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Research Article

Unveiling the size effect of nitrogen-doped carbon-supported copper-based catalysts on nitrate-to-ammonia electroreduction

Ran Li1,2, Taotao Gao2( ), Wenxi Qiu1, Minghao Xie3, Zhaoyu Jin4, Panpan Li1( )
College of Materials Science and Engineering, Sichuan University, Chengdu 610065, China
Institute for Advanced Study, Chengdu University, Chengdu 610106, China
Materials Science and Engineering Program and Walker Department of Mechanical Engineering, The University of Texas at Austin, Austin, Texas 78712, USA
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
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Graphical Abstract

The size-defined Cu nanoparticle, single-cluster, and single-atom catalysts have been prepared for studying the size effect on electrocatalytic nitrate-to-ammonia reduction.

Abstract

The electrocatalytic nitrate reduction reaction (NitRR) represents a promising approach toward achieving economically and environmentally sustainable ammonia. However, it remains a challenge to regulate the size effect of electrocatalysts to optimize the catalytic activity and ammonia selectivity. Herein, the Cu-based catalysts were tailored at the atomic level to exhibit a size gradient ranging from single-atom catalysts (SACs, 0.15–0.35 nm) to single-cluster catalysts (SCCs, 1.0–2.8 nm) and nanoparticles (NPs, 20–30 nm), with the aim of studying the size effect for the NO3−-to-NH3 reduction reaction. Especially, the Cu SCCs exhibit enhanced metal–substrate and metal–metal interactions by taking advantageous features of Cu SACs and Cu NPs. Thus, Cu SCCs achieve exceptional electrocatalytic performance for the NitRR with a maximum Faradaic efficiency of ca. 96% and the largest yield rate of ca. 1.99 mg NH3·h−1·cm−2 at −0.5 V vs. reversible hydrogen electrode (RHE). The theoretical calculation further reveals the size effect and coordination environment on the high catalytic activity and selectivity for the NitRR. This work provides a promising various size-controlled design strategy for aerogel-based catalysts effectively applied in various electrocatalytic reactions.

Keywords

nitrate electroreductionammonia electrosynthesissize effectsingle-cluster catalyst

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Nano Research
Volume 17 Issue 4,
April 2024
Pages 2438-2443
DOI: 10.1007/s12274-023-6094-z
Cite this article:
Li R, Gao T, Qiu W, et al. Unveiling the size effect of nitrogen-doped carbon-supported copper-based catalysts on nitrate-to-ammonia electroreduction. Nano Research, 2024, 17(4): 2438-2443. https://doi.org/10.1007/s12274-023-6094-z
Topics:
Catalyst activityElectrocatalysis Electrolytic reduction

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Received: 15 June 2023
Revised: 10 August 2023
Accepted: 14 August 2023
Published: 18 September 2023
© Tsinghua University Press 2023
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