Mechanistic studies of the photo-electrochemical hydrogen evolution reaction on poly(2,2′-bithiophene)

Chun Hin Ng, C. André Ohlin, Siyao Qiu, Chenghua Sun, Bjorn Winther-Jensen

Research output: Contribution to journalArticleResearchpeer-review

5 Citations (Scopus)

Abstract

The realisation of poly(2,2′-bithiophene) (PBTh) as an effective photo-electrocatalyst for the hydrogen evolution reaction is a novel discovery [Ng et al., Int. J. Hydrogen Energy, 2014, 39, 18230]; however, the underlying mechanism of this catalysis remains unknown. In this article, studies using electrochemical, photo-electrochemical, Raman spectroscopy and computational modelling are undertaken to shed some light on the mechanistic process. From these studies, a compelling reaction scheme is proposed involving the protonation of the PBTh chain via the sulphur atom and subsequent intersystem crossing to a long-lived triplet state for the reaction to form H2. This suggested mechanism is tentative but cohesively integrates all experimental and computational findings. Importantly, these insights into the PBTh system form an important mechanistic milestone study and will help inspire new developments and applications for polythiophenes and conducting polymers.

Original languageEnglish
Pages (from-to)3253-3262
Number of pages10
JournalCatalysis Science & Technology
Volume6
Issue number9
DOIs
Publication statusPublished - 2016

Cite this

Ng, Chun Hin ; Ohlin, C. André ; Qiu, Siyao ; Sun, Chenghua ; Winther-Jensen, Bjorn. / Mechanistic studies of the photo-electrochemical hydrogen evolution reaction on poly(2,2′-bithiophene). In: Catalysis Science & Technology. 2016 ; Vol. 6, No. 9. pp. 3253-3262.
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Mechanistic studies of the photo-electrochemical hydrogen evolution reaction on poly(2,2′-bithiophene). / Ng, Chun Hin; Ohlin, C. André; Qiu, Siyao; Sun, Chenghua; Winther-Jensen, Bjorn.

In: Catalysis Science & Technology, Vol. 6, No. 9, 2016, p. 3253-3262.

Research output: Contribution to journalArticleResearchpeer-review

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AU - Winther-Jensen, Bjorn

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AB - The realisation of poly(2,2′-bithiophene) (PBTh) as an effective photo-electrocatalyst for the hydrogen evolution reaction is a novel discovery [Ng et al., Int. J. Hydrogen Energy, 2014, 39, 18230]; however, the underlying mechanism of this catalysis remains unknown. In this article, studies using electrochemical, photo-electrochemical, Raman spectroscopy and computational modelling are undertaken to shed some light on the mechanistic process. From these studies, a compelling reaction scheme is proposed involving the protonation of the PBTh chain via the sulphur atom and subsequent intersystem crossing to a long-lived triplet state for the reaction to form H2. This suggested mechanism is tentative but cohesively integrates all experimental and computational findings. Importantly, these insights into the PBTh system form an important mechanistic milestone study and will help inspire new developments and applications for polythiophenes and conducting polymers.

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