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首页> 外文期刊>Advanced energy materials >Electron-Deficient Cu Sites on Cu_3Ag_1 Catalyst Promoting CO_2 Electroreduction to Alcohols
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Electron-Deficient Cu Sites on Cu_3Ag_1 Catalyst Promoting CO_2 Electroreduction to Alcohols

机译：Cu_3Ag_1催化剂上的电子缺陷Cu位点促进CO_2电荷对醇

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摘要

Copper-based catalysts electrochemically convert CO(2)into multicarbon molecules. However, the selectivity toward alcohol products has remained relatively low, due to the lack of catalysts favoring the adsorption of key intermediates in the alcohol pathways. Herein, a Cu(3)Ag(1)electrocatalyst is developed using galvanic replacement of an electrodeposited Cu matrix. The Cu(3)Ag(1)electrocatalyst enables a 63% Faradaic efficiency for CO2-to-alcohol production and an alcohol partial current density of -25 mA cm(-2)at -0.95 V versus reversible hydrogen electrode, corresponding to a 126-fold enhancement in selectivity and 25-fold increase in activity compared to the bare electrodeposited Cu matrix. Density functional theory calculations reveal that the interphase electron transfer from Cu to Ag generates electron-deficient Cu sites and favors the adsorption of CO(2)reduction intermediates in the alcohol pathway, such as CH3CHO* and CH3CH2O*. Thus, for this electron-deficient catalyst, the C2H5OH pathway is more preferable than the ethylene (C2H4) pathway, endowing the catalyst with an alcohol/ethylene ratio of 38:1. These findings suggest both experimental approaches and theoretical insights for exploring highly selective CO2-to-alcohol conversion.
机译：铜基催化剂将CO（2）电化学转化为多碳分子。然而，由于缺乏醇途径的催化剂缺乏催化剂，对醇产物的选择性相对较低。在此，使用电沉积的Cu基质的电常用替代来开发Cu（3）Ag（1）电催化剂。 Cu（3）Ag（1）电催化剂能够在-0.95V与可逆氢电极的-25mAcm（-2）的-25mA cm（-2）的醇部分电流密度的63％的佛兰施效率。与裸电沉积Cu基质相比，选择性126倍的选择性和25倍的增加。密度函数理论计算表明，来自Cu至Ag的相互电子转移产生电子缺陷的Cu位点，并有利于在醇途径中的Co（2）还原中间体的吸附，例如CH3CHO *和CH 3 CH 2 O *。因此，对于这种电子缺陷型催化剂，比乙​​烯（C2H4）途径更优选C 2 HOH途径，赋予醇/乙烯比为38：1的催化剂。这些研究结果表明，探索高度选择性二氧化碳对酒精转化的实验方法和理论见解。

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  • 来源
    《Advanced energy materials》 |2020年第37期|2001987.1-2001987.8|共8页
  • 作者

    Lv Ximeng; Shang Longmei; Zhou Si; Li Si; Wang Yuhang; Wang Zhiqiang; Sham Tsun-Kong; Peng Chen; Zheng Gengfeng;

  • 作者单位

    Fudan Univ Adv Mat Lab Dept Chem Shanghai 200438 Peoples R China|Fudan Univ Shanghai Key Lab Mol Catalysis & Innovat Mat Shanghai 200438 Peoples R China;

    Fudan Univ Adv Mat Lab Dept Chem Shanghai 200438 Peoples R China|Fudan Univ Shanghai Key Lab Mol Catalysis & Innovat Mat Shanghai 200438 Peoples R China;

    Dalian Univ Technol Key Lab Mat Modificat Laser Ion & Electron Beams Minist Educ Dalian 116024 Peoples R China;

    Fudan Univ Adv Mat Lab Dept Chem Shanghai 200438 Peoples R China|Fudan Univ Shanghai Key Lab Mol Catalysis & Innovat Mat Shanghai 200438 Peoples R China;

    Fudan Univ Adv Mat Lab Dept Chem Shanghai 200438 Peoples R China|Fudan Univ Shanghai Key Lab Mol Catalysis & Innovat Mat Shanghai 200438 Peoples R China;

    Univ Western Ontario Dept Chem London ON N6A 5B7 Canada|Univ Western Ontario Soochow Univ Western Univ Ctr Synchrotron Radiat London ON N6A 5B7 Canada;

    Univ Western Ontario Dept Chem London ON N6A 5B7 Canada|Univ Western Ontario Soochow Univ Western Univ Ctr Synchrotron Radiat London ON N6A 5B7 Canada;

    Fudan Univ Adv Mat Lab Dept Chem Shanghai 200438 Peoples R China|Fudan Univ Shanghai Key Lab Mol Catalysis & Innovat Mat Shanghai 200438 Peoples R China;

    Fudan Univ Adv Mat Lab Dept Chem Shanghai 200438 Peoples R China|Fudan Univ Shanghai Key Lab Mol Catalysis & Innovat Mat Shanghai 200438 Peoples R China;

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  • 正文语种 eng
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  • 关键词

    alcohols; CO(2)reduction; electrocatalysis; electron-deficient; Faradaic efficiency;

    机译：醇类;CO（2）减少;电催化;电子缺陷;佛罗里达州效率;

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