US2018170918A1PendingUtilityA1

Methods of synthesizing a difluorolactam analog

54
Assignee: CAYMAN CHEMICAL CO INCPriority: Mar 15, 2013Filed: Jan 30, 2018Published: Jun 21, 2018
Est. expiryMar 15, 2033(~6.7 yrs left)· nominal 20-yr term from priority
A61P 43/00A61P 25/04A61P 27/06C07D 207/273C07D 333/38C07D 409/06A61P 19/10C07F 9/4006C07D 498/04C07B 39/00
54
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Claims

Abstract

The present invention relates to processes and intermediates for preparing compounds of formula (IA), wherein R 1 , R 4 , R 5 , R 6 , and L 1 are as defined herein. Compounds of formula (IA) have been found useful as EP 4 receptor agonists useful in the treatment of glaucoma, osteoporosis, neuropathic pain, and related disorders.

Claims

exact text as granted — not AI-modified
We claim: 
     
         1 . A method of preparing a compound of formula (IA) 
       
         
           
           
               
               
           
         
         or a pharmaceutically acceptable salt thereof wherein: 
         L 1  is
 a) C 3 -C 7 alkylene, C 3 -C 7 alkenylene, or C 3 -C 7 alkynylene; or 
 b) —(CH 2 ) n1 -G 2 -(CH 2 ) p —, —(CH 2 ) n2 —C≡C-G 2 -, or —(CH 2 ) n2 —C(R 12 )═C(R 12 )-G 2 -, wherein n1 is 2, 3, 4, or 5, n2 is 1, 2, or 3, p is 0, 1, 2, or 3, and n1+p=2, 3, 4, 5, or 6; 
 
         G 2  is 
       
       
         
           
           
               
               
           
         
         R 1  is a carboxylic acid or a protected carboxylic acid; 
         R 12 , at each occurrence, is independently H or C 1 -C 4 alkyl; 
         R 4  and R 5  are each independently H or C 1 -C 4  alkyl; or R 4  and R 5  together with the carbon to which they are attached form a C 3 -C 5  cycloalkyl; 
         R 6  is aryl, heteroaryl, C 3 -C 10 alkyl, C 3 -C 10 alkenyl, C 3 -C 10 alkynyl, C 3 -C 10 haloalkyl, C 3 -C 10 haloalkenyl, C 3 -C 10 haloalkynyl, or L 3 -R 7 ; wherein the aryl and heteroaryl are optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy; and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; 
         L 3  is C 1 -C 6 alkylene, C 2 -C 6 alkenylene, C 2 -C 6 alkynylene; and 
         R 7  is C 3 -C 8 cycloalkyl, aryl, heteroaryl, or heterocyclyl; wherein R 7  is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; 
         the method comprising reacting a compound of formula (10), 
       
       
         
           
           
               
               
           
         
         with a carbonyl-reducing agent; and when R 1  is a protected carboxylic acid, optionally deprotecting the protected carboxylic acid. 
       
     
     
         2 . The method of  claim 1  wherein:
 L 1  is n-hexylene, —(CH 2 ) 3 -G 2 -, —CH 2 —C≡C-G 2 -, or —CH 2 —C(H)═C(H)-G 2 -; 
 G 2  is 
 
       
         
           
           
               
               
           
         
         R 4  and R 5  are each independently H or C 1 -C 4  alkyl; 
         R 6  is phenyl, C 3 -C 10 alkyl, C 3 -C 10 alkenyl, C 3 -C 10 alkynyl, C 3 -C 10 haloalkyl, C 3 -C 10 haloalkenyl, C 3 -C 10 haloalkynyl, or L 3 -R 7 ; wherein the phenyl is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; and 
         R 7  is phenyl, which is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy. 
       
     
     
         3 . The method of  claim 2  wherein:
 L 1  is —(CH 2 ) 3 -G 2 -; 
 G 2  is 
 
       
         
           
           
               
               
           
         
         R 4  and R 5  are each independently H or methyl; 
         R 6  is —CH 2 —C≡C—C 1 -C 4 alkyl or L 3 -R 7 ; 
         L 3  is C 3 -C 6 alkylene; and 
         R 7  is phenyl. 
       
     
     
         4 . The method of  claim 3  wherein R 4  is methyl and R 5  is H. 
     
     
         5 . The method of  claim 3  wherein R 4  is H and R 5  is methyl. 
     
     
         6 . The method of any of  claims 1 - 5  wherein the carbonyl-reducing agent comprises a mixture of 
       
         
           
           
               
               
           
         
       
       and catecholborane. 
     
     
         7 . The method of any of  claims 1 - 5  further comprising reacting a compound of formula (8) with a compound of formula (9) in the presence of a trialkylamine base and lithium chloride to produce the compound of formula (10), wherein R 1  is a protected carboxylic acid; and R 15  is C 1 -C 6 alkyl. 
       
         
           
           
               
               
           
         
       
     
     
         8 . The method of  claim 7  further comprising reacting a compound of formula (7) with an oxidizing agent to produce the compound of formula (8). 
       
         
           
           
               
               
           
         
       
     
     
         9 . The method of  claim 8  wherein the oxidizing agent is Dess-Martin periodinane. 
     
     
         10 . The method of  claim 8  further comprising removing a protecting group PG from a compound of formula (6) to produce the compound of formula (7). 
       
         
           
           
               
               
           
         
       
     
     
         11 . The method of  claim 10  wherein PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         12 . The method of  claim 10  further comprising reacting a compound of formula (5) with a base and a compound of formula X 1 -L 1 -R 1  to produce the compound of formula (6), wherein X 1  is a leaving group selected from the group consisting of bromo, chloro, iodo, an alkylsulfonate, a fluoroalkylsulfonate, and an arylsulfonate. 
       
         
           
           
               
               
           
         
       
     
     
         13 . The method of  claim 12  wherein the base is lithium hydride, sodium hydride, or potassium hydride; PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         14 . The method of  claim 12  further comprising adding a protecting group PG to a compound of formula (4) to produce the compound of formula (5). 
       
         
           
           
               
               
           
         
       
     
     
         15 . The method of  claim 14  wherein PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         16 . A method of preparing a compound of formula (10) comprising reacting a compound of formula (8) with a compound of formula (9) in the presence of a trialkylamine base and lithium chloride; 
       
         
           
           
               
               
           
         
         wherein: 
         L 1  is
 a) C 3 -C 7 alkylene, C 3 -C 7 alkenylene, or C 3 -C 7 alkynylene; or 
 b) —(CH 2 ) n1 -G 2 -(CH 2 ) p —, —(CH 2 ) n2 —C≡C-G 2 -, or —(CH 2 ) n2 —C(R 12 )═C(R 12 )-G 2 -, wherein n1 is 2, 3, 4, or 5, n2 is 1, 2, or 3, p is 0, 1, 2, or 3, and n1+p=2, 3, 4, 5, or 6; 
 
         G 2  is 
       
       
         
           
           
               
               
           
         
         R 1  is a protected carboxylic acid; 
         R 12 , at each occurrence, is independently H or C 1 -C 4 alkyl; 
         R 4  and R 5  are each independently H or C 1 -C 4  alkyl; or R 4  and R 5  together with the carbon to which they are attached form a C 3 -C 5  cycloalkyl; 
         R 6  is aryl, heteroaryl, C 3 -C 10 alkyl, C 3 -C 10 alkenyl, C 3 -C 10 alkynyl, C 3 -C 10 haloalkyl, C 3 -C 10 haloalkenyl, C 3 -C 10 haloalkynyl, or L 3 -R 7 ; wherein the aryl and heteroaryl are optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy; and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; 
         L 3  is C 1 -C 6 alkylene, C 2 -C 6 alkenylene, C 2 -C 6 alkynylene; 
         R 7  is C 3 -C 8 cycloalkyl, aryl, heteroaryl, or heterocyclyl; wherein R 7  is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3  alkylene-C 1 -C 3 alkoxy; and 
         R 15  is C 1 -C 6 alkyl. 
       
     
     
         17 . The method of  claim 16  wherein:
 L 1  is n-hexylene, —(CH 2 ) 3 -G 2 -, —CH 2 —C≡C-G 2 -, or —CH 2 —C(H)═C(H)-G 2 -; 
 G 2  is 
 
       
         
           
           
               
               
           
         
         R 4  and R 5  are each independently H or C 1 -C 4  alkyl; 
         R 6  is phenyl, C 3 -C 10 alkyl, C 3 -C 10 alkenyl, C 3 -C 10 alkynyl, C 3 -C 10 haloalkyl, C 3 -C 10 haloalkenyl, C 3 -C 10 haloalkynyl, or L 3 -R 7 ; wherein the phenyl is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; and 
         R 7  is phenyl, which is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy. 
       
     
     
         18 . The method of  claim 17  wherein:
 L 1  is —(CH 2 ) 3 -G 2 -; 
 R 4  and R 5  are each independently H or methyl; 
 R 6  is —CH 2 —C≡C—C 1 -C 4 alkyl or L 3 -R 7 ; 
 L 3  is C 3 -C 6 alkylene; and 
 R 7  is phenyl. 
 
     
     
         19 . The method of any of  claims 16 - 18  further comprising reacting a compound of formula (7) with an oxidizing agent to produce the compound of formula (8). 
       
         
           
           
               
               
           
         
       
     
     
         20 . The method of  claim 19  wherein the oxidizing agent is Dess-Martin periodinane. 
     
     
         21 . The method of  claim 19  further comprising removing a protecting group PG from a compound of formula (6) to produce the compound of formula (7). 
       
         
           
           
               
               
           
         
       
     
     
         22 . The method of  claim 21  wherein PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         23 . The method of  claim 21  further comprising reacting a compound of formula (5) with a base and a compound of formula X 1 -L 1 -R 1  to produce the compound of formula (6), wherein X 1  is a leaving group selected from the group consisting of bromo, chloro, iodo, an alkylsulfonate, a fluoroalkylsulfonate, and an arylsulfonate. 
       
         
           
           
               
               
           
         
       
     
     
         24 . The method of  claim 23  wherein the base is lithium hydride, sodium hydride, or potassium hydride; PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         25 . The method of  claim 23  further comprising adding a protecting group PG to a compound of formula (4) to produce the compound of formula (5). 
       
         
           
           
               
               
           
         
       
     
     
         26 . The method of  claim 25  wherein PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         27 . A method of preparing a compound of formula (8), comprising reacting a compound of formula (7) with an oxidizing agent, 
       
         
           
           
               
               
           
         
         wherein: 
         L 1  is
 a) C 3 -C 7 alkylene, C 3 -C 7 alkenylene, or C 3 -C 7 alkynylene; or 
 b) —(CH 2 ) n1 -G 2 -(CH 2 ) p —, —(CH 2 ) n2 —C≡C-G 2 -, or —(CH 2 ) n2 —C(R 12 )═C(R 12 )-G 2 -, wherein n1 is 2, 3, 4, or 5, n2 is 1, 2, or 3, p is 0, 1, 2, or 3, and n1+p=2, 3, 4, 5, or 6; 
 
         G 2  is 
       
       
         
           
           
               
               
           
         
         R 1  is a protected carboxylic acid; and 
         R 12 , at each occurrence, is independently H or C 1 -C 4 alkyl. 
       
     
     
         28 . The method of  claim 27  wherein:
 L 1  is n-hexylene, —(CH 2 ) 3 -G 2 -, —CH 2 —C≡C-G 2 -, or —CH 2 —C(H)═C(H)-G 2 -; and 
 G 2  is 
 
       
         
           
           
               
               
           
         
       
     
     
         29 . The method of  claim 28  wherein:
 L 1  is —(CH 2 ) 3 -G 2 -. 
 
     
     
         30 . The method of any of  claims 27 - 29  wherein the oxidizing agent is Dess-Martin periodinane. 
     
     
         31 . The method of any of  claims 27 - 29  further comprising removing a protecting group PG from a compound of formula (6) to produce the compound of formula (7). 
       
         
           
           
               
               
           
         
       
     
     
         32 . The method of  claim 31  wherein PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         33 . The method of  claim 32  wherein PG is —Si(R 21 ) 3  and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         34 . The method of  claim 31  further comprising reacting a compound of formula (5) with a base and a compound of formula X 1 -L 1 -R 1  to produce the compound of formula (6), wherein X 1  is a leaving group selected from the group consisting of bromo, chloro, iodo, an alkylsulfonate, a fluoroalkylsulfonate, and an arylsulfonate. 
       
         
           
           
               
               
           
         
       
     
     
         35 . The method of  claim 34  wherein the base is sodium hydride, lithium hydride, or potassium hydride; PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         36 . The method of  claim 34  further comprising adding a protecting group PG to a compound of formula (4) to produce the compound of formula (5). 
       
         
           
           
               
               
           
         
       
     
     
         37 . The method of  claim 36  wherein PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         38 . The method of  claim 37  wherein PG is —Si(R 21 ) 3  and R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
     
     
         39 . A method of preparing a compound of formula (6) comprising reacting a compound of formula (5) with a base and a compound of formula X 1 -L 1 -R 1 , 
       
         
           
           
               
               
           
         
         wherein: 
         X 1  is a leaving group selected from the group consisting of bromo, chloro, iodo, an alkylsulfonate, a fluoroalkylsulfonate, and an arylsulfonate; 
         PG is a protecting group; 
         L 1  is
 a) C 3 -C 7 alkylene, C 3 -C 7 alkenylene, or C 3 -C 7 alkynylene; or 
 b) —(CH 2 ) n1 -G 2 -(CH 2 ) p —, —(CH 2 ) n2 —C≡C-G 2 -, or —(CH 2 ) n2 —C(R 12 )═C(R 12 )-G 2 -, wherein n1 is 2, 3, 4, or 5, n2 is 1, 2, or 3, p is 0, 1, 2, or 3, and n1+p=2, 3, 4, 5, or 6; 
 
         G 2  is 
       
       
         
           
           
               
               
           
         
         R 1  is a protected carboxylic acid; and 
         R 12 , at each occurrence, is independently H or C 1 -C 4 alkyl. 
       
     
     
         40 . The method of  claim 39  wherein:
 L 1  is n-hexylene, —(CH 2 ) 3 -G 2 -, —CH 2 —C≡C-G 2 -, or —CH 2 —C(H)═C(H)-G 2 -; 
 G 2  is 
 
       
         
           
           
               
               
           
         
         PG is —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and 
         R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
       
     
     
         41 . The method of  claim 40  wherein:
 L 1  is —(CH 2 ) 3 -G 2 -; and 
 PG is —Si(R 21 ) 3 . 
 
     
     
         42 . The method of any one of  claims 39 - 41  wherein the base is sodium hydride, lithium hydride, or potassium hydride. 
     
     
         43 . A method of preparing a compound of formula (4) by reacting the compound of formula (2) with an acid, wherein R 13  is independently C 1 -C 3 alkyl or phenyl, or the R 13  groups, together with the carbon to which they are attached, form a C 3 -C 6 cycloalkyl. 
       
         
           
           
               
               
           
         
       
     
     
         44 . The method of  claim 43  wherein the acid is an acidic cation exchange resin. 
     
     
         45 . A method of preparing a compound of formula (2) from a compound of formula (1) comprising reacting a compound of formula (1) with a base and a fluorinating agent, wherein each R 13  is independently C 1 -C 3 alkyl or phenyl, or the R 13  groups, together with the carbon to which they are attached, form a C 3 -C 6 cycloalkyl. 
       
         
           
           
               
               
           
         
       
     
     
         46 . The method of  claim 45  wherein the reacting a compound of formula (1) with a base and a fluorinating agent comprises reacting the compound of formula (1) with a first base and a fluorinating agent and a second base and a fluorinating agent. 
     
     
         47 . The method of  claim 45  wherein the reacting a compound of formula (1) with a base and fluorinating agent comprises:
 adding a solution of sec-butyl lithium in an organic solvent to a solution of the compound of formula (1) in an organic solvent to produce a first reaction mixture; 
 adding N-fluorobenzene sulfonimide to the first reaction mixture to produce a second reaction mixture; 
 adding a solution of a base selected from the group consisting of lithium bis(trimethylsilyl)amide, sodium bis(trimethylsilyl)amide, potassium bis(trimethylsilyl)amide, and lithium diisopropylamide, in an organic solvent to the second reaction mixture to produce a third reaction mixture; and 
 adding N-fluorobenzene sulfonimide to the third reaction mixture. 
 
     
     
         48 . The method of  claim 45  further comprising preparing the compound of formula (1) from a compound of formula (0) by reacting the compound of formula (0) with a compound of formula 
       
         
           
           
               
               
           
         
       
       in the presence of an acid, wherein each R 13  is independently C 1 -C 3 alkyl or phenyl, or the R 13  groups, together with the carbon to which they are attached, form a C 3 -C 6 cycloalkyl; and R 14  is methyl or ethyl. 
       
         
           
           
               
               
           
         
       
     
     
         49 . The method of any of  claims 45 - 48  wherein R 13  is methyl. 
     
     
         50 . A compound of formula (10) 
       
         
           
           
               
               
           
         
         or salts thereof wherein: 
         L 1  is
 a) C 3 -C 7 alkylene, C 3 -C 7 alkenylene, or C 3 -C 7 alkynylene; or 
 b) —(CH 2 ) n1 -G 2 -(CH 2 ) p —, —(CH 2 ) n2 —C≡C-G 2 -, or —(CH 2 ) n2 —C(R 12 )═C(R 12 )-G 2 -, wherein n1 is 2, 3, 4, or 5, n2 is 1, 2, or 3, p is 0, 1, 2, or 3, and n1+p=2, 3, 4, 5, or 6; 
 
         G 2  is 
       
       
         
           
           
               
               
           
         
         R 1  is a carboxylic acid or a protected carboxylic acid; 
         R 12 , at each occurrence, is independently H or C 1 -C 4 alkyl; 
         R 4  and R 5  are each independently H or C 1 -C 4  alkyl; or R 4  and R 5  together with the carbon to which they are attached form a C 3 -C 5  cycloalkyl; 
         R 6  is aryl, heteroaryl, C 3 -C 10 alkyl, C 3 -C 10 alkenyl, C 3 -C 10 alkynyl, C 3 -C 10 haloalkyl, C 3 -C 10 haloalkenyl, C 3 -C 10 haloalkynyl, or L 3 -R 7 ; wherein the aryl and heteroaryl are optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy; and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; 
         L 3  is C 1 -C 6 alkylene, C 2 -C 6 alkenylene, C 2 -C 6 alkynylene; and 
         R 7  is C 3 -C 8 cycloalkyl, aryl, heteroaryl, or heterocyclyl; wherein R 7  is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy. 
       
     
     
         51 . The compound of  claim 50 , or salts thereof, wherein:
 L 1  is n-hexylene, —(CH 2 ) 3 -G 2 -, —CH 2 —C≡C-G 2 -, or —CH 2 —C(H)═C(H)-G 2 -;   G 2  is   
       
         
           
           
               
               
           
         
         R 4  and R 5  are each independently H or C 1 -C 4  alkyl; 
         R 6  is phenyl, C 3 -C 10 alkyl, C 3 -C 10 alkenyl, C 3 -C 10 alkynyl, C 3 -C 10 haloalkyl, C 3 -C 10 haloalkenyl, C 3 -C 10 haloalkynyl, or L 3 -R 7 ; wherein the phenyl is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; and 
         R 7  is phenyl; wherein R 7  is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy. 
       
     
     
         52 . The compound of  claim 51  wherein:
 L 1  is —(CH 2 ) 3 -G 2 -; 
 R 4  is methyl; 
 R 5  is hydrogen; 
 R 6  is —CH 2 —C≡C—C 1 -C 4 alkyl or L 3 -R 7 ; 
 L 3  is C 3 -C 6 alkylene; and 
 R 7  is phenyl. 
 
     
     
         53 . The compound of  claim 51  wherein:
 L 1  is —(CH 2 ) 3 -G 2 -; 
 R 4  is hydrogen; 
 R 5  is methyl; 
 R 6  is —CH 2 —C≡C—C 1 -C 4 alkyl or L 3 -R 7 ; 
 L 3  is C 3 -C 6 alkylene; and 
 R 7  is phenyl. 
 
     
     
         54 . A compound of formula (6.1) 
       
         
           
           
               
               
           
         
         wherein: 
         L 1  is
 a) C 3 -C 7 alkylene, C 3 -C 7 alkenylene, or C 3 -C 7 alkynylene; or 
 b) —(CH 2 ) n1 -G 2 -(CH 2 ) p —, —(CH 2 ) n2 —C≡C-G 2 -, or —(CH 2 ) n2 —C(R 12 )═C(R 12 )-G 2 -, wherein n1 is 2, 3, 4, or 5, n2 is 1, 2, or 3, p is 0, 1, 2, or 3, and n1+p=2, 3, 4, 5, or 6; 
 
         G 2  is 
       
       
         
           
           
               
               
           
         
         R 1  is a protected carboxylic acid; 
         R 12 , at each occurrence, is independently H or C 1 -C 4 alkyl; and 
         R 20  is H or a hydroxyl protecting group. 
       
     
     
         55 . The compound of  claim 54  wherein:
 L 1  is n-hexylene, —(CH 2 ) 3 -G 2 -, —CH 2 —C≡C-G 2 -, or —CH 2 —C(H)═C(H)-G 2 -; 
 G 2  is 
 
       
         
           
           
               
               
           
         
         R 20  is H, —Si(R 21 ) 3 , 1-ethoxyethyl, or tetrahydro-2H-pyran-2-yl; and 
         R 21 , at each occurrence, is independently selected from C 1 -C 4 alkyl and phenyl. 
       
     
     
         56 . The compound of  claim 55  wherein
 L 1  is —(CH 2 ) 3 -G 2 -. 
 
     
     
         57 . A compound of formula (2) 
       
         
           
           
               
               
           
         
         wherein each R 13  is independently C 1 -C 3 alkyl or phenyl, or the R 13  groups, together with the carbon to which they are attached, form a C 3 -C 6 cycloalkyl. 
       
     
     
         58 . The compound of  claim 57  wherein R 13  is methyl. 
     
     
         59 . A compound of formula (9) 
       
         
           
           
               
               
           
         
         wherein: 
         R 4  and R 5  are each independently H or C 1 -C 4  alkyl; or R 4  and R 5  together with the carbon to which they are attached form a C 3 -C 5  cycloalkyl; 
         R 6  is aryl, heteroaryl, C 3 -C 10 alkyl, C 3 -C 10 alkenyl, C 3 -C 10 alkynyl, C 3 -C 10 haloalkyl, C 3 -C 10 haloalkenyl, C 3 -C 10 haloalkynyl, or L 3 -R 7 ; wherein the aryl and heteroaryl are optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy; and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; 
         L 3  is C 1 -C 6 alkylene, C 2 -C 6 alkenylene, C 2 -C 6 alkynylene; 
         R 7  is C 3 -C 8 cycloalkyl, aryl, heteroaryl, or heterocyclyl; wherein R 7  is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; and 
         R 15  is C 1 -C 6 alkyl. 
       
     
     
         60 . The compound of  claim 59  wherein:
 R 4  and R 5  are each independently H or C 1 -C 4  alkyl; 
 R 6  is phenyl, C 3 -C 10 alkyl, C 3 -C 10 alkenyl, C 3 -C 10 alkynyl, C 3 -C 10 haloalkyl, C 3 -C 10 haloalkenyl, C 3 -C 10 haloalkynyl, or L 3 -R 7 ; wherein the phenyl is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy; and 
 R 7  is phenyl; wherein R 7  is optionally substituted with 1, 2, 3, or 4 substituents selected from the group consisting of C 1 -C 4 alkyl, C 1 -C 3 haloalkyl, cyano, halogen, C 1 -C 3 alkoxy, C 1 -C 3 haloalkoxy, and —C 1 -C 3 alkylene-C 1 -C 3 alkoxy. 
 
     
     
         61 . The compound of  claim 60  wherein:
 R 4  is methyl; 
 R 5  is hydrogen; 
 R 6  is —CH 2 —C≡C—C 1 -C 4 alkyl or L 3 -R 7 ; 
 L 3  is C 3 -C 6 alkylene; 
 R 7  is phenyl; and 
 R 15  is methyl or ethyl. 
 
     
     
         62 . The compound of  claim 60  wherein:
 R 4  is hydrogen; 
 R 5  is methyl; 
 R 6  is —CH 2 —C≡C—C 1 -C 4 alkyl or L 3 -R 7 ; 
 L 3  is C 3 -C 6 alkylene; 
 R 7  is phenyl; and 
 R 15  is methyl or ethyl. 
 
     
     
         63 . A compound of formula X 1 -L 1 -R 1 , wherein:
 X 1  is selected from the group consisting of bromo, chloro, iodo, an alkylsulfonate, a fluoroalkylsulfonate, and an arylsulfonate;   L 1  is
 a) C 3 -C 7 alkylene, C 3 -C 7 alkenylene, or C 3 -C 7 alkynylene; or 
 b) —(CH 2 ) n1 -G 2 -(CH 2 ) p —, —(CH 2 ) n2 —C≡C-G 2 -, or —(CH 2 ) n2 —C(R 12 )═C(R 12 )-G 2 -, wherein n1 is 2, 3, 4, or 5, n2 is 1, 2, or 3, p is 0, 1, 2, or 3, and n1+p=2, 3, 4, 5, or 6; 
   G 2  is   
       
         
           
           
               
               
           
         
         R 1  is a protected carboxylic acid; and 
         R 12  is H or C 1 -C 4  alkyl. 
       
     
     
         64 . The compound of  claim 63  wherein:
 L 1  is n-hexylene, —(CH 2 ) 3 -G 2 -, —CH 2 —C≡C-G 2 -, or —CH 2 —C(H)═C(H)-G 2 -; and 
 G 2  is 
 
       
         
           
           
               
               
           
         
       
     
     
         65 . The compound of  claim 64  wherein:
 L 1  is —(CH 2 ) 3 -G 2 -.

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