Electrocatalytic nitrate reduction to ammonia on defective Au1Cu (111) single-atom alloys

Electrocatalytic reduction of nitrate (NO3–) to ammonia (NH3) in wastewater is a promising economic process for NH3 synthesis. This work designed and prepared Au1Cu (111) single-atom alloys with surface Cu vacancies (VCu-Au1Cu SAAs), which exhibited superior NH3 Faradaic efficiency (98.7%) with a pr...

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Vydáno v:Applied catalysis. B, Environmental Ročník 310; s. 121346
Hlavní autoři: Zhang, Yuanzheng, Chen, Xiang, Wang, Weilai, Yin, Lifeng, Crittenden, John C.
Médium: Journal Article
Jazyk:angličtina
Vydáno: Amsterdam Elsevier B.V 05.08.2022
Elsevier BV
Témata:
Alloys
Ammonia
Catalysts
Chemical reduction
Copper
Cu vacancy
Decay
Distillation
Electrocatalysis
Gold
Nitrate reduction
Single-atom alloys
Synthetic ammonia
Wastewater
Electrocatalysis
Single-atom alloys
Cu vacancy
Nitrate reduction
Synthetic ammonia
ISSN:0926-3373, 1873-3883
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Shrnutí:Electrocatalytic reduction of nitrate (NO3–) to ammonia (NH3) in wastewater is a promising economic process for NH3 synthesis. This work designed and prepared Au1Cu (111) single-atom alloys with surface Cu vacancies (VCu-Au1Cu SAAs), which exhibited superior NH3 Faradaic efficiency (98.7%) with a production rate of 555 μg h–1 cm–2 at −0.2 V vs. RHE, while negligible activity decay was found after a durability test. Meanwhile, 97% of produced NH3 can be recovered by a simple membrane distillation. Characterizations evidence that electron migration from Cu to Au atoms creates electron-deficient Cu active sites in VCu-Au1Cu SAAs, which promote the generation of active hydrogen species (*H) that can readily hydrogenate NO3–. Theoretical calculation reveals that the bi-functional Cu sites not only promote the activation of water to produce *H but also lower the energy barrier of *NH3 desorption from the catalyst surface. [Display omitted] ●Au1Cu single-atom alloys with surface Cu vacancies (VCu-Au1Cu SAAs) is reported.●A highly NH3 Faradaic efficiency of 98.7% is obtained on the VCu-Au1Cu SAAs.●VCu-Au1Cu SAAs promoted H2O dissociation to *H that boost NO3–-to-NH3 conversion.●DFT revealed the role of single-atom and vacancy defect on catalytic performance.
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ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2022.121346