Structure and Potential-Dependent Selectivity in Redox-Metallopolymers: Electrochemically Mediated Multicomponent Metal Separations

Raylin Chen, Jiangyan Feng, Jemin Jeon, Thomas Sheehan, Christian Rüttiger, Markus Gallei, Diwakar Shukla, Xiao Su

Research output: Contribution to journalArticlepeer-review

Abstract

Electro-responsive functional materials can play a critical role in selective metal recovery and recycling due to the need for molecular differentiation between transition metals in complex mixtures. Redox-active metallopolymers are a promising platform for electrochemical separations, offering versatile structural tuning and fast electron transfer. First, through a judicious selection of polymer structure between a main-chain metallopolymer (polyferrocenylsilane) and a pendant-group metallopolymer (polyvinylferrocene), charge-transfer interactions and binding strength toward competing metal ions are tuned, which as a result, dictate selectivity. For example, almost an order of magnitude increase in separation factor between chromate and meta-vanadate can be achieved, depending on polymer structure. Second, these metallopolymer electrodes exhibit potential-dependent selectivity that can even flip ion preference, based solely on electrical means—indicating a control parameter that is orthogonal to structural modifications. Finally, this work presents a framework for evaluating electrochemical separations in multicomponent ion mixtures and elucidates the underlying charge-transfer mechanisms resulting in molecular selectivity through a combination of spectroscopy and electronic structure calculations. The findings demonstrate the applicability of redox-metallopolymers in tailored electrochemical separations for environmental remediation, value-added metal recovery, waste recycling, and even mining processing.

Original languageEnglish (US)
Article number2009307
JournalAdvanced Functional Materials
Volume31
Issue number15
DOIs
StatePublished - Apr 8 2021

Keywords

  • electrochemical separations
  • electrosorption
  • metal recovery
  • metallopolymers
  • redox electrochemistry
  • water purification
  • water treatment

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics

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