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Photoinduction of Cu Single Atoms Decorated on UiO-66-NH_2 for Enhanced Photocatalytic Reduction of CO_2 to Liquid Fuels

机译:UIO-66-NH_2上装饰的Cu单个原子的光诱导,用于增强光催化还原CO_2至液体燃料

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摘要

Photocatalytic reduction of CO_2 to value-added fuels is a promising route to reduce global warming and enhance energy supply. However, poor selectivity and low efficiency of catalysts are usually the limiting factor of their applicability. Herein, a photoinduction method was developed to achieve the formation of Cu single atoms on a UiO-66-NH_2 support (Cu SAs/UiO-66-NH_2) that could significantly boost the photoreduction of CO_2 to liquid fuels. Notably, the developed Cu SAs/UiO-66-NH_2 achieved the solar-driven conversion of CO_2 to methanol and ethanol with an evolution rate of 5.33 and 4.22 μmol h~(-1) g~(-1), respectively. These yields were much higher than those of pristine UiO-66-NH_2 and Cu nanoparticles/UiO-66-NH_2 composites. Theoretical calculations revealed that the introduction of the Cu SAs on the UiO-66-NH_2 greatly facilitates the conversion of CO_2 to CHO* and CO* intermediates, leading to excellent selectivity toward methanol and ethanol. This study provides new insights for designing high-performance catalyst for photocatalytic reduction of CO_2 at the atomic scale.
机译:将CO_2的光催化还原为增值燃料是减少全球变暖和增强能量供应的有希望的途径。然而,催化剂的选择性差和低效率通常是其适用性的限制因素。在此,开发了一种光诱导方法以在UIO-66-NH_2载体(Cu SAS / UIO-66-NH_2)上实现Cu单原子的形成,其可以显着提高CO_2的光电至液体燃料。值得注意的是,开发的Cu SAS / UIO-66-NH_2分别实现了CO_2至甲醇和乙醇的太阳能驱动转化,其演化速率分别为5.33和4.22μmolH〜(-1)g〜(-1)。这些产率远高于原始UIO-66-NH_2和Cu纳米颗粒/ UIO-66-NH_2复合材料。理论计算表明,UIO-66-NH_2上的Cu SAS的引入大大促进了CO_2对CHO *和CO *中间体的转化,导致对甲醇和乙醇的优异选择性。本研究提供了用于设计用于在原子尺度上的光催化减少CO_2的高性能催化剂的新见解。

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  • 来源
    《Journal of the American Chemical Society》 |2020年第45期|19339-19345|共7页
  • 作者单位

    Key Laboratory of Functional Molecular Solids Ministry of Education College of Chemistry and Materials Science Anhui Normal University Wuhu 241002 China;

    Key Laboratory of Functional Small Organic Molecule Ministry of Education College of Chemistry and Chemical Engineering Jiangxi Normal University Nanchang 330022 China;

    Key Laboratory of Functional Molecular Solids Ministry of Education College of Chemistry and Materials Science Anhui Normal University Wuhu 241002 China;

    Department of Chemistry Tsinghua University Beijing 100084 China;

    Key Laboratory of Functional Molecular Solids Ministry of Education College of Chemistry and Materials Science Anhui Normal University Wuhu 241002 China;

    Department of Chemistry Tsinghua University Beijing 100084 China;

  • 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);
  • 原文格式 PDF
  • 正文语种 eng
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  • 入库时间 2022-08-18 22:16:54

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