pesticides having very pronounced insecticidal activity. Further examples of this class of substances are, for example, the subjects of the following patent applications: European published specifications Nos. 285 985; 302 833; 376 279; 471 372; 364 844; 493 369; 381 130; 529 680; 163 855; 375 907; 259 738; 386 565; 383 091 and 590 425; U.S. Pat. Nos. 5 063 236; 5 302 605 and 4 742 060; and also DE-4 207 604; GB-2 228 003 and WO 93/24002. Certain substituted 4-nitroimino-perhydro-1.3.5-oxadiazine derivatives and the use as pesticides and intermediates are described in WO 98/06710.
Nitenpyram and other examples of this class of substances that have the said structural element of formula (II) are extremely effective when administered as contact pesticides, for example externally, that is to say topically, to an infested host animal where they come into direct contact with the parasites. They also, however, exhibit a good systemic immediate action when they are administered to the infested host animal orally, parenterally, via injection or via implant.
The action, which is pronounced per se, has a serious disadvantage, however, in that it has been found that while the compounds have a high initial action, their action falls off rapidly only a short time after administration. This can be observed particularly clearly after systemic administration and can be monitored by reference to the bioavailability. Blood level measurements show that in many cases high blood levels are achieved even after a few minutes or, more rarely, after a few hours, but these levels then fall within a few hours, at best within a few days, and therefore fall to below an effective concentration much too rapidly.
In order to eliminate this shortcoming, numerous, but unfortunately unsuccessful, experiments have already been carried out. For example, it has been shown that a prolongation of the systemic action by increasing the dose can be achieved only to a limited extent. If, for example, depots sufficiently large for the active ingredient to be released over several weeks were to be placed under the skin or in the muscles, then the amounts to be injected or implanted would have to be so large that they would no longer be tolerated by the host animal; local irritation, skin eruptions and painful areas develop. This solution, possible per se, therefore fails on practical and, of course, also ethical grounds. Similarly, it has been found that a long-term action is not achievable by an increased oral dose.
When the known compounds having the structural element of formula (II) are administered, it is principally observed that a major part of the substance exhibits its full action only over a short period of time immediately after administration and thereafter the action very rapidly declines. This has serious consequences for preparations for use in veterinary medicine, for example for tablets, injections or for treatment using the pour-on or spot-on method. Because of the short duration of action it is necessary to repeat treatments at short intervals, which means that the keeper of the animal must either repeat the treatment himself, or have it carried out by a veterinary surgeon, at short intervals. Such an intensive treatment programme requires a high degree of discipline, however, and, as experience has shown, after only a short time gives rise to stress on the part of the animal and on the part of the animal's keeper, which not infrequently results in aversion to the treatment and leads to its premature discontinuation.
Prolongation of the action of this inherently extremely effective class of substances has therefore long been a desirable but apparently unattainable goal. The problem underlying the present invention was to achieve that goal and provide substances suitable for use as pesticides having significantly improved properties, especially having a pronounced long-term action.
By the provision of the compounds of formula (I) below it has now, surprisingly, been possible for compounds having the structural element of formula (II) to be modified chemically in such a manner that a high degree of long-term bioavailability after administration is achieved without it being necessary to accept adverse effects as a result.
The new, improved compounds are compounds of formula (I) below
wherein
R
1
is hydrogen or a radical from the group C
1
-C
4
alkyl, formyl, C
1
-C
6
alkylcarbonyl, C
1
-C
4
-alkylsulfonyl, aryl, arylsulfonyl, arylcarbonyl, heterocyclyl and heterocyclyl-substituted C
1
-C
6
alkyl, which radical is unsubstituted or mono- or poly-substituted by identical or different substituents; the said substituents being C
1
-C
4
alkyl, C
1
-C
4
alkoxy, C
1
-C
4
alkyl-thio, C
1
-C
4
haloalkyl, halogen, hydroxy, cyano, nitro, amino, C
1
-C
4
alkylamino, (C
1
-C
4
-alkyl)
2
amino, alkoxycarbonyl, C
1
-C
4
alkylsulfonyl and arylsulfonyl;
X is CH or N;
Y is an electron-withdrawing radical, preferably cyano, nitro or C
1
-C
6
haloalkyl-carbonyl, especially CO—CF
3
;
T has the meanings of R
1
or together with U forms a C
1
-C
4
alkylene bridge which is unsubstituted or substituted by a radical R
1
, or T and U together with the group —N—C—N— form a saturated or unsaturated 5- or 6-membered heterocyclic ring which may in addition contain as further hetero atom O or S or the hetero group —N(C
1
-C
6
alkyl)—;
U is hydrogen or C
1
-C
6
alkyl, preferably hydrogen, methyl or ethyl;
R
2
is hydrogen or C
1
-C
6
alkyl; R
2
′ is hydrogen or C
1
-C
6
alkyl; and
R is C
1
-C
20
alkyl, C
2
-C
20
alkenyl, C
2
-C
6
alkynyl or heterocyclyl, each of those radicals being unsubstituted or substituted by one or more identical or different substituents, the said substituents being selected from the group halogen, cyano, nitro, hydroxy, C
1
-C
6
alkoxy, C
1
-C
6
alkylthio, C
1
-C
6
haloalkyl, C
1
-C
6
haloalkoxy and phenyl; or is C
3
-C
7
cycloalkyl that is unsubstituted or mono- or poly-substituted by identical or different substituents selected from halogen, cyano, nitro, hydroxy, C
1
-C
6
alkyl, C
2
-C
6
alkenyl, C
2
-C
6
alkynyl, C
1
-C
6
alkoxy, C
1
-C
6
alkylthio, C
1
-C
6
haloalkyl, C
1
-C
20
haloalkoxy and phenyl; wherein each phenyl moiety is itself unsubstituted or mono- or poly-substituted by identical or different substituents selected from halogen, cyan

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