US2017101392A1PendingUtilityA1

Processes for the preparation of pesticidal compounds

63
Assignee: DOW AGROSCIENCES LLCPriority: Oct 17, 2013Filed: Dec 23, 2016Published: Apr 13, 2017
Est. expiryOct 17, 2033(~7.3 yrs left)· nominal 20-yr term from priority
C07D 401/04A01N 47/40A01N 43/56
63
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Claims

Abstract

The present application provides processes for making pesticidal compounds and compounds useful both as pesticides and in the making of pesticidal compounds.

Claims

exact text as granted — not AI-modified
1 . A process comprising:
 (a) reacting 3-hydrazinopyridine dihydrochloride with methyl acrylate, under basic conditions, to yield 1-(pyridin-3-yl)pyrazolidin-3-one; and   (b) chlorinating 1-(pyridine-3-yl)pyrazolidin-3-one with phosphoryl chloride (POCl 3 ) to yield dihydropyrazole chloride (5a)   
       
         
           
           
               
               
           
         
       
     
     
         2 . (canceled) 
     
     
         3 . A process comprising nitrating 3-(3-chloro-1H-pyrazol-1-yl)pyridine (5b) to yield 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) 
       
         
           
           
               
               
           
         
       
     
     
         4 . A process comprising reducing 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) to yield 3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-amine (5d) 
       
         
           
           
               
               
           
         
       
     
     
         5 . A process comprising reacting 3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-amine (5d) with an activated carbonyl thioether of formula X 1 C(═O)C 1 -C 4 -alkyl-S—R 1  to yield pesticidal thioether (3b) 
       
         
           
           
               
               
           
         
       
       wherein,
 R 1  is selected from the group consisting of C 1 -C 4 -haloalkyl and C 1 -C 4 -alkyl-C 3 -C 6 -halocycloalkyl, and 
 X 1  is selected from the group consisting of Cl, OC(═O)C 1 -C 4  alkyl, and a group that forms an activated carboxylic acid. 
 
     
     
         6 .- 7 . (canceled) 
     
     
         8 . A process comprising
 (a) reacting 3-chloro-N-ethyl-1-(pyridin-3-yl)-1H-pyrazol-amine (5d) with 3-chloropropionyl chloride to yield 3-chloro-N-(3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-yl)-N-ethylpropanamide (5e);   
       
         
           
           
               
               
           
         
         (b) reacting compound (5e) with HSR 1    
         wherein, 
         R 1  is selected from the group consisting of C 1 -C 4 -haloalkyl and C 1 -C 4 -alkyl-C 3 -C 6 -halocycloalkyl 
       
       to yield pesticidal thioether (5f) 
       
         
           
           
               
               
           
         
       
     
     
         9 . A process comprising:
 (a) nitrating 3-(3-chloro-1H-pyrazol-1-yl)pyridine (5b)   
       
         
           
           
               
               
           
         
       
       to yield 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) 
       
         
           
           
               
               
           
         
         (b) reducing 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) to yield 3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-amine (5d) 
       
       
         
           
           
               
               
           
         
         (c) reacting 3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-amine (5d) with an activated carbonyl thioether of formula X 1 C(═O)C 1 -C 4 -alkyl-S—R 1  to yield pesticidal thioether (3b) 
       
       
         
           
           
               
               
           
         
       
       wherein,
 R 1  is selected from the group consisting of C 1 -C 4 -haloalkyl and C 1 -C 4 -alkyl-C 3 -C 6 -halocycloalkyl, and 
 X 1  is selected from the group consisting of Cl, OC(═O)C 1 -C 4  alkyl, and a group that forms an activated carboxylic acid; and 
 (d) alkylating pesticidal thioether (3b) with R 2 —X 2  to yield pesticidal thioether (3c), 
 
       
         
           
           
               
               
           
         
       
       wherein,
 X 2  is a leaving group, and 
 R 2  is selected from the group consisting of C 1 -C 4 -alkyl and C 2 -C 4 -alkynyl. 
 
     
     
         10 . A process comprising:
 (a) reacting 3-hydrazinopyridine dihydrochloride with methyl 2-acetamidoacrylate to yield N-(3-oxo-1-(pyridin-3-yl)pyrazolidin-4-yl)acetamide   
       
         
           
           
               
               
           
         
         (b) chlorinating/eliminating N-(3-oxo-1-(pyridin-3-yl)pyrazolidin-4-yl)acetamide to yield 3-(3-chloro-1H-pyrazol-1-yl)pyridine (5b) 
       
       
         
           
           
               
               
           
         
         (c) nitrating 3-(3-chloro-1H-pyrazol-1-yl)pyridine (5b) to yield 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) 
       
       
         
           
           
               
               
           
         
         (d) reducing 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) to yield 3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-amine (5d) 
       
       
         
           
           
               
               
           
         
         (e) reacting 3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-amine (5d) with an activated carbonyl thioether of formula X 1 C(═O)C 1 -C 4 -alkyl-S—R 1  to yield pesticidal thioether (3b) 
       
       
         
           
           
               
               
           
         
       
       wherein,
 R 1  is selected from the group consisting of C 1 -C 4 -haloalkyl and C 1 -C 4 -alkyl-C 3 -C 6 -halocycloalkyl, and 
 X 1  is selected from the group consisting of Cl, OC(═O)C 1 -C 4  alkyl, and a group that forms an activated carboxylic acid; and 
 (f) alkylating pesticidal thioether (3b) with R 2 —X 2  to yield pesticidal thioether (3c), 
 
       
         
           
           
               
               
           
         
       
       wherein,
 X 2  is a leaving group, and 
 R 2  is selected from the group consisting of C 1 -C 4 -alkyl and C 2 -C 4 -alkynyl. 
 
     
     
         11 . A process comprising:
 (a) nitrating 3-(3-chloro-1H-pyrazol-1-yl)pyridine (5b)   
       
         
           
           
               
               
           
         
       
       to yield 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) 
       
         
           
           
               
               
           
         
         (b) reducing 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) to yield 3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-amine (5d) 
       
       
         
           
           
               
               
           
         
         (c)
 (1) reacting 3-chloro-N-ethyl-1-(pyridin-3-yl)-1H-pyrazol-amine (5d) with 3-chloropropionyl chloride to yield 3-chloro-N-(3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-yl)-N-ethylpropanamide (5e); 
 
       
       
         
           
           
               
               
           
         
         
           (2) reacting compound (5e) with HSR 1    
         
         wherein, 
         R 1  is selected from the group consisting of C 1 -C 4 -haloalkyl and C 1 -C 4 -alkyl-C 3 -C 6 -halocycloalkyl 
       
       to yield pesticidal thioether (5f) 
       
         
           
           
               
               
           
         
       
       and
 (d) alkylating pesticidal thioether (5f) with R 2 —X 2  to yield pesticidal thioether (5g), 
 
       
         
           
           
               
               
           
         
       
       wherein,
 X 2  is a leaving group, and 
 R 2  is selected from the group consisting of C 1 -C 4 -alkyl and C 2 -C 4 -alkynyl. 
 
     
     
         12 . A process comprising:
 (a) reacting 3-hydrazinopyridine dihydrochloride with methyl 2-acetamidoacrylate to yield N-(3-oxo-1-(pyridin-3-yl)pyrazolidin-4-yl)acetamide   
       
         
           
           
               
               
           
         
         (b) chlorinating/eliminating N-(3-oxo-1-(pyridin-3-yl)pyrazolidin-4-yl)acetamide to yield 3-(3-chloro-1H-pyrazol-1-yl)pyridine (5b) 
       
       
         
           
           
               
               
           
         
         (c) nitrating 3-(3-chloro-1H-pyrazol-1-yl)pyridine (5b) to yield 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) 
       
       
         
           
           
               
               
           
         
         (d) reducing 3-(3-chloro-4-nitro-1H-pyrazol-1-yl)pyridine (5c) to yield 3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-amine (5d) 
       
       
         
           
           
               
               
           
         
         (e)
 (1) reacting 3-chloro-N-ethyl-1-(pyridin-3-yl)-1H-pyrazol-amine (5d) with 3-chloropropionyl chloride to yield 3-chloro-N-(3-chloro-1-(pyridin-3-yl)-1H-pyrazol-4-yl)-N-ethylpropanamide (5e); 
 
       
       
         
           
           
               
               
           
         
         
           (2) reacting compound (5e) with HSR 1    
         
         wherein, 
         R 1  is selected from the group consisting of C 1 -C 4 -haloalkyl and C 1 -C 4 -alkyl-C 3 -C 6 -halocycloalkyl to yield pesticidal thioether (5f) 
       
       
         
           
           
               
               
           
         
       
       and
 (f) alkylating pesticidal thioether (5f) with R 2 —X 2  to yield pesticidal thioether (5g), 
 
       
         
           
           
               
               
           
         
       
       wherein,
 X 2  is a leaving group, and 
 R 2  is selected from the group consisting of C 1 -C 4 -alkyl and C 2 -C 4 -alkynyl. 
 
     
     
         13 . A compound 1-(pyridin-3-yl)pyrazolidin-3-one 
       
         
           
           
               
               
           
         
       
     
     
         14 . A compound N-(3-oxo-1-(pyridin-3-yl)pyrazolidin-4-yl)acetamide 
       
         
           
           
               
               
           
         
       
     
     
         15 . A compound 3-chloro-N-(3-chloro-1-(pyridine-3-yl)-1H-pyrazol-4-yl)propanamide (5e) 
       
         
           
           
               
               
           
         
       
     
     
         16 . A compound 3-(3-chloro-4,5-dihydro-1H-pyrazol-1-yl)pyridine (5a) 
       
         
           
           
               
               
           
         
       
     
     
         17 .- 20 . (canceled) 
     
     
         21 . A process according to  claim 11 , wherein thioether (5g) 
       
         
           
           
               
               
           
         
       
       is prepared by alkylating thioether (5f) with R 2 —X 2    
       
         
           
           
               
               
           
         
         wherein R 2  is selected from the group consisting of C 1 -C 4 -alkyl and C 2 -C 4 -alkynyl, 
         wherein X 2  is a leaving group, 
       
       in the presence of a base, in the presence of a polar aprotic solvent, and in the presence of an additive. 
     
     
         22 .- 28 . (canceled) 
     
     
         29 . A process according to  claim 5 , wherein X 1 C(═O)C 1 -C 4 -alkyl-S—R 1 ,
 wherein, 
 R 1  is selected from the group consisting of C 1 -C 4 -haloalkyl and C 1 -C 4 -alkyl-C 3 -C 6 -halocycloalkyl, and 
 X 1  is selected from the group consisting of Cl, OC(═O)C 1 -C 4  alkyl, and a group that forms an activated carboxylic acid 
 
       is prepared from 
       
         
           
           
               
               
           
         
       
       which is prepared by the photochemical free-radical coupling of 3-mercaptopropionic acid and esters thereof with 3,3,3-trifluoropropene in the presence of 2,2-dimethoxy-2-phenylaceto-phenone initiator and long wavelength UV light in an inert organic solvent. 
     
     
         30 . A process according to  claim 5 , wherein X 1 C(═O)C 1 -C 4 -alkyl-S—R 1 ,
 wherein, 
 R 1  is selected from the group consisting of C 1 -C 4 -haloalkyl and C 1 -C 4 -alkyl-C 3 -C 6 -halocycloalkyl, and 
 X 1  is selected from the group consisting of Cl, OC(═O)C 1 -C 4  alkyl, and a group that forms an activated carboxylic acid 
 
       is prepared from 
       
         
           
           
               
               
           
         
       
       which is prepared by the low temperature free-radical initiated coupling of 3-mercaptopropionic acid with 3,3,3-trifluoropropene in the presence of 2,2′-azobis(4-methoxy-2,4-dimethyl) valeronitrile (V-70) initiator at temperatures of about −50° C. to about 40° C. in an inert organic solvent. 
     
     
         31 . (canceled)

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