Nitrate-to-ammonia conversion with a plasmonic antenna-reactor catalyst

Weihui Ou*, Ying Guo, Jing Zhong, Fucong Lyu, Junda Shen, Hongkun Li, Shaoce Zhang, Zebiao Li, Zhijian He, Jun He, Quanxi Mo, Chunyi Zhi*, Yang Yang Li*, Jian Lu*

*Corresponding author for this work

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

4 Citations (Scopus)

Abstract

Electrochemical conversion of nitrate to ammonia is an appealing route to efficiently synthesize ammonia under ambient conditions while reducing environmental nitrate pollutants. However, this approach is obstructed by the limited yield and selectivity of ammonia because the electrochemical nitrate-to-ammonia conversion involves multi-electron/proton transfer and faces competition from the hydrogen evolution reaction. Here, we demonstrate a plasmon-assisted strategy to improve the performance of nitrate-to-ammonia electrochemical conversion by constructing plasmonic antenna-reactor catalysts, where Au and Pd nanoparticles/hydrogen substituted graphdiyne (Pd/HsGDY) work as the light antenna and reaction site, respectively. Plasmonic excitation of Au-Pd/HsGDY catalysts can remarkably accelerate the nitrate reduction, with the yield rate, selectivity, and Faradaic efficiency of ammonia respectively increased by 14.3, 2.1, and 1.8 times under optimal conditions. Mechanistic investigations unveil that Au plasmon-induced hot electrons facilitate nitrate-to-ammonia reaction by regulating the adsorption of reaction intermediates on Pd/HsGDY, wherein the rate-determining step was shifted from nitrate adsorption to *NH protonation and the overall apparent activation was reduced. Moreover, hot electrons suppress the competing hydrogen evolution by enlarging the Gibbs free energy of hydrogen formation. These results open a way to develop desirable catalysts for producing value-added ammonia from environmentally hazardous nitrate by a synergistic combination of electricity and light. © 2024 The Royal Society of Chemistry.
Original languageEnglish
Pages (from-to)1673-1682
JournalEnergy and Environmental Science
Volume18
Issue number4
Online published27 Nov 2024
DOIs
Publication statusPublished - 21 Feb 2025

Funding

This work was jointly supported by the Innovation and Technology Commission of HKSAR through the Hong Kong Branch of the National Precious Metals Material Engineering Research Centre, the Research Grants Council of Hong Kong (GRF grant no. 15304519), the National Natural Science Foundation of China (22408055), the Foundation of Basic and Applied Basic Research of Guangdong Province (2023A1515110233), the Foundation of Basic and Applied Basic Research of Guangzhou (SL2024A04J00921), and the Guangdong Province Science and Technology Plan Project (2023B1212120008). Prof. Lu thanks the support from Guangdong-Hong Kong Joint Laboratory of Modern Surface Engineering Technology, City University of Hong Kong, Hong Kong, China.

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