Imaging Single-Chain Nanoparticle Folding via High-Resolution Mass Spectrometry

Jan Steinkoenig; Hannah Rothfuss; Andrea Lauer; Bryan T Tuten; Christopher Barner-Kowollik

doi:10.1021/jacs.6b10952

Imaging Single-Chain Nanoparticle Folding via High-Resolution Mass Spectrometry

J Am Chem Soc. 2017 Jan 11;139(1):51-54. doi: 10.1021/jacs.6b10952. Epub 2016 Dec 27.

Authors

Jan Steinkoenig^{1

2}, Hannah Rothfuss^{1

2}, Andrea Lauer^{1

2}, Bryan T Tuten^{1

2}, Christopher Barner-Kowollik^{1

2

3}

Affiliations

¹ Preparative Macromolecular Chemistry, Institut für Technische Chemie und Polymerchemie, Karlsruhe Institute of Technology (KIT) , Engesserstraße 18, 76128 Karlsruhe, Germany.
² Institut für Biologische Grenzflächen, Karlsruhe Institute of Technology (KIT) , Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany.
³ School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology (QUT) , 2 George Street, Brisbane, QLD 4000, Australia.

PMID: 27973776
DOI: 10.1021/jacs.6b10952

Abstract

Herein, we introduce the first approach to map single-chain nanoparticle (SCNP) folding via high-resolution electrospray ionization mass spectrometry (ESI MS) coupled with size exclusion chromatography. For the first time, the successful collapse of polymeric chains into SCNPs is imaged by characteristic mass changes, providing detailed mechanistic information regarding the folding mechanism. As SCNP system we employed methyl methacrylate (MMA) statistically copolymerized with glycidyl methacrylate (GMA), resulting in p(MMA-stat-GMA), subsequently collapsed by using B(C₆F₅)₃ as catalyst. Both the precursor polymer and the SCNPs can be well ionized via ESI MS, and the strong covalent cross-links are stable during ionization. Our high-resolution mass spectrometric approach can unambiguously differentiate between two mechanistic modes of chain collapse for every chain constituting the SCNP sample.

Publication types

Research Support, Non-U.S. Gov't