Precise alkoxyamine-design enables automated tandem mass spectrometry sequencing of digital poly(phosphodiester)s.
Fiche publication
Date publication
septembre 2020
Journal
Angewandte Chemie (International ed. in English)
Auteurs
Membres identifiés du Cancéropôle Est :
Dr CARAPITO Christine
Tous les auteurs :
Launay K, Amalian JA, Laurent E, Oswald L, Al Ouahabi A, Burel A, Dufour F, Carapito C, Clément JL, Lutz JF, Charles L, Gigmes D
Lien Pubmed
Résumé
Increasing data storage density is one of the major challenges of the information industry. To be widely applicable, writing and reading information have to be dense, convenient and fast. A major step towards reliable reading of information coded in the sequence of long poly(phosphodiester)s was previously achieved by introducing an alkoxyamine spacer between information sub-segments. However, MS/MS decoding had to be performed manually to safely identify useful fragments of low abundance compared to side-products induced by the amide-based alkoxyamine used. Here, alternative alkoxyamines were designed to prevent these side-reactions and enable automated MS/MS sequencing. Different styryl-TEMPO spacers were prepared to increase radical delocalization and stiffness of the structure. Their dissociation behavior was investigated by EPR and best MS/MS data were recorded for polymers with alkoxyamines containing in-chain benzyl ring, avoiding all side-reactions during synthesis or sequencing. As a result, automated decoding of these polymers can be achieved using the MS-DECODER software, which performs interpretation of fragmentation data recorded for each sub-segment prior to align the so-obtained digital sequences in their original order based on the mass tag defining the initial location of each sub-segment.
Mots clés
alkoxyamine synthesis, digital information, mass spectrometry, radical ions, sequence-defined synthetic polymers
Référence
Angew. Chem. Int. Ed. Engl.. 2020 Sep 22;: