Journal
MACROMOLECULES
Volume 48, Issue 13, Pages 4319-4328Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.macromol.5b01051
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Funding
- European Funding [FEDER OBJ2142-3341]
- European Research Council [258593]
- Cluster of Excellence Chemistry of Complex Systems (LabEx CSC)
- CNRS
- ERC
- LabEX CSC
- European Research Council (ERC) [258593] Funding Source: European Research Council (ERC)
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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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