US2013217640A1PendingUtilityA1

Glycosylated acetaminophen pro-drug

44
Assignee: SHULL BRIANPriority: Jul 22, 2010Filed: Jul 18, 2011Published: Aug 22, 2013
Est. expiryJul 22, 2030(~4 yrs left)· nominal 20-yr term from priority
C07H 15/203A61P 25/04
44
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Claims

Abstract

The present invention relates to methods and compositions for the synthesis, production, and use of pro-drug analogs of the analgesic acetaminophen. This invention relates to a method for the production of a broad group of glycosides of acetaminophen derivatives.

Claims

exact text as granted — not AI-modified
We claim: 
     
         1 . A compound of the formula: 
       
         
           
           
               
               
           
         
         wherein R 1  is an alkyl, alkyl alkanoate, alkenyl, alkynyl, acyl, alkanediyl, aryl, aralkyl, heteroaryl, heteroaralkyl, alkyl oximes (R═CH═NOH), alkyl hydrazones (R═CH═NHNHR), alkyl amines, or a substituted version of any of these groups or a protecting group, phosphates [R═OP(O)(OH) 2 ], sulfonates [R═OS(O) 2 OH], sugar, OH, or H; and R 2  is an alkyl, alkyl alkanoate, alkenyl, alkynyl, acyl, alkanediyl, aryl, aralkyl, heteroaryl, heteroaralkyl, allyl oximes (R═CH═NOH), alkyl hydrazones (R═CH═NHNHR), alkyl amines or a substituted version of any of these groups or a protecting group, phosphates [R═—OP(O)(OH) 2 ], sulfonates [R═OS(O) 2 OH], sugar, or H. 
       
     
     
         2 . The compound of  claim 1 , further comprising a pharmaceutically effective carrier. 
     
     
         3 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         4 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         5 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         6 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         7 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         8 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         9 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         10 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         11 . The compound of  claim 1  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         12 . A composition comprising a compound of the formula: 
       
         
           
           
               
               
           
         
         wherein R 1  is an alkyl, alkyl alkanoate, alkenyl, alkynyl, acyl, alkanediyl, aryl, aralkyl, heteroaryl, heteroaralkyl, alkyl oximes (R═CH═NOH), allyl hydrazones (R═CH═NHNHR), alkyl amines, or a substituted version of any of these groups or a protecting group, phosphates [R═—OP(O)(OH) 2 ], sulfonates [R═OS(O) 2 OH], sugar, OH, or H; and R 2  is an alkyl, alkyl alkanoate, alkenyl, alkynyl, acyl, alkanediyl, aryl, aralkyl, heteroaryl, heteroaralkyl, alkyl oximes (R═CH═NOH), alkyl hydrazones (R═CH═NHNHR), alkyl amines or a substituted version of any of these groups or a protecting group, phosphates [R═—OP(O)(OH) 2 ], sulfonates [R═OS(O) 2 OH], sugar, or H. 
       
     
     
         13 . The compound of  claim 12 , further comprising a pharmaceutically effective carrier. 
     
     
         14 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         15 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         16 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         17 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         18 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         19 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         20 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         21 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         22 . The compound of  claim 12  having the formula: 
       
         
           
           
               
               
           
         
       
     
     
         23 . A method of producing a 2,3-hydroxy-glycoside derivative of acetaminophen, comprising:
 a) providing a glycoside derivative of acetaminophen wherein the glycoside has an olefin at the 2,3 position relative to the anomeric carbon bonded to the acetaminophen;   b) treating said glycoside derivative of acetaminophen under conditions so as to hydroxylate the olefin and produce a 2,3-hydroxy-glycoside derivative of acetaminophen.   
     
     
         24 . The method of  claim 23  wherein said hydroxylating conditions comprise using OsO 4 . 
     
     
         25 . The method of  claim 23 , wherein said glycoside derivative of acetaminophen of step a) contains protecting groups. 
     
     
         26 . The method of  claim 25 , wherein said protecting groups are removed before hydroxylation of the olefin. 
     
     
         27 . The method of  claim 25 , wherein said protecting groups are removed after hydroxylation of the olefin. 
     
     
         28 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         29 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         30 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         31 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         32 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         33 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         34 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         35 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         36 . The method of  claim 23 , wherein said 2,3-hydroxy-glycoside derivative of acetaminophen derivative has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         37 . A method of synthesizing a 2,3-dideoxy-glycoside derivative of acetaminophen wherein the glycoside has methylene groups at the 2 and 3 positions relative to the anomeric carbon bonded to the acetaminophen, comprising:
 a) providing a glycoside derivative of acetaminophen wherein the glycoside has an olefin at the 2,3 position relative to the anomeric carbon bonded to the acetaminophen;   b) treating said glycoside derivative of acetaminophen under such reducing conditions so as to reduce the olefin and produce a 2,3-dideoxy-glycoside derivative of acetaminophen.   
     
     
         38 . The method of  claim 37 , wherein said reducing conditions comprise using TsNHNH 2 . 
     
     
         39 . The method of  claim 38 , wherein said glycoside derivative of acetaminophen of step a) contains protecting groups. 
     
     
         40 . The method of  claim 39 , wherein said protecting groups are removed before reduction of the olefin. 
     
     
         41 . The method of  claim 39 , wherein said protecting groups are removed after reduction of the olefin. 
     
     
         42 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         43 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         44 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         45 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         46 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         47 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         48 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         49 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         50 . The method of  claim 37 , wherein said 2,3-dideoxy-glycoside derivative of acetaminophen has the formula: 
       
         
           
           
               
               
           
         
       
     
     
         51 . The method of treating a subject, comprising:
 a) providing a subject;   b) treating said subject with a 2,3-hydroxylated glycoside derivative of acetaminophen.   
     
     
         52 . The method of  claim 51 , wherein said treatment reduces one or more symptoms of a diseased state. 
     
     
         53 . The method of treating a subject, comprising:
 a) providing a subject;   b) treating said subject with a 2,3-dideoxy-glycoside derivative of acetaminophen.   
     
     
         54 . The method of  claim 53 , wherein said treatment reduces one or more symptoms of a diseased state. 
     
     
         55 . A method of synthesizing a glycosylated acetaminophen, comprising:
 a) providing a 4-nitrophenol, a per-acylated carbohydrate, an acid catalyst, and solvent;   b) glycosylating said 4-nitrophenol with said per-acylated carbohydrate with said acid catalyst in said solvent so as to produce a first product, said first product comprising a nitro group;   c) treating said first product so as to reduce said nitro group to an amide and to concomitantly acylate said amide, thereby creating a second product, said second product comprising a plurality of acetate groups;   d) treating said second product under conditions such that all of said acetate groups are hydrolyzed, thereby creating a third product, said third product comprising a plurality of hydroxyl groups, one of said hydroxyl groups at position C-6; and   e) treating said third product under conditions such that said hydroxyl at position C-6 is selectively acylated, thereby synthesizing a glycosylated acetaminophen.   
     
     
         56 . The method of  claim 55 , wherein said per-acylated carbohydrate is pentaacetyl mannose. 
     
     
         57 . The method of  claim 55 , wherein said per-acylated carbohydrate is pentaacetyl glucsose. 
     
     
         58 . The method of  claim 55 , wherein said per-acylated carbohydrate is pentaacetyl galactose. 
     
     
         59 . The method of  claim 55 , wherein said per-acylated carbohydrate is tetraacetyl rhamnose. 
     
     
         60 . The method of  claim 55 , wherein said per-acylated carbohydrate is octaacetyl maltose. 
     
     
         61 . The method of  claim 55 , wherein said per-acylated carbohydrate is octaacetyl lactose. 
     
     
         62 . The method of  claim 55 , wherein said acid catalyst is BF 3 OEt 2 . 
     
     
         63 . The method of  claim 55 , wherein said solvent is CH 2 Cl 2 . 
     
     
         64 . The method of  claim 56 , wherein the structure of said first product is: 
       
         
           
           
               
               
           
         
       
     
     
         65 . The method of  claim 64 , wherein the structure of said second product is: 
       
         
           
           
               
               
           
         
       
     
     
         66 . The method of  claim 65 , wherein the structure of said third product is: 
       
         
           
           
               
               
           
         
       
     
     
         67 . The method of  claim 66 , wherein the structure of said glycosylated acetaminophen is: 
       
         
           
           
               
               
           
         
       
     
     
         68 . A method of synthesizing an amino hydroxyl glycosylated acetaminophen analog, comprising:
 a) providing acetylated protecting group protected 2,3-olefin glycosylated acetaminophen analog, m-CPBA, and solvent;   b) epoxidizing said acetylated protecting group protected 2,3-olefin glycosylated acetaminophen analog with said m-CPBA in said solvent so as to produce a first product, said first product comprising an 2,3-epoxide group;   c) treating said first product so as to change said epoxide group to an azide and hydroxyl group, thereby creating a second product, said second product comprising an azide and hydroxyl group;   d) treating said second product under conditions such that all of said azide groups are hydrogenated and reduced, thereby creating a third product, said third product comprising an amine and hydroxyl groups; and   e) treating said third product under conditions such that said acetylated hydroxyl protecting groups are selectively removed, thereby synthesizing an amino hydroxyl glycosylated acetaminophen analog.   
     
     
         69 . The method of  claim 68 , wherein the structure of said first product is: 
       
         
           
           
               
               
           
         
       
     
     
         70 . The method of  claim 68 , wherein the structure of said second product is selected from the group: 
       
         
           
           
               
               
           
         
       
     
     
         71 . The method of  claim 68 , wherein the structure of said third product is selected from the group: 
       
         
           
           
               
               
           
         
       
     
     
         72 . The method of  claim 68 , wherein the structure of said amino hydroxyl glycosylated acetaminophen analog is selected from the group: 
       
         
           
           
               
               
           
         
       
     
     
         73 . A method of synthesizing 2,3-dideoxy-glycoside derivative of acetaminophen, comprising:
 a) providing protecting group protected 2,3-olefin glycosylated acetaminophen analog, H 2 , and a metal which catalyzes hydrogenation;   b) hydrogenating said protecting group protected 2,3-olefin glycosylated acetaminophen analog with said H 2  and metal so as to produce a first product, said first product comprising a protecting group protected 2,3-dideoxy-glycoside derivative of acetaminophen;   c) treating said first product so as to remove the protecting group of said first product, thereby creating a 2,3-dideoxy-glycoside derivative of acetaminophen.   
     
     
         74 . The method of  claim 73 , wherein the structure of said protecting group protected 2,3-olefin glycosylated acetaminophen analog is selected from the group: 
       
         
           
           
               
               
           
         
         wherein R is a protecting group, acetate, or H. 
       
     
     
         75 . The method of  claim 73 , wherein the structure of said first product is selected from the group: 
       
         
           
           
               
               
           
         
         wherein R is a protecting group, acetate, or H. 
       
     
     
         76 . The method of  claim 73 , wherein the structure of said 2,3-dideoxy-glycoside derivative of acetaminophen is selected from the group: 
       
         
           
           
               
               
           
         
       
     
     
         77 . The method of  claim 73 , wherein said metal which catalyzes hydrogenation is selected from the group: nickel, platinum, palladium, rhodium, and ruthenium based metals.

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