In:
Journal of Materials Chemistry A, Royal Society of Chemistry (RSC)
Abstract:
Electrocatalytic nitrate (NO3-) reduction reaction (NITRR) to synthesize ammonia (NH3) synthesis 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 TiO2 to regulate the localized electron density for selective NH3 synthesis. Our results show a significant increase in NH3 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 NH3 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.
Type of Medium:
Online Resource
ISSN:
2050-7488
,
2050-7496
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2023
detail.hit.zdb_id:
2702232-8
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