首页|Weak Acetylene Adsorption Terminated Carbon-Carbon Coupling Kinetics on Silver Electrocatalysts

Weak Acetylene Adsorption Terminated Carbon-Carbon Coupling Kinetics on Silver Electrocatalysts

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Owing to serious poison of downstream olefin poly-merization catalysts from acetylene impurities,selec-tive reduction of acetylene to ethylene is a pivotal process in petrochemical industry.However,during thermocatalytic and electrocatalytic acetylene semi-hydrogenation,acetylene C-C coupling inevitably occurs on current catalysts.The resultant oligomeric species(particularly long-chain hydrocarbons)block active sites and mass transportation,and eventually decrease catalytic activity and stability.In this work,we report Ag nanowires(NWs)as high-performance electrocatalysts for acetylene semihydrogenation,where the C-C coupling is unprecedentedly sup-pressed by weakening acetylene adsorption.In pure acetylene,1,3-butadiene Faradaic efficiency(FE)of Ag NWs is only 2.1％,which is far lower than 41.2％for Cu nanoparticles at-0.2 V versus reversible hydrso-gen electrode.Ethylene partial current density of Ag NWs reaches 217 mA/cm2 at 0.85 V,which is consid-erably higher than those for state-of-the-art Cu-based electrocatalysts.Markedly,no 1,3-butadiene is pro-duced on Ag NWs in a large two-electrode flow cell fed with crude ethylene containing 1 vol％acetylene,presenting thorough termination of acetylene C-C coupling.In situ electrochemical Raman spectroscopy and theoretical investigations reveal that weak acety-lene adsorption on Ag surfaces is intrinsically respon-sible for prohibiting their oligomerization.This work will spark the rapid development of high-performance and stable electrocatalysts for reducing alkynes to olefins.

acetyleneelectrocatalysiscarbon-carbon couplingsemihydrogenationsilver nanowires

Rui Bai、Jinjin Li、Jin Lin、Zhenpeng Liu、Chen Yan、Lei Zhang、Jian Zhang

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Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology,School of Chemistry and Chemical Engineering,Northwestern Polytechnical University,Xi'an,Shaanxi 710129

State Key Laboratory of Solidification Processing and School of Materials Science and Engineering,Northwestern Polytechnical University,Xi'an,Shaanxi 710072

Fundamental Research Funds for the Natural Science Foundation of Shaanxi ProvinceFundamental Research Funds for the Natural Science Foundation of Shaanxi Province国家自然科学基金国家自然科学基金国家重点研发计划Startup Fund of Northwest-ern Polytechnical University

2020JQ-1412021JQ-0942200524552101271SQ2021YFE010191D5000210090

2023

10.31635/ccschem.022.202101750

中国化学会会刊(英文)

中国化学会会刊(英文)

CSCD
ISSN：
年,卷(期)：2023.5(1)
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