US2017247324A1PendingUtilityA1

Aldehyde capture ligation technology for synthesis of amide bonds

Assignee: UNIV NEW YORKPriority: Dec 26, 2013Filed: Mar 13, 2017Published: Aug 31, 2017
Est. expiryDec 26, 2033(~7.4 yrs left)· nominal 20-yr term from priority
C07K 5/0806C07K 1/1075C07C 231/10C07D 207/16C07K 7/06C07C 231/12C07C 391/02C07K 5/06165C07K 5/06034C07C 319/12C07D 209/20C07K 5/06026C07K 5/1008C07D 233/64C07K 5/06078C07C 2603/10C07K 5/0808C07K 5/06052C07C 245/08
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Claims

Abstract

The present invention relates to ligation agents and their use in making an amide ligation product. Methods of making the ligation agents are also disclosed.

Claims

exact text as granted — not AI-modified
1 . A ligation agent of Formula I: 
       
         
           
           
               
               
           
         
         wherein 
         A is selected from the group consisting of 
       
       
         
           
           
               
               
           
         
       
       fluorescent dyes, and cytotoxic small molecule drugs;
 X is selected from the group consisting of 
 
       
         
           
           
               
               
           
         
       
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —C(O)—Se—X—(CR 4   2 ) m C(O)R 3 ; 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —(CR 4   2 ) m C(O)R 3 ; 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —Se—C(O)-A;
 n is 1-3; 
 m is 0-3; 
 each R 1  is independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, aryl, amino acids, peptides, and protecting groups for the protection of an amine; 
 each R 2  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , —C(O)NR 5 R 6 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, aryl, C 1 -C 6  alkoxy, and amino acid side chains; 
 R 3  is selected from the group consisting of H, C 1 -C 6  alkyl, and aryl; 
 each R 4  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, aryl, and C 1 -C 6  alkoxy; and 
 R 5 , R 6 , R 7 , and R 8  are each independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, and aryl; 
 with the proviso that m is 0-3 when A is (R 1 ) 2 N(C(R 2 ) 2 ) n — and X is 
 
       
         
           
           
               
               
           
         
       
       and with the proviso that m is 0-2 when A is (R 1 ) 2 N(C(R 2 ) 2 ) n — and X is 
       
         
           
           
               
               
           
         
       
     
     
         2 . The ligation agent of  claim 1 , wherein X is 
       
         
           
           
               
               
           
         
       
     
     
         3 . The ligation agent of  claim 2 , wherein the ligation agent is selected from the group consisting of: 
       
         
           
           
               
               
           
         
       
       wherein R 3  is an aryl or an alkyl; 
       
         
           
           
               
               
           
         
       
       wherein R 3  is an aryl or an alkyl. 
     
     
         4 . The ligation agent of  claim 1 , wherein X is 
       
         
           
           
               
               
           
         
       
     
     
         5 . The ligation agent of  claim 4 , wherein the ligation agent is selected from the group consisting of: 
       
         
           
           
               
               
           
         
       
       wherein R 3  is an aryl or an alkyl. 
     
     
         6 - 15 . (canceled) 
     
     
         16 . A compound of Formula II: 
       
         
           
           
               
               
           
         
         wherein 
         each X is selected from the group consisting of 
       
       
         
           
           
               
               
           
         
         each 
       
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —Se—Se—X—(CR 4   2 ) m C(O)R 3 ;
 each 
 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —(CR 4   2 ) m C(O)R 3 ;
 each m is independently 0-3; 
 each R 3  is independently selected from the group consisting of H, C 1 -C 6  alkyl, and aryl; 
 each R 4  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, aryl, and C 1 -C 6  alkoxy; and 
 R 5 , R 6 , R 7 , and R 8  are each independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, and aryl; 
 with the proviso that m is 0-3 when X is 
 
       
         
           
           
               
               
           
         
       
       and with the proviso that m is 0-2 when X is 
       
         
           
           
               
               
           
         
       
     
     
         17 . The compound of  claim 16 , wherein X is 
       
         
           
           
               
               
           
         
       
     
     
         18 . The compound of  claim 17 , wherein the compound is selected from the group consisting of: 
       
         
           
           
               
               
           
         
       
       wherein R 3  is an aryl or an alkyl; 
       
         
           
           
               
               
           
         
       
       wherein R 3  is an aryl or an alkyl. 
     
     
         19 . The compound of  claim 16 , wherein X is 
       
         
           
           
               
               
           
         
       
     
     
         20 . The compound of  claim 19 , wherein the compound is selected from the group consisting of: 
       
         
           
           
               
               
           
         
       
       wherein R 3  is an aryl or an alkyl. 
     
     
         21 . A method of making a ligation agent of Formula I: 
       
         
           
           
               
               
           
         
         wherein 
         A is selected from the group consisting of 
       
       
         
           
           
               
               
           
         
       
       fluorescent dyes, and cytotoxic small molecule drugs;
 X is selected from the group consisting of 
 
       
         
           
           
               
               
           
         
       
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —C(O)—Se—X—(CR 4   2 ) m C(O)R 3 ; 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —(CR 4   2 ) m C(O)R 3 ; 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —Se—C(O)-A;
 n is 1-3; 
 m is 0-3; 
 each R 1  is independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, aryl, amino acids, peptides, and protecting groups for the protection of an amine; 
 each R 2  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , —C(O)NR 5 R 6 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, aryl, C 1 -C 6  alkoxy, and amino acid side chains; 
 R 3  is selected from the group consisting of H, C 1 -C 6  alkyl, and aryl; 
 each R 4  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, aryl, and C 1 -C 6  alkoxy; and 
 R 5 , R 6 , R 7 , and R 8  are each independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, and aryl; 
 with the proviso that m is 0-3 when A is (R 1 ) 2 N(C(R 2 ) 2 ) n — and X is 
 
       
         
           
           
               
               
           
         
       
       and with the proviso that m is 0-2 when A is (R 1 ) 2 N(C(R 2 ) 2 ) n — and X is 
       
         
           
           
               
               
           
         
         said method comprising:
 (i) providing a compound of Formula II: 
 
       
       
         
           
           
               
               
           
         
         
           
             wherein 
             each X is selected from the group consisting of 
           
         
       
       
         
           
           
               
               
           
         
         
           
             each 
           
         
       
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —Se—Se—X—(CR 4   2 ) m C(O)R 3 ;
     each     
 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to (CR 4   2 ) m C(O)R 3 ;
     each m is independently 0-3;   each R 3  is independently selected from the group consisting of H, C 1 -C 6  alkyl, and aryl;   each R 4  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, aryl, and C 1 -C 6  alkoxy; and   R 5 , R 6 , R 7 , and R 8  are each independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, and aryl;   with the proviso that m is 0-3 when X is     
 
       
         
           
           
               
               
           
         
       
       and
     with the proviso that m is 0-2 when X is     
 
       
         
           
           
               
               
           
         
         
           (ii) (a) providing a compound of Formula III: 
         
       
       
         
           
           
               
               
           
         
         
           
             wherein 
             A is selected from the group consisting of 
           
         
       
       
         
           
           
               
               
           
         
       
       fluorescent dyes, and cytotoxic small molecule drugs; 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —C(O)—OH;
     n is 1-3;   each R 1  is independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, aryl, amino acids, peptides, and protecting groups for the protection of an amine; and   each R 2  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , —C(O)NR 5 R 6 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, aryl, C 1 -C 6  alkoxy, and amino acid side chains;   each R 4  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, aryl, and C 1 -C 6  alkoxy; and   R 5 , R 6 , R 7 , and R 8  are each independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, and aryl; or     (ii) (b) providing a compound of Formula III′:   
 
       
         
           
           
               
               
           
         
         
           
             wherein 
             A is selected from the group consisting of 
           
         
       
       
         
           
           
               
               
           
         
       
       fluorescent dyes, and cytotoxic small molecule drugs;
     Y is selected from the group consisting of O, S, Se, a good leaving group, and Dawson's auxiliary;   Y′ is optionally present and, if present, is a C 1 -C 6  alkyl, an ester, or an amide;     
 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to 
       
         
           
           
               
               
           
         
       
       
         
           
           
               
               
           
         
       
       is a solid support;
     n is 1-3;   each R 1  is independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, aryl, amino acids, peptides, and protecting groups for the protection of an amine; and   each R 2  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , —C(O)NR 5 R 6 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, aryl, C 1 -C 6  alkoxy, and amino acid side chains;   each R 4  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, aryl, and C 1 -C 6  alkoxy; and   R 5 , R 6 , R 7 , and R 8  are each independently selected from the group consisting of H, C 1 -C 6  alkyl, C 2 -C 6  alkenyl, C 2 -C 6  alkynyl, and aryl; and     (iii) reacting the compound of Formula II with the compound of Formula III or the compound of Formula III′ under conditions effective to make a ligation agent of Formula I.   
 
     
     
         22 . The method of  claim 21 , wherein said providing a compound of Formula II comprises:
 providing a substituted halogenated benzene aldehyde or substituted halogenated benzene ketone; and   reacting the substituted halogenated benzene aldehyde or substituted halogenated benzene ketone with a diselenide in the presence of a cation scavenger under conditions effective to produce a compound of Formula II.   
     
     
         23 . The method of  claim 22 , wherein the substituted halogenated benzene aldehyde or substituted halogenated benzene ketone is a compound of Formula IV: 
       
         
           
           
               
               
           
         
         wherein 
         X is selected from the group consisting of 
       
       
         
           
           
               
               
           
         
       
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —X′; 
       
         
           
           
               
               
           
         
       
       represents a point of attachment to —(CR 4   2 ) m C(O)R 3 ;
 X′ is a halogen; 
 each m is independently 0-3; 
 each R 3  is independently selected from the group consisting of H, C 1 -C 6  alkyl, and aryl; and 
 each R 4  is independently selected from the group consisting of H, —C(O)R 7 , —C(O)OR 8 , NO 2 , —NR 5 R 6 , halogen, OH, C 1 -C 6  alkyl, aryl, and C 1 -C 6  alkoxy. 
 
     
     
         24 . The method of  claim 22 , wherein the diselenide is an alkaline metal diselenide. 
     
     
         25 . The method of  claim 22 , wherein the cation scavenger is selected from the group consisting of HMPA, DMPU, DMI, tetraalkyl ureas, and cyclic alkyl ureas. 
     
     
         26 . The method of  claim 21 , wherein a compound of Formula III is provided. 
     
     
         27 . The method of  claim 21 , wherein a compound of Formula III′ is provided. 
     
     
         28 . The method of  claim 27 , wherein the solid support is selected from the group consisting of a Tenta gel, Rink amide resin, Merrifield resin, trityl resin, PAM resin, and Kaiser resin.

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