Strain-promoted conductive metal-benzenhexathiolate frameworks for overall water splitting

Xiting Wang; Huan Niu; Xuhao Wan; Zhaofu Zhang; Feng Ryan Wang; Yuzheng Guo

doi:10.1016/j.jcis.2022.05.127

Strain-promoted conductive metal-benzenhexathiolate frameworks for overall water splitting

J Colloid Interface Sci. 2022 Oct 15:624:160-167. doi: 10.1016/j.jcis.2022.05.127. Epub 2022 May 25.

Authors

Xiting Wang¹, Huan Niu¹, Xuhao Wan¹, Zhaofu Zhang², Feng Ryan Wang³, Yuzheng Guo⁴

Affiliations

¹ School of Electrical Engineering and Automation, Wuhan University, Wuhan 430072, Hubei, China.
² Department of Engineering, University of Cambridge, Cambridge CB2 1PZ, United Kingdom.
³ Departments of Chemical Engineering, University College London, Torrington Place, London WC1E 7JE, United Kingdom.
⁴ School of Electrical Engineering and Automation, Wuhan University, Wuhan 430072, Hubei, China. Electronic address: yguo@whu.edu.cn.

PMID: 35660885
DOI: 10.1016/j.jcis.2022.05.127

Abstract

Designing efficient catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is a desirable strategy for overall water splitting and the generation of clean and renewable energies. Herein, the electrocatalytic HER and OER activity of the conductive metal-benzenhexathiolate (M-BHT) frameworks has been evaluated utilizing first-principles calculations. The in-plane π-d conjugation of M-BHT guarantees fast electron transfer during electrocatalytic reactions. Notably, Rh-BHT holds the promise of bifunctional HER/OER activity with the overpotentials of 0.07/0.36 V. Furthermore, the application of strain engineering tailors the adsorption of intermediates and promotes the overall water splitting performance. Rh-BHT with the +1% tensile strain shows the HER/OER overpotential of 0.02/0.37 V. This work not only demonstrates the prospects of conductive metal-organic frameworks in electrocatalysis but also offers new insights into designing efficient catalysts by strain engineering.

Keywords: Electrocatalysis; First-principles calculations; Metal-organic frameworks; Overall water splitting; Strain engineering.