Enhanced localized electron density from PdCu nanoparticle loading on a defective TiO2 support for selective nitrate electroreduction to ammonia


Wu, H, Guo, H ORCID: 0000-0002-8117-6790, Zhang, F, Yang, P, Liu, J, Yang, Y, Huang, ZF ORCID: 0000-0001-9656-9186, Zhu, C, Wang, W, Tu, X ORCID: 0000-0002-6376-0897 et al (show 2 more authors) (2023) Enhanced localized electron density from PdCu nanoparticle loading on a defective TiO2 support for selective nitrate electroreduction to ammonia Journal of Materials Chemistry A, 11 (41). pp. 22466-22477. ISSN 2050-7488, 2050-7496

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Abstract

The electrocatalytic nitrate (NO<inf>3</inf>−) reduction reaction (NITRR) to synthesize ammonia (NH<inf>3</inf>) offers a promising method for both pollution abatement and chemical production. However, the sluggish multi-electron/proton-involved steps limit ammonia selectivity and yield. Herein, we loaded PdCu nanoparticles (PdCu NPs) onto defective TiO<inf>2</inf> to regulate the localized electron density for selective NH<inf>3</inf> synthesis. Our results show a significant increase in NH<inf>3</inf> yield and selectivity (112.0 to 322.7 μmol cm−2 h−1 and 34.6 to 80.1%, respectively), induced by the introduction of PdCu NPs. Importantly, in situ and operando investigations combined with density functional theory (DFT) calculations reveal that PdCu NPs enhance the localized electron density at oxygen vacancies. This regulated electron density suppresses N-N coupling and accelerates N-H bonding processes, thus modulating NH<inf>3</inf> selectivity. This unique insight based on localized electron density control provides a rational design strategy for metal-defect support catalysts in ammonia production using electrochemical processes.

Item Type: Article
Uncontrolled Keywords: 40 Engineering, 34 Chemical Sciences, 4018 Nanotechnology, 3406 Physical Chemistry, Nanotechnology, Bioengineering
Divisions: Faculty of Science & Engineering > School of Electrical Engineering, Electronics and Computer Science
Depositing User: Symplectic Admin
Date Deposited: 06 Nov 2023 15:41
Last Modified: 22 Jan 2026 12:26
DOI: 10.1039/d3ta04155g
Open Access URL: https://pubs.rsc.org/en/content/articlelanding/202...
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URI: https://livrepository.liverpool.ac.uk/id/eprint/3176662
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