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

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

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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 mgNH3·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.

nitrate electroreductionammonia electrosynthesissize effectsingle-cluster catalyst

Ran Li、Taotao Gao、Wenxi Qiu、Minghao Xie、Zhaoyu Jin、Panpan Li

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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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National Nature Science Foundation of ChinaSichuan Science and Technology ProgramSichuan Science and Technology ProgramFundamental Research Funds for the Central UniversitiesFundamental Research Funds for the Central UniversitiesChengdu University new faculty startup funding

522023722023NSFSC04362023NSFSC0089YJ202115120826041G41852081920074

2024

10.1007/s12274-023-6094-z

纳米研究(英文版)

纳米研究(英文版)

CSTPCD
ISSN：
年,卷(期)：2024.17(4)
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