Polymeric viologen-based electron transfer mediator for improving the photoelectrochemical water splitting on Sb2Se3 photocathode

Chang Liu ¹Fusheng Li ¹Linqin Wang ²Zeju Li ¹Yilong Zhao ¹Yingzheng Li ¹Wenlong Li ¹Ziqi Zhao ¹Ke Fan ¹Fei Li ¹Licheng Sun³

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作者信息

1. State Key Laboratory of Fine Chemicals,Institute of Artificial Photosynthesis,DUT-KTH Joint Education and Research Centre on Molecular Devices,Institute for Energy Science and Technology,Dalian University of Technology,Dalian 116024,China
2. Center of Artificial Photosynthesis for Solar Fuels,School of Science,Westlake University,Hangzhou 310024,China
3. State Key Laboratory of Fine Chemicals,Institute of Artificial Photosynthesis,DUT-KTH Joint Education and Research Centre on Molecular Devices,Institute for Energy Science and Technology,Dalian University of Technology,Dalian 116024,China;Center of Artificial Photosynthesis for Solar Fuels,School of Science,Westlake University,Hangzhou 310024,China;Department of Chemistry,School of Engineering Sciences in Chemistry,Biotechnology and Health,KTH Royal Institute of Technology,Stockholm 10044,Sweden
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Abstract

The photogenerated charge carrier separation and transportation of inside photocathodes can greatly influence the performance of photoelectrochemical(PEC)H2 production devices.Coupling TiO2 with p-type semiconduc-tors to construct heterojunction structures is one of the most widely used strategies to facilitate charge separation and transportation.However,the band position of TiO2 could not perfectly match with all p-type semiconductors.Here,taking antimony selenide(Sb2Se3)as an example,a rational strategy was developed by introducing a vio-logen electron transfer mediator(ETM)containing polymeric film(poly-1,1'-dially-[4,4'-bipyridine]-1,1'-diium,denoted as PV2+)at the interface between Sb2Se3 and TiO2 to regulate the energy band alignment,which could inhibit the recombination of photogenerated charge carriers of interfaces.With Pt as a catalyst,the constructed Sb2Se3/PV2+/TiO2/Pt photocathode showed a superior PEC hydrogen generation activity with a photocurrent density of-18.6 mA cm-2 vs.a reversible hydrogen electrode(RHE)and a half-cell solar-to-hydrogen efficiency(HC-STH)of 1.54％at 0.17 V vs.RHE,which was much better than that of the related Sb2Se3/TiO2/Pt photo-cathode without PV2+(-9.8 mA cm-2,0.51％at 0.10 V vs.RHE).

Key words

Viologen/Electron transfer mediator/Sb2Se3 photocathode/Solar water splitting/Hydrogen evolution reaction

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基金项目

Fundamental Research Center of Artificial Photosynthesis(FReCAP)()

国家自然科学基金(22172011)

国家自然科学基金(22088102)

K & A Wallenberg Foundation(KAW 2016.0072)

Key Laboratory of Biobased Chemicals of Liaoning Province of China()

Zhejiang Province Selected Funding for Postdoctoral Research Projects(ZJ2021001)

出版年

2024

自然科学基础研究(英文)

CSTPCD

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参考文献量50

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