US2004220235A1PendingUtilityA1

Method of inhibiting amyloid protein aggregation and imaging amyloid deposits

Priority: Jun 10, 1999Filed: Jun 2, 2004Published: Nov 4, 2004
Est. expiryJun 10, 2019(expired)· nominal 20-yr term from priority
C07D 257/04C07D 217/02C07D 213/82A61K 31/402C07C 229/62C07C 311/51A61K 31/4164C07D 209/44C07D 233/88C07D 413/06C07C 229/64A61P 25/28C07D 295/135C07D 317/58C07C 233/43A61K 31/196C07C 229/58
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Claims

Abstract

The present invention provides a method of treating Alzheimer's disease using a compound of Formula I Also provided is a method of inhibiting the aggregation of amyloid proteins using a compound of Formula I and a method of imaging amyloid deposits, as well as new compounds of Formula I.

Claims

exact text as granted — not AI-modified
1 . A method of treating Alzheimer's disease, the method comprising administering to a patient having Alzheimer's disease a therapeutically effective amount of a compound of Formula I  
       
         
           
           
               
               
           
         
         wherein  
         R a  is hydrogen, C 1 -C 6  alkyl, or  
         
           
             
             
                 
                 
             
           
         
         n is 0 to 5 inclusive;  
         R 1 , R 2 , R 3 , R 4 , R 5 , R 6 , and R 7  are independently hydrogen, halogen, —OH, —NH 2 , NR b R c , —CO 2 H, —CO 2 C 1 -C 6  alkyl, —NO 2 , —OC 1 -C 12  alkyl, —C 1 -C 8  alkyl, —CF 3 , —CN, —OCH 2  phenyl, —OCH 2 -substituted phenyl, —(CH 2 ) m -phenyl, —O-phenyl, —O-substituted phenyl, 
 —CH═CH-phenyl, —O(CH 2 ) p NR b R c ,  
                     
 —NH(CH 2 ) p NR b R c , —N(C 1 -C 6 alkyl)(CH 2 ) p NR b R c ,  
                     
 
         R 8  is COOH, tetrazolyl, —SO 2 R d , or —CONHSO 2 R d ;  
         R b  and R C  are independently hydrogen, —C 1 -C 6  alkyl, —(CH 2 ) m -phenyl, or R b  and R c  taken together with the nitrogen atom to which they are attached form a cyclic ring selected from piperidinyl, pyrrolyl, imidazolyl, piperazinyl, 4-C 1 -C 6  alkylpiperazinyl, morpholino, thiomorpholino, decahydroisoquinoline, or pyrazolyl;  
         R d  is hydrogen, —C 1 -C 6  alkyl, —CF 3 , or phenyl;  
         m is 0 to 5 inclusive;  
         p is 1 to 5 inclusive;  
         A is CH or N;  
         R 1  and R 2 , when adjacent to one another, can be methylene-dioxy;  
         or the pharmaceutically acceptable salts thereof.  
       
     
     
         2 . The method of  claim 1  wherein 
 R a  is hydrogen;  
 n is 2; and  
 R 3  and R 4  are hydrogen.  
 
     
     
         3 . The method of  claim 1  wherein 
 R a  is hydrogen;  
 R 3  and R 4  are hydrogen; and  
 n is 2 to 5 inclusive.  
 
     
     
         4 . The method of  claim 1  wherein 
 R a  is hydrogen;  
 n is 2;  
 R 3  and R 4  are hydrogen; and  
 R 1 , R 2 , and R 7  are independently chlorine, —N(CH 2 CH 3 ) 2 , —OH, CH 3 —, fluorine, —CF 3 , phenyl, hydrogen, —OCH 2  phenyl, —O(CH 2 ) 3 N(CH 3 ) 2 , —O phenyl, —O(CH 2 ) 7 CH 3 , —CH(CH 2 OCH 2 CH 3 ) 2 , pyrrolyl, —CH═CH-phenyl,  
                     
  —N[(CH 2 ) 3 CH 3 ] 2 , substituted phenyl, —OCH 2 — substituted phenyl, pyrrozolyl, or —N(phenyl) 2 .  
 
     
     
         5 . The method of  claim 1  wherein 
 R a  is hydrogen;  
 n is 3, 4, or 5;  
 R 3  and R 4  are hydrogen; and  
 R 1 , R 2 , and R 7  are independently chlorine or hydrogen.  
 
     
     
         6 . The method of  claim 1  wherein 
 R a  is hydrogen;  
 n is 2;  
 R 3  and R 4  are hydrogen; and  
 R 5 , R 6 , and R 8  are independently hydrogen, —CO 2 H, —NO 2 , —OCH 3 ,  
 imidazolyl, —CN, fluorine, —CH 3 , —CF 3 , halogen,  
 —NH—C 1 -C 6  alkyl, —N(C 1 -C 6 alkyl) 2 , —NH 2 , or pyrrolyl.  
 
     
     
         7 . The method of  claim 1  wherein 
 R a  is hydrogen;  
 n is 2;  
 R 3  and R 4  are hydrogen; and  
 R 5  is —CO 2 H.  
 
     
     
         8 . A method of treating Alzheimer's disease, the method comprising administering to a patient having Alzheimer's disease a therapeutically effective amount of a compound of Formula I  
       
         
           
           
               
               
           
         
         wherein  
         R a  is hydrogen;  
         n is 1 to 5 inclusive;  
         R 3  and R 4  are hydrogen;  
         R 1 , R 7 , and R 2  are independently chlorine, —N(CH 2 CH 3 ) 2 , —OH, CH 3 —, fluorine, —CF 3 , phenyl, hydrogen, —OCH 2  phenyl, —O(CH 2 ) 3 N(CH 3 ) 2 , —O phenyl, —O(CH 2 ) 7 CH 3 , —CH(CH 2 OCH 2 CH 3 ) 2 , pyrrolyl, —CH═CH-phenyl, —N[(CH 2 ) 3 CH 3 ]2, substituted phenyl, —OCH 2 -substituted phenyl, pyrazolyl, or —N(phenyl) 2 ;  
         R 5  and R 6  are independently hydrogen, —CO 2 H, —NO 2 , —OCH 3 , imidazolyl, —CN, fluorine, —CH 3 , —CF 3 , or pyrrolyl;  
         R 8  is COOH or tetrazolyl;  
         or the pharmaceutically acceptable salts thereof.  
       
     
     
         9 . The method of  claim 1  wherein the compound of Formula I is: 
 2-[[4-[2-(3,4-Dichlorophenyl)ethyl]phenyl]amino-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]phenylamino}-5-nitrobenzoic acid;  
 2-{4-[4-(3,4-Dichloro-phenyl)-ethyl]phenylamino}-4-methoxy-5-nitrobenzoic acid;  
 2-{4-[2-(3,4-Dihydroxy-phenyl)-ethyl]-phenylamino}benzoic acid;  
 2-{4-[2-(4-Dibutylamino-phenyl)-ethyl]phenylamino}benzoic acid;  
 2-{4-[2-(3,4,5-Trihydroxy-phenyl)-ethyl]phenylamino}benzoic acid;  
 2-{4-[3-(3,4-Dichlorophenyl)propyl]phenylamino}-4-methoxy-5-nitrobenzoic acid;  
 2-{4-[3-(3,4-Dichlorophenyl)propyl]phenylamino}-4-imidazo-1-yl-5-nitrobenzoic acid;  
 2-{4-[3-(3,4-Dichlorophenyl)-propyl]phenylamino}benzoic acid;  
 2-{4-[4-(3,4-Dichlorophenyl)butyl]phenylamino}benzoic acid;  
 2-{4-[4-(3,4-Dichloro-phenyl)-butyl]-phenylamino}-5-nitro-benzoic acid;  
 2-{4-[4-(3,4-Dichlorophenyl)-butyl]phenylamino}-3,5-dinitrobenzoic acid;  
 2-{4-[5-(3,4-Dichlorophenyl)pentyl]phenylamino}-5-nitrobenzoic acid;  
 2-{4-[5-(3,4-Dichloro-phenyl)pentyl]phenylamino}-4-methoxy-5-nitrobenzoic acid;  
 2-[4-(3,4-Dichloro-benzyl)-phenylamino]-benzoic acid;  
 2-{4-[2-(3,4-Dimethyl-phenyl)-ethyl]-phenylamino}-5-nitro-benzoic acid;  
 2-{4-[2-(3,4-Difluoro-phenyl)-ethyl]-phenylamino}-5-nitro-benzoic acid;  
 2-{4-[2-(4-Chloro-3-trifluoromethyl-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-[4-(2-Biphenyl-4-yl-ethyl)-phenylamino]-5-nitro-benzoic acid;  
 5-Nitro-2-(4-phenethyl-phenylamino)-benzoic acid;  
 2-(4-Phenethyl-phenylamino)-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-5-methoxy-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-terephthalic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-5-methyl-benzoic acid;  
 4-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-isophthalic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-5-methanesulfonyl-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-5-imidazol-1-yl-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-6-nitro-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-4-nitro-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-3-nitro-benzoic acid;  
 5-Cyano-2-{4-[2-(3,4-dichloro-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-4,6-difluoro-benzoic acid;  
 6-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-2,3-difluoro-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-6-fluoro-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-3-fluoro-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-3-methyl-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-4-fluoro-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-3,5-difluoro-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-3-trifluoromethyl-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-6-trifluoromethyl-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-5-trifluoromethyl-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-5-pyrrol-1-yl-benzoic acid;  
 2-{4-[2-(4-Benzyloxy-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-(4-{2-[4-(3-Dimethylamino-propoxy)-phenyl]-ethyl}-phenylamino)-benzoic acid;  
 2-{4-[2-(4-Diethylamino-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-{4-[2-(4-Phenoxy-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-{4-[2-(4-Octyloxy-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-(4-{2-[4-(2-Ethoxy-1-ethoxymethyl-ethyl)-phenyl]-ethyl}-phenylamino)-benzoic acid;  
 2-{4-[2-(4-Pyrrol-1-yl-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-{4-[2-(4-Styryl-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-{4-[2-(4-Dibutylamino-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-{4-[2-(4′-Ethyl-biphenyl-4-yl)-ethyl]-phenylamino}-benzoic acid;  
 2-{4-[2-(4-Octyl-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-(4-{2-[3-(3,5-Dichloro-phenoxy)-phenyl]-ethyl}-phenylamino)-benzoic acid;  
 2-(4-{2-[4-(2-Chloro-6-fluoro-benzyloxy)-phenyl]-ethyl}-phenylamino)-benzoic acid;  
 2-{4-[2-(4-Pyrazol-1-yl-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-{4-[2-(4-Diphenylamino-phenyl)-ethyl]-phenylamino}-benzoic acid;  
 2-(4-{2-[4-(3,4-Dichloro-benzyloxy)-phenyl]-ethyl}-phenylamino)-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-5-amino-benzoic acid;  
 2-{4-[2-(3,4-Dichloro-phenyl)-ethyl]-phenylamino}-5-trifluoromethyl-benzoic acid;  
 2-{4-[2-(3,4-Dichlorophenyl)]phenylamino}-5-nitrobenzoic acid;  
 2-{4-[3-(3,4-Dichlorophenyl)propyl]phenylamino}-5-nitrobenzoic acid;  
 2-{4-[2-(3,4-Dimethyl-phenyl)-ethyl]phenylamino}-5-nitrobenzoic acid;  
 2-[[4-[2-(4-Chloro-3-trifluoromethylphenyl)ethyl]phenyl]amino-benzoic acid; or  
 2-[4-(3,4-Dichlorophenyl)phenyl]aminobenzoic acid.  
 
     
     
         10 . A method of inhibiting the aggregation of amyloid proteins to form amyloid deposits, the method comprising administering to a patient in need of inhibition of the aggregation of amyloid protein an amyloid protein aggregation inhibiting amount of a compound of Formula I  
       
         
           
           
               
               
           
         
         wherein  
         R a  is hydrogen, C 1 -C 6  alkyl, or  
         
           
             
             
                 
                 
             
           
         
         n is 0 to 5 inclusive;  
         R 1 , R 2 , R 3 , R 4 , R 5 , R 6 , and R 7  are independently hydrogen, halogen, —OH, —NH 2 , NR b R c , —CO 2 H, —CO 2 C 1 -C 6  alkyl, —NO 2 , —OC 1 -C 12  alkyl, —C 1 -C 8  alkyl, —CF 3 , —CN, —OCH 2  phenyl, —OCH 2 -substituted phenyl, —(CH 2 ) m -phenyl, —O-phenyl, —O-substituted phenyl, 
 —CH═CH-phenyl, —O(CH 2 ) p NR b R c ,  
                     
 —NH(CH 2 ) p NR b R c , —N(C 1 -C 6 alkyl)(CH 2 ) p NR b R c ,  
                     
 
         R 8  is COOH, tetrazolyl, —SO 2 R d , or —CONHSO 2 R d ;  
         R b  and R c  are independently hydrogen, —C 1 -C 6  alkyl, —(CH 2 ) m -phenyl, or R b  and R C  taken together with the nitrogen atom to which they are attached form a cyclic ring selected from piperidinyl, pyrrolyl, imidazolyl, piperazinyl, 4-C 1 -C 6  alkylpiperazinyl, morpholino, thiomorpholino, decahydroisoquinoline, or pyrazolyl;  
         R d  is hydrogen, —C 1 -C 6  alkyl, —CF 3 , or phenyl;  
         m is 0 to 5 inclusive;  
         p is 1 to 5 inclusive;  
         A is N;  
         R 1  and R 2 , when adjacent to one another, can be methylene-dioxy;  
         or the pharmaceutically acceptable salts thereof.  
       
     
     
         11 . The method of  claim 10  wherein 
 R a  is hydrogen;  
 n is 2; and  
 R 3  and R 4  are hydrogen.  
 
     
     
         12 . The method of  claim 10  wherein 
 R a  is hydrogen;  
 R 3  and R 4  are hydrogen; and  
 n is 2 to 5 inclusive.  
 
     
     
         13 . The method of  claim 10  wherein 
 R a  is hydrogen;  
 n is 2;  
 R 3  and R 4  are hydrogen; and  
 R 1 , R 2 , and R 7  are independently chlorine, —N(CH 2 CH 3 ) 2 , —OH, CH 3 —, fluorine, —CF 3 , phenyl, hydrogen, —OCH 2  phenyl, —O(CH 2 ) 3 N(CH 3 ) 2 , —O phenyl, —O(CH 2 ) 7 CH 3 , —CH(CH 2 OCH 2 CH 3 ) 2 , pyrrolyl, —CH═CH-phenyl,  
                     —N[(CH 2 ) 3 CH 3 ] 2 , substituted phenyl, —OCH 2 -substituted phenyl, pyrazolyl, or    —N(phenyl) 2 .    
 
     
     
         14 . The method of  claim 10  wherein 
 R a  is hydrogen;  
 n is 3, 4, or 5;  
 R 3  and R 4  are hydrogen; and  
 R 1 , R 2 , and R 7  are independently chlorine or hydrogen.  
 
     
     
         15 . The method of  claim 10  wherein 
 R a  is hydrogen;  
 n is 2;  
 R 3  and R 4  are hydrogen; and  
 R 5  and R 6  are independently hydrogen, —CO 2 H, —NO 2 , —OCH 3 , imidazolyl, —CN, fluorine, —CH 3 , —CF 3 , halogen,  
 —NH—C 1 -C 6  alkyl, —N(C 1 -C 6 alkyl) 2 , —NH 2 , or pyrrolyl.  
 
     
     
         16 . The method of  claim 10  wherein 
 R a  is hydrogen;  
 n is 2;  
 R 3  and R 4  are hydrogen; and  
 R 8  is —CO 2 H.  
 
     
     
         17 . A method of inhibiting the aggregation of amyloid proteins to form amyloid deposits, the method comprising administering to a patient in need of inhibition of the aggregation of amyloid protein an amyloid protein aggregation inhibiting amount of a compound of Formula I  
       
         
           
           
               
               
           
         
       
       wherein  
       R a  is hydrogen; 
 n is 1 to 5 inclusive;  
 R 3  and R 4  are hydrogen;  
 R 1 , R 7 , and R 2  are independently chlorine, —N(CH 2 CH 3 ) 2 , —OH, CH 3 —, fluorine, —CF 3 , phenyl, hydrogen, —OCH 2  phenyl, —O(CH 2 ) 3 N(CH 3 ) 2 , —O phenyl, —O(CH 2 ) 7 CH 3 , —CH(CH 2 OCH 2 CH 3 ) 2 , pyrrolyl, —CH═CH-phenyl, —N[(CH 2 ) 3 CH 3 ]2, substituted phenyl, —OCH 2 -substituted phenyl, pyrazolyl, or —N(phenyl) 2 ;  
 R 5  and R 6  are independently hydrogen, —CO 2 H, —NO 2 , —OCH 3 , imidazolyl, —CN, fluorine, —CH 3 , —CF 3 , or pyrrolyl;  
 R 8  is COOH or tetrazolyl;  
 A is N;  
 R 1  and R 2 , when adjacent to one another, can be methylene-dioxy;  
 or the pharmaceutically acceptable salts thereof.  
 
     
     
         18 - 21 . (Cancelled).  
     
     
         22 . The compounds: 
 4-{4-[2-(3,4-Dicloro-phenyl)-ethyl]-phenylamino}-nicotinic acid.    
     
     
         23 - 27 . (Cancelled).  
     
     
         28 . A method of imaging amyloid deposits, the method comprising: 
 a. introducing into a patient a detectable quantity of a labeled compound having the Formula I or a pharmaceutically acceptable salt thereof:                           wherein 
 R a  is hydrogen, C 1 -C 6  alkyl, or  
                     
 n is 0 to 5 inclusive;  
 R 1 , R 2 , R 3 , R 4 , R 5 , R 6 , and R 7  are independently hydrogen, halogen, —OH, —NH 2 , NR b R c , —CO 2 H, —CO 2 C 1 -C 6  alkyl, —NO 2 , —OC 1 -C 12  alkyl, —C 1 -C 8  alkyl, —CF 3 , —CN, —OCH 2  phenyl, —OCH 2 -substituted phenyl, —(CH 2 ) m -phenyl, —O-phenyl, —O-substituted phenyl, 
 —CH═CH-phenyl, —O(CH 2 ) p NR b R c ,  
                     
 —NH(CH 2 ) p NR b R c , —N(C 1 -C 6 alkyl)(CH 2 ) p NR b R c ,  
                     
 
 R 8  is COOH, tetrazolyl, —SO 2 R d , or —CONHSO 2 R d ;  
 R b  and R c  are independently hydrogen, —C 1 -C 6  alkyl, —(CH 2 ) m -phenyl, or R b  and R c  taken together with the nitrogen atom to which they are attached form a cyclic ring selected from piperidinyl, pyrrolyl, imidazolyl, piperazinyl, 4-C 1 -C 6  alkylpiperazinyl, morpholino, thiomorpholino, decahydroisoquinoline, or pyrazolyl;  
 R d  is hydrogen, —C 1 -C 6  alkyl, —CF 3 , or phenyl;  
 m is 0 to 5 inclusive;  
 p is 1 to 5 inclusive;  
 A is CH or N;  
 R 1  and R 2 , when adjacent to one another, can be methylene-dioxy;  
    or the pharmaceutically acceptable salts thereof.    b. allowing sufficient time for the labeled compound to become associated with amyloid deposits; and    c. detecting the labeled compound associated with the amyloid deposits.    
     
     
         29 . The method of  claim 28  wherein the patient has or is suspected to have Alzheimer's disease.  
     
     
         30 . The method of  claim 28  wherein the labeled compound is a radio labeled compound.  
     
     
         31 . The method of  claim 28  wherein the labeled compound is detected using MRI.  
     
     
         32 - 41 . (Cancelled).  
     
     
         42 . A compound of Formula I.  
       
         
           
           
               
               
           
         
         wherein  
         R a  is hydrogen, C 1 -C 6  alkyl, or  
         
           
             
             
                 
                 
             
           
         
         n is 0 to 5 inclusive;  
         R 1 , R 2 , R 3 , R 4 , R 5 , R 6 , and R 7  are independently hydrogen, halogen, —OH, —NH 2 , NR b R c , —CO 2 H, —CO 2 C 1 -C 6  alkyl, —NO 2 , —OC 1 -C 12  alkyl, —C 1 -C 8  alkyl, —CF 3 , —CN, —OCH 2  phenyl, —OCH 2 -substituted phenyl, —(CH 2 ) m -phenyl, —O-phenyl, —O-substituted phenyl, 
 —CH═CH-phenyl, —O(CH 2 ) p NR b R c ,  
                     
 —NH(CH 2 ) p NR b R c , —N(C 1 -C 6 alkyl)(CH 2 ) p NR b R c ,  
                     
 
         R 8  is COOH, tetrazolyl, —SO 2 R d , or —CONHSO 2 R d ;  
         R b  and R c  are independently hydrogen, —C 1 -C 6  alkyl, —(CH 2 ) m -phenyl; or R b  and R c  taken together with the nitrogen atom to which they are attached form a cyclic ring selected from piperidinyl, pyrrolyl, imidazolyl, piperazinyl, 4-C 1 -C 6  alkylpiperazinyl, morpholino, thiomorpholino, decahydroisoquinoline, or pyrazolyl;  
         R d  is hydrogen, —C 1 -C 6  alkyl, —CF 3 , or phenyl;  
         m is 0 to 5 inclusive;  
         p is 1 to 5 inclusive;  
         A is CH or N;  
         R 1  and R 2 , when adjacent to one another, can be methylene-dioxy;  
         or the pharmaceutically acceptable salts thereof.  
       
     
     
         43 . A pharmaceutical formulation comprising a compound of  claim 42  admixed with a pharmaceutically acceptable diluent, excipient, or carrier therefor.

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