MS/MS Sequencing of Digitally Encoded Poly(alkoxyamine amide)s
Monodisperse sequence-coded oligo(alkoxyamine amide)s were thoroughly investigated by tandem mass spectrometry to evaluate the robustness of this analytical approach as a reliable sequencing methodology. Studied samples were synthesized by orthogonal iterative chemistry on a solid support, and the...
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| Published in: | Macromolecules Vol. 48; no. 13; pp. 4319 - 4328 |
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American Chemical Society
14-07-2015
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| Abstract | Monodisperse sequence-coded oligo(alkoxyamine amide)s were thoroughly investigated by tandem mass spectrometry to evaluate the robustness of this analytical approach as a reliable sequencing methodology. Studied samples were synthesized by orthogonal iterative chemistry on a solid support, and the 0/1 coding system was based on the mass of two amide synthons that alternate with a nitroxide moiety. The major fragmentation pathway experienced by these co-oligomers proceeded via homolysis of all fragile C–ON bonds between a coding unit and a nitroxide moiety. The relative rate of competing C–ON bond cleavages was observed to be sequence-dependent, offering an additional means to validate the sequences reconstructed from the MS/MS fragments. The same fragmentation rules applied for all studied samples, varying in terms of chain length, charge state, encoded sequence, end-groups, and nitroxide moiety. Ion mobility separation was coupled to MS/MS to sequence some more complex co-oligomers composed of both different nitroxides and coding units. |
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| AbstractList | Monodisperse sequence-coded oligo(alkoxyamine amide)s were thoroughly investigated by tandem mass spectrometry to evaluate the robustness of this analytical approach as a reliable sequencing methodology. Studied samples were synthesized by orthogonal iterative chemistry on a solid support, and the 0/1 coding system was based on the mass of two amide synthons that alternate with a nitroxide moiety. The major fragmentation pathway experienced by these co-oligomers proceeded via homolysis of all fragile C–ON bonds between a coding unit and a nitroxide moiety. The relative rate of competing C–ON bond cleavages was observed to be sequence-dependent, offering an additional means to validate the sequences reconstructed from the MS/MS fragments. The same fragmentation rules applied for all studied samples, varying in terms of chain length, charge state, encoded sequence, end-groups, and nitroxide moiety. Ion mobility separation was coupled to MS/MS to sequence some more complex co-oligomers composed of both different nitroxides and coding units. Monodisperse sequence-coded oligo(alkoxyamine amide)s were thoroughly investigated by tandem mass spectrometry to evaluate the robustness of this analytical approach as a reliable sequencing methodology. Studied samples were synthesized by orthogonal iterative chemistry on a solid support, and the 0/1 coding system was based on the mass of two amide synthons that alternate with a nitroxide moiety. The major fragmentation pathway experienced by these co-oligomers proceeded via homolysis of all fragile C-ON bonds between a coding unit and a nitroxide moiety. The relative rate of competing C-ON bond cleavages was observed to be sequence-dependent, offering an additional means to validate the sequences reconstructed from the MS/MS fragments. The same fragmentation rules applied for all studied samples, varying in terms of chain length, charge state, encoded sequence, end-groups, and nitroxide moiety. Ion mobility separation was coupled to MS/MS to sequence some more complex co-oligomers composed of both different nitroxides and coding units. |
| Author | Laure, Chloé Charles, Laurence Roy, Raj Kumar Lutz, Jean-François |
| AuthorAffiliation | Aix-Marseille Université − CNRS, UMR 7273 Institute of Radical Chemistry Precision Macromolecular Chemistry, UPR22-CNRS, BP84047 Institut Charles Sadron |
| AuthorAffiliation_xml | – name: Precision Macromolecular Chemistry, UPR22-CNRS, BP84047 – name: Institute of Radical Chemistry – name: Institut Charles Sadron – name: Aix-Marseille Université − CNRS, UMR 7273 |
| Author_xml | – sequence: 1 givenname: Laurence surname: Charles fullname: Charles, Laurence email: laurence.charles@univ-amu.fr – sequence: 2 givenname: Chloé surname: Laure fullname: Laure, Chloé – sequence: 3 givenname: Jean-François surname: Lutz fullname: Lutz, Jean-François email: jflutz@unistra.fr – sequence: 4 givenname: Raj Kumar surname: Roy fullname: Roy, Raj Kumar |
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| Title | MS/MS Sequencing of Digitally Encoded Poly(alkoxyamine amide)s |
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