Issue 20, 2023

Low-coordination single Ni atoms on graphitic C3N4 for nitrite electroreduction to ammonia

Abstract

Electrocatalytically converting NO2 to NH3 (NO2RR) offers an attractive approach to realize both hazardous NO2 abatement and sustainable NH3 production. Single-atom catalysts (SACs) show a great potential for N-cycle electrocatalysis, whereas their application for the NO2RR remain largely unexplored. In this study, isolated Ni atoms on graphitic C3N4 (Ni1/C3N4) are explored as an efficient catalyst towards the NO2RR. Atomic coordination characterizations reveal the construction of low-coordination Ni1–N2 moieties on Ni1/C3N4. Theoretical calculations unveil that Ni1–N2 moieties serve as active centers to promote the activation of NO2 and minimize the energy barrier of the *NO → *NOH rate-determining step, whilst inhibiting the competitive hydrogen evolution. As a result, Ni1/C3N4 exhibits a high NH3-faradaic efficiency of 96.9% with a corresponding NH3 yield rate of 483.3 μmol h−1 cm−2 at −0.7 V. RHE, along with an excellent electrocatalytic stability.

Graphical abstract: Low-coordination single Ni atoms on graphitic C3N4 for nitrite electroreduction to ammonia

Supplementary files

Article information

Article type
Research Article
Submitted
24 ጁላይ 2023
Accepted
06 ሴፕቴ 2023
First published
06 ሴፕቴ 2023

Inorg. Chem. Front., 2023,10, 5950-5957

Low-coordination single Ni atoms on graphitic C3N4 for nitrite electroreduction to ammonia

H. Zhao, J. Xiang, G. Zhang, K. Chen and K. Chu, Inorg. Chem. Front., 2023, 10, 5950 DOI: 10.1039/D3QI01425H

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