Issue

Vol. 14 (2022)

Conversion of Catalytically Inert 2D Bismuth Oxide Nanosheets for Effective Electrochemical Hydrogen Evolution Reaction Catalysis via Oxygen Vacancy Concentration Modulation

https://doi.org/10.1007/s40820-022-00832-6
Ziyang Wu
School of Mechanical, Medical and Process Engineering, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Ting Liao
School of Mechanical, Medical and Process Engineering, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Sen Wang
School of Earth and Atmospheric Sciences, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Janith Adikaram Mudiyanselage
School of Chemistry and Physics, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Aaron S. Micallef
School of Chemistry and Physics, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Wei Li
School of Chemistry and Physics, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Anthony P. O’Mullane
Centre for Materials Science, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Jianping Yang
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, People’s Republic of China
Wei Luo
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, People’s Republic of China
Kostya Ostrikov
Centre for Materials Science, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Yuantong Gu
School of Mechanical, Medical and Process Engineering, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia
Ziqi Sun
Centre for Materials Science, Queensland University of Technology, 2 George Street, Brisbane, QLD 4000, Australia

Corresponding Author: Ziqi Sun

ziqi.sun@qut.edu.au

Nano-Micro Letters, Vol. 14 (2022), Article Number: 90

Abstract

Oxygen vacancies (Vo) in electrocatalysts are closely correlated with the hydrogen evolution reaction (HER) activity. The role of vacancy defects and the effect of their concentration, however, yet remains unclear. Herein, Bi2O3, an unfavorable electrocatalyst for the HER due to a less than ideal hydrogen adsorption Gibbs free energy (ΔGH*), is utilized as a perfect model to explore the function of Vo on HER performance. Through a facile plasma irradiation strategy, Bi2O3 nanosheets with different Vo concentrations are fabricated to evaluate the influence of defects on the HER process. Unexpectedly, while the generated oxygen vacancies contribute to the enhanced HER performance, higher Vo concentrations beyond a saturation value result in a significant drop in HER activity. By tunning the Vo concentration in the Bi2O3 nanosheets via adjusting the treatment time, the Bi2O3 catalyst with an optimized oxygen vacancy concentration and detectable charge carrier concentration of 1.52 × 1024 cm−3 demonstrates enhanced HER performance with an overpotential of 174.2 mV to reach 10 mA cm−2, a Tafel slope of 80 mV dec−1, and an exchange current density of 316 mA cm−2 in an alkaline solution, which approaches the top-tier activity among Bi-based HER electrocatalysts. Density-functional theory calculations confirm the preferred adsorption of H* onto Bi2O3 as a function of oxygen chemical potential (∆μO) and oxygen partial potential (PO2) and reveal that high Vo concentrations result in excessive stability of adsorbed hydrogen and hence the inferior HER activity. This study reveals the oxygen vacancy concentration-HER catalytic activity relationship and provides insights into activating catalytically inert materials into highly efficient electrocatalysts.


Highlights:


1 Catalytically inert 2D Bi2O3 is activated for boosting electrochemical hydrogen evolution reaction (HER) via oxygen vacancy concentration modulation.
2 The relationship between the varied oxygen vacancy concentrations and the corresponding HER activity is revealed by both experimental Vo verification and theoretical density-functional theory calculations.
3 This work provides insights into activating catalytically inert materials into high-performance catalysts.

Keywords

Alkaline hydrogen evolution reaction Bismuth oxide Plasma irradiation 2D materials Oxygen vacancy
Wu, Ziyang, Ting Liao, Sen Wang, Janith Adikaram Mudiyanselage, Aaron S. Micallef, Wei Li, Anthony P. O’Mullane, Jianping Yang, Wei Luo, Kostya Ostrikov, Yuantong Gu, and Ziqi Sun. 2022. “Conversion of Catalytically Inert 2D Bismuth Oxide Nanosheets for Effective Electrochemical Hydrogen Evolution Reaction Catalysis via Oxygen Vacancy Concentration Modulation”. Nano-Micro Letters 14 (April):90. https://doi.org/10.1007/s40820-022-00832-6.
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