US2023220388A1PendingUtilityA1

Multimeric oligonucleotides with divided strands

62
Assignee: MPEG LA L L CPriority: Apr 30, 2020Filed: Apr 29, 2021Published: Jul 13, 2023
Est. expiryApr 30, 2040(~13.8 yrs left)· nominal 20-yr term from priority
C12N 15/113C12N 15/1137C12N 2310/14C12N 2310/51C12N 2310/3519C12N 2330/30C12N 15/111A61K 31/713C12N 2310/314C12N 2310/321
62
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Claims

Abstract

The present disclosure relates to multimeric oligonucleotides comprising subunits, each of the subunits independently comprises a single-stranded or double-stranded oligonucleotide. Each of the subunits is joined to another subunit by a covalent linker, and at least one subunit comprises at least one partial single-stranded oligonucleotide. The present disclosure also relates to methods of synthesizing the multimeric oligonucleotides and the methods of using the multimeric oligonucleotides disclosed herein.

Claims

exact text as granted — not AI-modified
What is claimed is: 
     
         1 . A multimeric oligonucleotide comprising subunits, wherein:
 each of the subunits independently comprises a single-stranded or double-stranded oligonucleotide; each of the subunits is joined to another subunit by a covalent linker; and   at least one subunit comprises at least one partial single-stranded oligonucleotide.   
     
     
         2 . The multimeric oligonucleotide of  claim 1 , wherein at least one subunit comprises two partial single-stranded oligonucleotides annealed to a complementary strand to form a double-stranded subunit. 
     
     
         3 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 1: 
       
         
           
           
               
               
           
         
       
       wherein:
   is a single-stranded oligonucleotide; 
    is a partial single-stranded oligonucleotide; and 
 ● is a covalent linker. 
 
     
     
         4 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 2: 
       
         
           
           
               
               
           
         
       
       wherein:
    is a single-stranded oligonucleotide; 
    is a partial single-stranded oligonucleotide; and 
 ● is a covalent linker. 
 
     
     
         5 . A multimeric oligonucleotide comprising Structure 3: 
       
         
           
           
               
               
           
         
       
       wherein: each
    is independently a partial single-stranded oligonucleotide; and 
 ● is a covalent linker. 
 
     
     
         6 . The multimeric oligonucleotide of  claim 5 , wherein Structure 3 is a homodimer. 
     
     
         7 . The multimeric oligonucleotide of  claim 5 , wherein Structure 3 is a heterodimer. 
     
     
         8 . The multimeric oligonucleotide of  claim 1 , wherein at least one subunit comprises Structure 4: 
       
         
           
           
               
               
           
         
       
       wherein:
 each   is a partial single-stranded oligonucleotide; 
 • is a covalent linker joined to a partial single-stranded oligonucleotide and an adjoining oligonucleotide subunit; and 
    is a complementary strand. 
 
     
     
         9 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 5: 
       
         
           
           
               
               
           
         
       
       wherein:
 each   is a single-stranded oligonucleotide; 
 each   is a partial single-stranded oligonucleotide; 
 each ● is a covalent linker joining a single-stranded oligonucleotide to a partial single-stranded oligonucleotide; and 
    is a complementary strand. 
 
     
     
         10 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 6: 
       
         
           
           
               
               
           
         
         wherein: 
         each   is a single-stranded oligonucleotide; 
         each   is a partial single-stranded oligonucleotide; 
         ● each is a covalent linker joining adjacent oligonucleotides; 
         each   is a complementary strand; and 
         each of a, h, c, d, e, f, g, h, i, j and k is independently an integer greater than or equal to zero, with the proviso that at least one of c, e, h, and j is greater than or equal to 1. 
       
     
     
         11 . The multimeric oligonucleotide of  claim 10 , wherein each of a, h, c, d, e, f, g, h, i, j and k is independently an integer in the range of 0 to 10, with the proviso that at least one of c, e, h and j is greater than or equal to 1. 
     
     
         12 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 7: 
       
         
           
           
               
               
           
         
       
       wherein:
    are each a single-stranded oligonucleotide; 
    are each a complementary strand; 
    are each a partial single-stranded oligonucleotide; 
 ● are each a covalent linker; 
 m and n are each independently an integer greater than or equal to 1; and 
 o is an integer greater than or equal to 0. 
 
     
     
         13 . The multimeric oligonucleotide of  claim 12 , wherein m and n are each independently an integer in the range of 1 to 10; and o is an integer in the range of 0 to 10. 
     
     
         14 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric, oligonucleotide comprises Structure 8 
       
         
           
           
               
               
           
         
         wherein: 
            are each a single-stranded oligonucleotide; 
            are each a complementary strand; 
            are each a partial single-stranded oligonucleotide; 
         ● are each covalent linkers; and 
         p and q are each independently an integer greater than or equal to zero. 
       
     
     
         15 . The multimeric oligonucleotide of  claim 14 , wherein p and q are each independently an integer in the range of 0 to 10; or wherein p and q are each independently an integer in the range of 0 to 3. 
     
     
         16 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 9: 
       
         
           
           
               
               
           
         
         wherein: 
            are each a single-stranded oligonucleotide; 
            are each a complementary strand; 
            are each a partial single-stranded oligonucleotide; 
         ● are each a covalent linker; 
         r is an integer greater than or equal to 1; and 
         s is an integer greater than or equal to 0. 
       
     
     
         17 . The multimeric oligonucleotide of  claim 16 , wherein r is an integer in the range of 1 to 10 and s is an integer in the range of 0 to 10; or wherein r is an integer in the range of 1 to 3 and s is 0 or 1. 
     
     
         18 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 10: 
       
         
           
           
               
               
           
         
       
       wherein:
    each is a single-stranded oligonucleotide; 
 each   is a partial single-stranded oligonucleotide; 
 each ● is a covalent linker joining adjacent oligonucleotides; and 
 each   is a complementary strand. 
 
     
     
         19 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 11: 
       
         
           
           
               
               
           
         
         wherein: 
         each   is a single-stranded oligonucleotide; 
         each   is a partial single-stranded oligonucleotide; 
         each ● is a covalent linker joining adjacent oligonucleotides; 
         each   is a complementary strand. 
       
     
     
         20 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 12: 
       
         
           
           
               
               
           
         
       
       wherein:
 each   is a single-stranded oligonucleotide; 
 each   is a partial single-stranded oligonucleotide; 
 each ● is a covalent linker joining adjacent oligonucleotides; and 
 each   is a complementary strand. 
 
     
     
         21 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 13: 
       
         
           
           
               
               
           
         
       
       wherein:
 each   is a single-stranded oligonucleotide; 
 each   is a partial single-stranded oligonucleotide; 
 each ● is a covalent linker joining adjacent oligonucleotides; and 
 each   is a complementary strand. 
 
     
     
         22 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 14: 
       
         
           
           
               
               
           
         
         wherein: 
         each   is a single-stranded oligonucleotide; 
         each   is a partial single-stranded oligonucleotide; 
         each ● is a covalent linker joining adjacent oligonucleotides; and 
         each   is a complementary strand. 
       
     
     
         23 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 15: 
       
         
           
           
               
               
           
         
         wherein: 
         each   is a single-stranded oligonucleotide; 
         each   is a partial single-stranded oligonucleotide; 
         each ● is a covalent linker joining adjacent oligonucleotides; and 
         each   is a complementary strand. 
       
     
     
         24 . The multimeric oligonucleotide of  claim 1 , wherein the multimeric oligonucleotide comprises Structure 16: 
       
         
           
           
               
               
           
         
         wherein each 
            is a single-stranded oligonucleotide; 
            is a complementary strand; 
            is a partial single-stranded oligonucleotide; 
         ● is a covalent linker; and 
         t and u are each independently an integer greater than or equal to 0 with the proviso that at least one of t and u are an integer greater than or equal to 1. 
       
     
     
         25 . The multimeric oligonucleotide of  claim 24 , wherein t and u are each independently an integer in the range of 0 to 10 with the proviso that at least one of t and u are an integer greater than or equal to 1; or wherein t and u are each independently an integer in the range of 0 to 3 with the proviso that at least one oft and u are an integer greater than or equal to 1. 
     
     
         26 . The multimeric oligonucleotide of any of  claims 1 - 25 , wherein each partial single-stranded oligonucleotide is 5-14 nucleotides in length. 
     
     
         27 . The multimeric oligonucleotide of any of  claims 1 - 26 , wherein at least two subunits are active against different cellular targets. 
     
     
         28 . The multimeric oligonucleotide of  claim 27 , wherein all of the subunits are active against different cellular targets. 
     
     
         29 . The multimeric oligonucleotide of any of  claims 1 - 26 , wherein at least two subunits are active against the same cellular target. 
     
     
         30 . The multimeric oligonucleotide of  claim 29 , wherein all of the subunits are active against different cellular targets. 
     
     
         31 . The multimeric oligonucleotide of any of  claims 1 - 30 , wherein the multimeric oligonucleotide comprises four or more subunits. 
     
     
         32 . The multimeric oligonucleotide of  claim 31 , wherein the multimeric oligonucleotide comprises four, five, six, seven, eight, nine, or ten subunits. 
     
     
         33 . The multimeric oligonucleotide of any of  claims 1 - 32 , wherein each nucleic acid in the multimeric oligonucleotide is RNA, DNA, or an artificial or non-natural nucleic acid analog. 
     
     
         34 . The multimeric oligonucleotide of any of  claims 1 - 33 , wherein at least one subunit is siRNA, saRNA, or miRNA. 
     
     
         35 . The multimeric oligonucleotide of  claim 34 , wherein all of the subunits are siRNA. 
     
     
         36 . The multimeric oligonucleotide of  claim 34 , wherein all of the subunits are saRNA. 
     
     
         37 . The multimeric oligonucleotide of  claim 34 , wherein all of the subunits are miRNA. 
     
     
         38 . The multimeric oligonucleotide of any of  claims 1 - 33 , wherein at least one subunit is a single-stranded subunit. 
     
     
         39 . The multimeric oligonucleotide of  claim 38 , wherein the at least one single-stranded subunit is an antisense oligonucleotide. 
     
     
         40 . The multimeric oligonucleotide of any one of  claims 1 - 39 , wherein at least one covalent linker ● is a cleavable covalent linker. 
     
     
         41 . The multimeric oligonucleotide of  claim 40 , wherein the cleavable covalent linker comprises an acid cleavable bond, a reductant cleavable bond, a bio-cleavable bond, or an enzyme cleavable bond. 
     
     
         42 . The multimeric oligonucleotide of  claim 40  or  41 , wherein the cleavable covalent linker is cleavable under intracellular conditions. 
     
     
         43 . The multimeric oligonucleotide of any of  claims 1 - 42 , wherein each covalent linker is, independently, a disulfide bond or a compound of Structure 25: 
       
         
           
           
               
               
           
         
       
       wherein:
 S is attached by a covalent bond or by a linker to an oligonucleotide subunit; 
 each R 1  is independently a C 2 -C 10  alkyl, C 2 -C 10  alkoxy, or C 1 -C 10  aryl group; 
 R 2  is a thiopropionate or disulfide group; and 
 each X is independently selected from: 
 
       
         
           
           
               
               
           
         
       
     
     
         44 . The multimeric oligonucleotide of  claim 43 , wherein the compound of Structure 25 is 
       
         
           
           
               
               
           
         
         wherein each terminal S is attached by a covalent bond or by a linker to an oligonucleotide subunit. 
       
     
     
         45 . The multimeric oligonucleotide of  claim 43 , wherein the compound of Structure 25 is a compound according to Structure 26: 
       
         
           
           
               
               
           
         
         wherein each terminal S is attached by a covalent bond or by a linker to an oligonucleotide subunit. 
       
     
     
         46 . The multimeric oligonucleotide of  claim 43 , wherein the compound of Structure 25 is a compound according to Structure 27: 
       
         
           
           
               
               
           
         
         wherein each terminal S is attached by a covalent bond or by a linker to an oligonucleotide subunit. 
       
     
     
         47 . The multimeric oligonucleotide of  claim 43 , wherein the compound of Structure 25 is a compound according to Structure 28: 
       
         
           
           
               
               
           
         
         wherein each terminal S is attached by a covalent bond or by a linker to an oligonucleotide subunit. 
       
     
     
         48 . The multimeric oligonucleotide any of  claims 43 - 47 , wherein the covalent linker of Structure 25 is formed from a covalent linker precursor according to Structure 29: 
       
         
           
           
               
               
           
         
         wherein each R is independently a C 2 -C 10  alkyl, C 2 -C 10  alkoxy, or C 1 -C 10  aryl group; and 
         R 2  is a thiopropionate or disulfide group. 
       
     
     
         49 . The multimeric oligonucleotide of any of  claims 1 - 48 , wherein at least one covalent linker is attached to the 3′ or 5′ terminus of an oligonucleotide subunit. 
     
     
         50 . The multimeric oligonucleotide of  claim 49 , wherein all covalent linkers are attached to the 3′ or 5′ terminus of an oligonucleotide subunit. 
     
     
         51 . The multimeric oligonucleotide of any of  claims 1 - 49 , wherein at least one covalent linker is attached to an internal nucleotide of an oligonucleotide subunit. 
     
     
         52 . The multimeric oligonucleotide of any of  claims 1 - 51 , wherein at least one covalent linker e comprises a nucleotide linker. 
     
     
         53 . The multimeric oligonucleotide of  claim 52 , wherein the nucleotide linker is between 2-6 nucleotides in length. 
     
     
         54 . The multimeric oligonucleotide of any of  claims 1 - 53 , wherein each covalent linker is the same. 
     
     
         55 . The multimeric oligonucleotide of any of  claims 1 - 53  wherein at least one covalent linker ● is different from the other covalent linkers. 
     
     
         56 . The multimeric oligonucleotide of any of  claims 1 - 55 , at least two subunits are joined by a covalent linker ● between the 3′ end of a first subunit and the 3′ of a second subunit. 
     
     
         57 . The multimeric oligonucleotide of any of  claims 1 - 56 , wherein at least two subunits are joined by a covalent linker ● between the 5′ end of a first subunit and the 3′ of a second subunit. 
     
     
         58 . The multimeric oligonucleotide as in any of  claims 1 - 57 , wherein at least two subunits are joined by a covalent linker ● between the 5′ end of a first subunit and the 5′ of a second subunit. 
     
     
         59 . The multimeric oligonucleotide of any of  claims 1 - 58 , further comprising a chemical or biological moiety that is not an oligonucleotide. 
     
     
         60 . The multimeric oligonucleotide as in any of  claims 1 - 59 , wherein the multimeric oligonucleotide is at least 75, 80, 85, 90, 95, 96, 97, 98, 99, or 100% pure. 
     
     
         61 . A method of synthesizing a multimeric oligonucleotide comprising Structure 16: 
       
         
           
           
               
               
           
         
         wherein each   is an single-stranded oligonucleotide, each   is a partial single-stranded oligonucleotide, each   is a complementary strand; each ● is a covalent linker joining adjacent oligonucleotides, and t and u are each independently an integer greater than or equal to 1; 
         the method comprising annealing Structure 17 
       
       
         
           
           
               
               
           
         
         and Structure 18 
       
       
         
           
           
               
               
           
         
         with complementary strands  , thereby forming Structure 16. 
       
     
     
         62 . A method of synthesizing a multimeric oligonucleotide comprising Structure 8: 
       
         
           
           
               
               
           
         
         wherein each   is a single-stranded oligonucleotide, each   is a partial single-stranded oligonucleotide, each   is a complementary strand; each ● is a covalent linker joining adjacent oligonucleotides, and p and q are each independently an integer greater than or equal to 1; 
         the method comprising annealing Structure 19, 
       
       
         
           
           
               
               
           
         
         Structure 20, 
       
       
         
           
           
               
               
           
         
         and one or more of Structure 21, 
       
       
         
           
           
               
               
           
         
         with complementary strands  , thereby forming Structure 8. 
       
     
     
         63 . A method of synthesizing a multimeric oligonucleotide comprising Structure 9A: 
       
         
           
           
               
               
           
         
         wherein each   is a single-stranded oligonucleotide, each   is a partial single-stranded oligonucleotide, each   is a complementary strand; each ● is a covalent linker joining adjacent oligonucleotides; and r and s are each independently an integer greater than or equal to the method comprising annealing Structure 22 
       
       
         
           
           
               
               
           
         
         and Structure 23 
       
       
         
           
           
               
               
           
         
         and one or more of Structure 24 
       
       
         
           
           
               
               
           
         
         with complementary strands  , thereby forming Structure 9A. 
       
     
     
         64 . A method of synthesizing a multimeric oligonucleotide comprising Structure 9B: 
       
         
           
           
               
               
           
         
         wherein each   is a single-stranded oligonucleotide; each   is a partial single-stranded oligonucleotide; each   is a complementary strand; each • is a covalent linker joining adjacent oligonucleotides; and r is an integer greater than or equal to 1; 
         the method comprising annealing Structure 22, 
       
       
         
           
           
               
               
           
         
         and one or more of Structure 24 
       
       
         
           
           
               
               
           
         
         and a partial single-stranded oligonucleotide   with complementary strands  , thereby forming Structure 9B. 
       
     
     
         65 . A composition comprising the multimeric oligonucleotide of any of  claims 1 - 60  and a pharmaceutically acceptable excipient. 
     
     
         66 . A composition comprising the multimeric oligonucleotide of any of  claims 1 - 60  for use in the manufacture of a medicament. 
     
     
         67 . A method for treating a subject comprising administering to the subject an effective amount of the multimeric oligonucleotide of any of  claims 1 - 60 .

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