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Accelerating CO_2 Electroreduction to CO Over Pd Single-Atom Catalyst

机译：钯单原子催化剂上促进CO_2电还原为CO

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摘要

The electrochemical conversion of carbon dioxide (CO2) into value-added chemicals is regarded as one of the promising routes to mitigate CO2 emission. A nitrogen-doped carbon-supported palladium (Pd) single-atom catalyst that can catalyze CO2 into CO with far higher mass activity than its Pd nanoparticle counterpart, for example, 373.0 and 28.5 mA mg(Pd)(-1), respectively, at -0.8 V versus reversible hydrogen electrode, is reported. A combination of in situ X-ray characterization and density functional theory (DFT) calculation reveals that the Pd-N-4 site is the most likely active center for CO production without the formation of palladium hydride (PdH), which is essential for typical Pd nanoparticle catalysts. Furthermore, the well-dispersed Pd-N-4 single-atom site facilitates the stabilization of the adsorbed CO2 intermediate, thereby enhancing electrocatalytic CO2 reduction capability at low overpotentials. This work provides important insights into the structure-activity relationship for single-atom based electrocatalysts.
机译：二氧化碳（CO2）电化学转化为增值化学品被认为是减轻CO2排放的有前途的途径之一。氮掺杂的碳负载钯（Pd）单原子催化剂，其催化活性可以远高于其Pd纳米颗粒对应物，例如可以将CO2转化为CO，例如分别为373.0和28.5 mA mg（Pd）（-1）。报道了相对于可逆氢电极在-0.8 V下的电压。原位X射线表征和密度泛函理论（DFT）计算的结合表明，Pd-N-4位点是最可能产生CO的活性中心，而不会形成氢化钯（PdH），这对于典型的合成氢至关重要。钯纳米颗粒催化剂。此外，分散良好的Pd-N-4单原子位点有助于稳定所吸附的CO2中间体，从而在低超电势下增强电催化CO2还原能力。这项工作为基于单原子的电催化剂的结构-活性关系提供了重要的见识。

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  • 来源
    《Advanced Functional Materials》 |2020年第17期|2000407.1-2000407.8|共8页
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    Columbia Univ Dept Chem Engn New York NY 10027 USA|Univ Sci & Technol China CAS Ctr Excellence Nanosci Natl Synchrotron Radiat Lab Hefei 230029 Anhui Peoples R China;

    Columbia Univ Dept Chem Engn New York NY 10027 USA;

    Nanyang Technol Univ Sch Mat Sci & Engn Singapore 639798 Singapore;

    Brookhaven Natl Lab Div Chem Upton NY 11973 USA;

    Brookhaven Natl Lab Ctr Funct Nanomat Upton NY 11973 USA;

    Florida A&M Univ Dept Phys Tallahassee FL 32307 USA;

    Univ Sci & Technol China CAS Ctr Excellence Nanosci Natl Synchrotron Radiat Lab Hefei 230029 Anhui Peoples R China;

    Columbia Univ Dept Chem Engn New York NY 10027 USA|Brookhaven Natl Lab Div Chem Upton NY 11973 USA;

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  • 正文语种 eng
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  • 关键词

    CO2 electroreduction; density functional theory; palladium; single-atom catalysis; X-ray absorption spectroscopy;

    机译：二氧化碳电还原密度泛函理论;钯;单原子催化;X射线吸收光谱;

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