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A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction

机译：分子表面功能化方法以调节用于还原二氧化碳的纳米粒子电催化剂

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摘要

Conversion of the greenhouse gas carbon dioxide (CO_2) to value-added products is an important challenge for sustainable energy research, and nanomaterials offer a broad class of heterogeneous catalysts for such transformations. Here we report a molecular surface functionalization approach to tuning gold nanoparticle (Au NP) electrocatalysts for reduction of CO_2 to CO. The N-heterocyclic (NHC) carbene-functionalized Au NP catalyst exhibits improved faradaic efficiency (FE = 83%) for reduction of CO_2 to CO in water at neutral pH at an overpotential of 0.46 V with a 7.6-fold increase in current density compared to that of the parent Au NP (FE = 53%). Tafel plots of the NHC carbene-functionalized Au NP (72 mV/decade) vs parent Au NP (138 mV/decade) systems further show that the molecular ligand influences mechanistic pathways for CO_2 reduction. The results establish molecular surface functionalization as a complementary approach to size, shape, composition, and defect control for nanoparticle catalyst design.
机译：将温室气体二氧化碳（CO_2）转化为增值产品是可持续能源研究的重要挑战，纳米材料为此类转化提供了广泛的非均相催化剂。在这里，我们报告了一种分子表面官能化方法，用于调节金纳米颗粒（Au NP）电催化剂以将CO_2还原为CO。N-杂环（NHC）卡宾官能化的Au NP催化剂显示出降低的法拉第效率（FE = 83％）与母金Au NP（FE = 53％）相比，在中性pH值为0.46 V的超电势下水中的CO_2至CO的电流密度增加了7.6倍。 NHC卡宾官能化的金纳米颗粒（72 mV /十年）与母金纳米颗粒（138毫伏/十年）的Tafel图进一步表明，分子配体影响了CO_2还原的机理。结果确定了分子表面功能化作为纳米颗粒催化剂设计的尺寸，形状，组成和缺陷控制的补充方法。

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  • 来源
    《Journal of the American Chemical Society》 |2016年第26期|8120-8125|共6页
  • 作者

    Zhi Cao; Dohyung Kim; Dachao Hong; Yi Yu; Jun Xu; Song Lin; Xiaodong Wen; Eva M. Nichols; Keunhone Jeong; Jeffrey A. Reimer; Peidong Yang; Christopher J. Chang;

  • 作者单位

    Department of Chemistry University of California, Berkeley, California 94720, United States;

    Department of Materials Science and Engineering, University of California, Berkeley, California 94720, United States;

    Department of Chemistry University of California, Berkeley, California 94720, United States;

    Department of Chemistry University of California, Berkeley, California 94720, United States,Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States;

    Department of Chemistry University of California, Berkeley, California 94720, United States;

    Department of Chemistry University of California, Berkeley, California 94720, United States,Chemical Sciences Division Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States;

    Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi 030001, China,Synfuels China, Beijing 100195, China;

    Department of Chemistry University of California, Berkeley, California 94720, United States,Chemical Sciences Division Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States;

    Department of Chemistry University of California, Berkeley, California 94720, United States;

    Department of Chemistry University of California, Berkeley, California 94720, United States;

    Department of Chemistry University of California, Berkeley, California 94720, United States,Department of Materials Science and Engineering, University of California, Berkeley, California 94720, United States,Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States,Kavli Energy Nanosciences Institute, Berkeley, California 94720, United States;

    Department of Chemistry University of California, Berkeley, California 94720, United States,Department of Molecular and Cell Biology, University of California, Berkeley, California 94720, United States,Howard Hughes Medical Institute, University of California, Berkeley, California 94720, United States,Chemical Sciences Division Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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  • 入库时间 2022-08-18 03:08:50

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