Localized Geometry Determined Selectivity of Iodide-Derived Copper for Electrochemical CO_2 Reduction

Yuchuan Shi; Yiqing Wang; Chung-Li DongTa Thi Thuy NgaDaixing WeiJialin WangXiaoli ZhaoMiao WangKaini ZhangMingtao LiFan DongShaohua Shen

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Localized Geometry Determined Selectivity of Iodide-Derived Copper for Electrochemical CO_2 Reduction

机译：Localized Geometry Determined Selectivity of Iodide-Derived Copper for Electrochemical CO_2 Reduction

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Two iodide-derived copper (ID-Cu) electrocatalysts (E-ID-Cu and W-ID-Cu)are prepared by electrochemical/wet chemical iodination of Cu foil andsubsequent in situ electrochemical reduction reaction. In comparison toelectropolished Cu (EP-Cu), both E-ID-Cu and W-ID-Cu can produce multicarbon(C_(2+)) products with much-improved selectivity, with Faradic efficiency(FE) reaching 64.39% for E-ID-Cu and 71.16% for W-ID-Cu at ?1.1 V versusreversible hydrogen electrodes (RHE), which can be attributed to their localizedgeometry features with high defect density and high surface roughness.Given the well-determined FEs towards C_(2+) products, the partial current densitiesfor C_(2+) production can be estimated to be 251.8 mA cm~(?2) for E-ID-Cuand 290.0 mA cm~(?2) for W-ID-Cu at ?1.2 V versus RHE in a flow cell. In situcharacterizations and theoretical calculations reveal that the high-densitydefects and high surface roughness can promote *CO adsorption by raisingthe d band center and then facilitate C–C coupling, contributing to the highselectivity of C_(2+) products for ID-Cu. Interestingly, the high surface roughnesscan increase the residence time of *C–H intermediates and decreasethe formation energy of the *OCCO and*CH_3CH_2O intermediates, thusfavoring C_(2+) production, with a unique C_2H_6 product observed over W-ID-Cuwith FE of 10.14% at ?0.7 V versus RHE.

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来源
《Advanced energy materials》 |2023年第11期|2203896.1-2203896.11|共11页
作者
Yuchuan Shi; Yiqing Wang; Chung-Li DongTa Thi Thuy NgaDaixing WeiJialin WangXiaoli ZhaoMiao WangKaini ZhangMingtao LiFan DongShaohua Shen;
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作者单位

International Research Center for Renewable EnergyState Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049, P. R. China;

Department of PhysicsTamkang UniversityNew Taipei City 25137, Taiwan;

School of Resources and EnvironmentUniversity of Electronic Science and Technology of ChinaChengdu 611731, P. R. ChinaResearch Center for Environmental and Energy CatalysisInstitute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731, P. R. China;

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defect density; electrochemical CO_2 reduction; flow cells; iodide derived copper; surface roughness;

Localized Geometry Determined Selectivity of Iodide-Derived Copper for Electrochemical CO_2 Reduction

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