Cleavable Binary Dyads: Simplifying Data Extraction and Increasing Storage Density in Digital Polymers.
Fiche publication
Date publication
avril 2018
Journal
Angewandte Chemie (International ed. in English)
Auteurs
Membres identifiés du Cancéropôle Est :
Dr CARAPITO Christine
Tous les auteurs :
Cavallo G, Poyer S, Amalian JA, Dufour F, Burel A, Carapito C, Charles L, Lutz JF
Lien Pubmed
Résumé
Digital polymers are uniform macromolecules that store monomer-based binary sequences. Molecularly stored information is usually extracted from the polymer by a tandem mass spectrometry (MS/MS) measurement, in which the coded chains are fragmented to reveal each bit (i.e. basic coded monomer unit) of the sequence. Here, we show that data-extraction can be greatly simplified by favoring the formation of MS/MS fragments containing two bits instead of one. In order to do so, digital poly(alkoxyamine phosphodiester)s, containing binary dyads in each repeat unit, were prepared by an orthogonal solid-phase approach involving successive phosphoramidite and radical-radical coupling steps. Three different sets of monomers were considered to build these polymers. In all cases, four coded building blocks-two hydroxy-nitroxides and two phosphoramidite monomers-were required to build the dyads. Among the three studied monomer sets, one combination allowed synthesis of uniform sequence-coded polymers. The resulting polymers led to clear dyad-containing fragments in MS/MS and could therefore be efficiently decoded. Additionally, an algorithm was created to detect specific dyad fragments, thus enabling automated sequencing.
Mots clés
digital polymers, mass spectrometry, sequence-controlled polymers, sequencing, solid-phase chemistry
Référence
Angew. Chem. Int. Ed. Engl.. 2018 Apr 6;: