US2014135455A1PendingUtilityA1

Transketalized compositions, synthesis, and applications

63
Assignee: SEGETIS INCPriority: Apr 16, 2008Filed: Jan 20, 2014Published: May 15, 2014
Est. expiryApr 16, 2028(~1.8 yrs left)· nominal 20-yr term from priority
C07D 407/12C07D 493/04C07D 407/14C07D 493/22C07D 317/22C07D 317/12C07D 407/04C08G 63/668C07D 493/16C08L 77/06C08G 69/48C08G 69/28C07D 493/18C07D 493/10C08L 77/12C07D 493/14C07D 317/30C08G 69/26C08G 69/44
63
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Claims

Abstract

The present disclosure relates to the preparation of ketal compounds from polyols and oxocarboxylates, and uses thereof.

Claims

exact text as granted — not AI-modified
1 - 62 . (canceled) 
     
     
         63 . A compound comprising structure II 
       
         
           
           
               
               
           
         
       
       wherein
 R 1  is hydrogen, a metal cation, an organic cation, a linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, alkaryl, or an oligomeric or polymeric moiety; 
 R 2  is a covalent bond or a linear or branched alkyl group; 
 R 3  is hydrogen, a linear, branched, or cyclic alkyl group; 
 R 4  and R 5  are independently linear, branched, or cyclic alkyl groups; and 
 Z is O or NR, wherein R is hydrogen or a linear or branched alkyl group having between 1 and 6 carbon atoms. 
 
     
     
         64 . The compound of  claim 63  wherein R 2  is —CH 2 CH 2 —, R 3  is CH 3 —, Z is O, and R 1  is a cation or a linear or branched alkyl group having between 1 and 8 carbon atoms. 
     
     
         65 . A compound comprising structure IIIa or IIIb 
       
         
           
           
               
               
           
         
       
       wherein
 R 3  and R 5  are independently isobutyl or 
 
       
         
           
           
               
               
           
         
         
           wherein
 R 1  is hydrogen, a metal cation, an organic cation, a linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, alkaryl, or an oligomeric or polymeric moiety; 
 
         
         R 2  is a covalent bond or a linear or branched alkyl group; and 
         Z is O or NR where R is hydrogen or a linear or branched alkyl group having between 1 and 6 carbon atoms; and 
         R 4  and R 6  are independently hydrogen or linear, branched, or cyclic alkyl groups. 
       
     
     
         66 . The compound of  claim 65  wherein both R 3  and R 5  are 
       
         
           
           
               
               
           
         
       
       R 2  is —CH 2 —CH 2 —, and R 4  and R 6  are methyl. 
     
     
         67 . A compound comprising structure Ic 
       
         
           
           
               
               
           
         
         R 1  is a divalent linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, or alkaryl moiety; 
         R 2  is a covalent bond, a linear, branched, or cyclic alkyl group, or a linear, cyclic, or branched alkenyl group; 
         R 3 , R 5  and R 6  are independently hydrogen or linear, branched, or cyclic alkyl groups, or linear, cyclic, or branched alkenyl groups; and 
         R 4  is a covalent bond or a linear, branched, or cyclic alkyl group, or linear, cyclic, or branched alkenyl group, or a linear or branched alkynyl, aryl, aralkyl, or aralkenyl group; and 
         Z and Z′ are independently O or NR, wherein R is hydrogen or an alkyl group having between 1 and 6 carbon atoms. 
       
     
     
         68 . The compound of  claim 67  wherein
 R′ is selected from —(CH 2 ) 2 —, —(CH 2 ) 3 —, —(CH 2 ) 4 —, —(CH 2 ) 5 —, —(CH 2 ) 6 —, —(CH 2 ) 2 —O—(CH 2 ) 2 —, or 
 
       
         
           
           
               
               
           
         
         R 4  is selected from a covalent bond or 
       
       
         
           
           
               
               
           
         
       
       wherein R 7  and R 8  are independently linear alkyl groups, branched alkyl groups, cyclic alkyl groups, linear alkenyl groups, branched alkenyl groups, cyclic alkenyl groups, alkynyl groups, aryl groups, aralkyl groups, or aralkenyl groups; or R 7  and R 8  are connected to each other as part of an alkyl or alkenyl ring having 5 to 12 members,
 one of R 5  or R 6  is 
 
       
         
           
           
               
               
           
         
       
       wherein R 7  and R 8  are independently linear alkyl groups, branched alkyl groups, cyclic alkyl groups, linear alkenyl groups, branched alkenyl groups, or cyclic alkenyl groups, alkynyl groups, aryl groups, aralkyl groups, or aralkenyl groups; or R 7  and R 8  are connected to each other as part of an alkyl or alkenyl ring having 5 to 12 members, and
 R 2  is —CH 2 CH 2 — and R 3  is —CH 3 . 
 
     
     
         69 . A compound comprising at least one repeat unit corresponding to structure IV: 
       
         
           
           
               
               
           
         
       
       wherein
 R 1  is a divalent linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, or alkaryl moiety, wherein R 1  is the same or different for each occurrence; 
 R 2  is a covalent bond or a linear or branched alkyl group wherein R 2  is the same or different for each occurrence; 
 R 3  is hydrogen, a linear, branched, or cyclic alkyl wherein R 3  is the same or different for each occurrence; 
 R 4  is a covalent bond, methylene, or alkylmethylene, wherein a covalent bond indicates a 5-membered ring and a methylene or alkylmethylene indicates a 6-membered ring, wherein R 4  is the same or different for each occurrence; 
 R 5  is a covalent bond, methylene, ethylene, hydroxymethylene, —CH 2 —O—CH 2 —, or a polymeric moiety wherein R 5  is the same or different for each occurrence; 
 R 6  and R 7  are independently linear, branched, or cyclic alkyl groups; 
 R 8  and R 9  are independently hydrogen, a linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, alkaryl, or a polymeric moiety; 
 Z and Z′ are independently O or NR where R is hydrogen or an alkyl group having between 1 and 6 carbon atoms; 
 α is an integer of at least 1 and defines a ketal unit, wherein a ketal units are disposed contiguously to R 5 , R 8 , R 9 , or a combination thereof; and 
 δ is an integer of at least 1. 
 
     
     
         70 . The compound of  claim 69  wherein α is 1, all R 2  are —CH 2 CH 2 —, all R 3  are CH 3 —, R 8  and R 9  are hydrogen, and all R 4  and R 5  are covalent bonds. 
     
     
         71 . The compound of  claim 69  wherein one or more Z or Z′ are NH and the compound is a polyamide, a copolyamide, or a poly(ester amide). 
     
     
         72 . The compound of  claim 69  wherein all Z and Z′ are O and the compound further comprises ester, isocyanate, urethane, carbonate, polymerized allyl, polymerized epoxy, polymerized acrylate, or polymerized methacrylate groups or a combination of one or more thereof. 
     
     
         73 . The compound of  claim 69  wherein R 6  and R 7  are chosen from the group consisting of methyl, ethyl, and isobutyl. 
     
     
         74 . A compound comprising at least one repeat unit corresponding to structure Va, Vb, or a combination thereof 
       
         
           
           
               
               
           
         
       
       wherein
 R 1  is a divalent linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, or alkaryl moiety, wherein R 1  is the same or different for each occurrence; 
 R 2  is a covalent bond or a linear or branched alkyl group wherein R 2  is the same or different for each occurrence; 
 R 3  is hydrogen, a linear, branched, or cyclic alkyl wherein R 3  is the same or different for each occurrence; 
 Z and Z′ are independently O or NR where R is hydrogen or an alkyl group having between 1 and 6 carbon atoms; and 
 δ is between about 1 and 500. 
 
     
     
         75 . The compound of  claim 74  wherein one or more Z or Z′ are NH and the compound is a polyamide, a copolyamide, or a poly(ester amide). 
     
     
         76 . The compound of  claim 74  wherein all Z and Z′ are O and the compound further comprises ester, isocyanate, urethane, carbonate, allylic, epoxy, acrylate, or methacrylate groups or a combination of one or more thereof. 
     
     
         77 . A method of making a compound having structure I, comprising
 a. contacting a compound comprising structure VI   
       
         
           
           
               
               
           
         
         wherein
 R 4  is a covalent bond, methylene, or alkylmethylene, wherein a covalent bond indicates a 5-membered ring and a methylene or alkylmethylene indicates a 6-membered ring, wherein R 4  is the same or different for each occurrence; 
 R 5  is a covalent bond, methylene, ethylene, hydroxymethylene, —CH 2 —O—CH 2 —, or a polymeric moiety, and R 5  is the same or different for each occurrence; 
 R 8  and R 9  are independently hydrogen, a linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, alkaryl, or a polymeric moiety; and α and β are integers of at least 1 such that the sum α+β is at least 2, 
 
         with at least (α+β) moles of one or more compounds comprising structure VII 
       
       
         
           
           
               
               
           
         
         wherein
 R 1  is hydrogen, a metal cation, an organic cation, a linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, alkaryl, or an oligomeric or polymeric moiety; 
 R 2  is a covalent bond or a linear or branched alkyl group; 
 R 3  is a linear, branched, or cyclic alkyl group; 
 Z is O or NR, wherein R is hydrogen or a linear or branched alkyl group having between 1 and 6 carbon atoms; 
 
         b. reacting the compound VI and the compound VII to form a first ketal in the presence of a catalyst; 
         c. contacting the first ketal with at least a equivalents of a dialkyl ketone of the formula O═CR 6 R 7  wherein R 6  and R 7  are independently linear, branched, or cyclic alkyl groups; and 
         d. reacting the first ketal with the dialkyl ketone to form a second ketal having structure I 
       
       
         
           
           
               
               
           
         
       
       wherein
 Z, R, R 1 , R 2 , R 3 , R 4 , R 5 , R 6 , R 7 , R 8 , and R 9  are as defined in structures VI and VII; 
 γ is an integer of at least 1; and 
 α and β are independently 0 or 1 for each γ such that at least one α is 1 and at least one β is 1, and α and β are the same or different for each γ. 
 
     
     
         78 . The method of  claim 77  wherein the catalyst is a strong protic acid catalyst and further comprising neutralizing the catalyst after affecting the first reaction, the second reaction, or both. 
     
     
         79 . The method of  claim 77  further comprising removing the compound of structure VII during or after forming the second ketal. 
     
     
         80 . A method of making a compound having structure I wherein R 8  and R 9  are hydrogen, all Z are O, and all R 4  and R 5  are covalent bonds, the method comprising
 a. reacting sorbitol or mannitol with at least 3 molar equivalents of a dialkyl ketone of the formula O═CR 6 R 7  wherein R 6  and R 7  are independently linear, branched, or cyclic alkyl groups having between 3 and 6 carbon atoms to form a first ketal in the presence of a catalyst; and   b. reacting the first ketal with at least one molar equivalent of one or more compounds comprising structure VII   
       
         
           
           
               
               
           
         
         wherein
 R 1  is hydrogen, a metal cation, an organic cation, a linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, alkaryl, or an oligomeric or polymeric moiety; 
 R 2  is a covalent bond or a linear or branched alkyl group; 
 R 3  is a linear, branched, or cyclic alkyl group; and 
 Z is O 
 
       
       to form a second ketal having a structure comprising compound I 
       
         
           
           
               
               
           
         
       
       wherein
 R, R 1 , R 2 , R 3 , R 6 , and R 7  are as defined in structure VII; 
 R 8  and R 9  are hydrogen, 
 all Z are O, 
 all R 4  and R 5  are covalent bonds, 
 γ is an integer of at least 1, and 
 α and β are independently 0 or 1 for each γ such that at least one α is 1 and at least one β is 1, and α and β are the same or different for each γ. 
 
     
     
         81 . The method of  claim 80  wherein the catalyst is a strong protic acid catalyst and further comprising neutralizing the catalyst. 
     
     
         82 . The method of  claim 80  further comprising removing dialkyl ketone after forming the second ketal. 
     
     
         83 . The method of  claim 80  wherein greater than about 80 mole percent of compound I comprises 
       
         
           
           
               
               
           
         
       
     
     
         84 . A method of making a compound comprising at least one repeat unit of structure (IV) wherein Z and Z′ are NR where R is hydrogen or an alkyl group having between 1 and 6 carbon atoms, the method comprising:
 a) contacting a bisketal carboxylate of formula (I) 
 
       
         
           
           
               
               
           
         
       
       wherein
 R 1  is R 1  is hydrogen, a linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, alkaryl, or an oligomeric or polymeric moiety, wherein R 1  is the same or different for each occurrence; 
 R 2  is a covalent bond or a linear or branched alkyl group wherein R 2  is the same or different for each occurrence; 
 R 3  is the same or different for each occurrence and is a linear, branched, or cyclic alkyl group, or at least one R 3  is 
 
       
         
           
           
               
               
           
         
         
           wherein
 n is 0, 1, or 2, 
 R′ is a linear or branched alkyl having between 1 and 6 carbon atoms, and 
 X is O or NR, wherein R is hydrogen or a linear or branched alkyl group having six or less carbon atoms; 
 
         
         R 4  is a covalent bond, methylene, or alkylmethylene, wherein a covalent bond indicates a 5-membered ring and a methylene or alkylmethylene indicates a 6-membered ring, wherein R 4  is the same or different for each occurrence; 
         R 5  is a covalent bond, methylene, ethylene, hydroxymethylene, —CH 2 —O—CH 2 —, or a polymeric moiety, wherein R 5  is the same or different for each occurrence; 
         R 6  and R 7  are independently linear, branched, or cyclic alkyl groups; 
         R 8  and R 9  are independently hydrogen, a linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, alkaryl, or a polymeric moiety; 
         Z is O; 
         γ is an integer of at least 1; and 
         α is 0 or 1 and β is at least two for each γ, and α and β are the same or different for each γ 
       
       and a diamine of formula RHN—R 1 —NRH
 wherein
 R is hydrogen or an alkyl group having between 1 and 6 carbon atoms and 
 R 1  is a divalent linear, branched, or cyclic alkyl, a linear, branched, or cyclic alkenyl, alkynyl, aryl, or alkaryl moiety; and 
 
 b. heating the contacted bisketal carboxylate of formula (I) and the diamine at a pressure and for a time effective to form the polymer of formula IV: 
 
       
         
           
           
               
               
           
         
       
       wherein
 R 1 , R 2 , R 3 , R 4 , R 5 , R 6 , R 7 , R 8 , R 9 , Z, Z′, and α are as defined above; and δ is an integer of at least 1.

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