首页|Synergistic rare-earth yttrium single atoms and copper phosphide nanoparticles for high-selectivity ammonia electrosynthesis

Synergistic rare-earth yttrium single atoms and copper phosphide nanoparticles for high-selectivity ammonia electrosynthesis

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Electrochemical nitrate reduction to NH3 holds a great promise for N-upcycling in nature,while its slug-gish reaction kinetics involved in both the stepwise deoxygenation and hydrogenation processes necessitates the development of bespoke catalysts with multi-site engineering.Herein,we report a hybrid catalyst composed of rare-earth(RE)yttrium(Y)single atoms and copper phosphide(Cu3P)nanoparticles loaded on N,P-doped carbon(YSA-Cu3P/CNP)through a chelating and pyrolysis method.Owing to a synergistic contribution of Y single atoms and Cu3P nanoparticles,YSA-Cu3P/CNP achieves an impressive NH3 Faradaic efficiency(FE)of 92％at-0.5 V(vs.RHE)and the highest NH3 yield rate of 11.4 mg·h-1·cm-2 at-0.6 V(vs.RHE)in an alkaline media,which surpass most of the reported electrocatalysts.The intricate reaction pathway has been explored by online differential electrochemical mass spectrometry(DEMS),and the synergistic effect between Y single atoms and Cu3P nanoparticles has been studied by in situ synchrotron X-ray absorption spectroscopy.Moreover,density-functional theory(DFT)calculations unveil that the high-efficiency nitrate reduction on YSA-Cu3P/CNP is attributed to a reduced energy barrier of the rate-determining deoxy-genation step coupled with the enhanced stabilization of active hydrogen favorable for the hydrogenation steps,thereby boosting the overall reaction rates.In addition,a prototype Zn-nitrate battery utilizing YSA-Cu3P/CNP as the cathode is unveiled.This work not only elucidates the mechanism behind the enhanced catalytic performance but also paves the way for the future development of high-efficiency electrocatalysts through dual-site engineering.

Rare-earth single atomCu3P nanoparticleSynergistic electrocatalysisNitrate reduction reactionZn-nitrate battery

Yi-Meng Cai、Yang-Hua Li、Yi Xiao、Quentin Meyer、Qian Sun、Wan-Jing Lai、Shu-Wen Zhao、Jun Li、Lin-Jie Zhang、Han Wang、Zhang Lin、Jun Luo、Li-Li Han

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School of Materials Science and Engineering,Institute for New Energy Materials and Low-Carbon Technologies,Tianjin University of Technology,Tianjin 300384,China

State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China

School of Chemistry,The University of New South Wales,Sydney,NSW 2052,Australia

School of Metallurgy and Environment,Central South University,Changsha 410083,China

Chinese National Engineering Research Center for Control &Treatment of Heavy Metal Pollution,Changsha 410083,China J.Luo

ShenSi Lab,Shenzhen Institute for Advanced Study,University of Electronic Science and Technology of China,Shenzhen 518110,China

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2024

10.1007/s12598-024-02822-6

稀有金属(英文版)
中国有色金属学会

稀有金属(英文版)

CSTPCDEI
影响因子：0.801
ISSN：1001-0521
年,卷(期)：2024.43(11)