Theoretical Evaluation of Highly Efficient Nitrate Reduction to Ammonia on InBi

Qingchao Fang; Hanqing Yin; Xin Mao; Yun Han; Cheng Yan; Anthony P O'Mullane; Aijun Du

doi:10.1021/acs.jpclett.2c03900

Theoretical Evaluation of Highly Efficient Nitrate Reduction to Ammonia on InBi

J Phys Chem Lett. 2023 Mar 9;14(9):2410-2415. doi: 10.1021/acs.jpclett.2c03900. Epub 2023 Mar 1.

Authors

Qingchao Fang¹, Hanqing Yin^{1

2}, Xin Mao¹, Yun Han³, Cheng Yan⁴, Anthony P O'Mullane¹, Aijun Du^{1

2}

Affiliations

¹ School of Chemistry and Physics, Queensland University of Technology (QUT), Gardens Point Campus, Brisbane, Queensland, 4000, Australia.
² QUT Centre for Materials Science, Queensland University of Technology (QUT), Gardens Point Campus, Brisbane, Queensland, 4000, Australia.
³ School of Engineering and Built Environment, Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Nathan, Queensland 4111, Australia.
⁴ School of Mechanical, Medical and Process Engineering, Queensland University of Technology (QUT), Gardens Point Campus, Brisbane, Queensland 4000, Australia.

PMID: 36856465
DOI: 10.1021/acs.jpclett.2c03900

Abstract

Electrocatalytic reduction of nitrate to ammonia has become a popular approach for wastewater treatment and ammonia production. However, the development of highly efficient electrocatalysts remains a great challenge. Herein, we systematically studied the potential of InBi for nitrate reduction to ammonia (NRA) based on density functional theory (DFT) calculations. Our results reveal that InBi exhibits high activity for NRA via an O-end pathway, where the free energy evolution of all intermediates is downhill in the most favorable elementary steps. The activation of nitrate originates from the strong orbital hybridization between oxygen and indium atoms, leading to an enhanced charge transfer as well as NO₃^- adsorption. In particular, the competing hydrogen evolution reaction (HER) is effectively suppressed due to the weak adsorption of proton. Our study not only proves the great electrocatalytic potential of InBi as a novel catalyst for NRA but also points out a new way to design NRA electrocatalysts for practical applications.