解析 Ag-Cu 双金属表面合金对电化学 CO 还原的可控产物选择性。
Decrypting the Controlled Product Selectivity over Ag-Cu Bimetallic Surface Alloys for Electrochemical CO Reduction.
机构信息
International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, 710049, China.
Department of Physics, Tamkang University, New Taipei City, 25137, Taiwan.
出版信息
Angew Chem Int Ed Engl. 2023 May 2;62(19):e202217369. doi: 10.1002/anie.202217369. Epub 2023 Mar 30.
Electrochemical CO reduction reaction (ECO RR) with controlled product selectivity is realized on Ag-Cu bimetallic surface alloys, with high selectivity towards C2 hydrocarbons/alcohols (≈60 % faradaic efficiency, FE), C1 hydrocarbons/alcohols (≈41 % FE) and CO (≈74 % FE) achieved by tuning surface compositions and applied potentials. In situ spectral investigations and theoretical calculations reveal that surface-composition-dependent d-band center could tune *CO binding strengths, regulating the *CO subsequent reaction pathways and then the product selectivity. Further adjusting the applied potentials will alter the energy of participated electrons, which leads to controlled ECO RR selectivity towards desired products. A predominant region map, with an indicator proposed to evaluate the thermodynamic predominance of the *CO subsequent reactions, is then provided as a reliable theoretical guidance for the controllable ECO RR product selectivity over bimetallic alloys.
在 Ag-Cu 双金属表面合金上实现了电化学 CO 还原反应 (ECO RR)，具有可控的产物选择性，对 C2 烃/醇（≈60%的法拉第效率，FE）、C1 烃/醇（≈41%的 FE）和 CO（≈74%的 FE）具有高选择性，通过调整表面组成和施加的电势来实现。原位光谱研究和理论计算表明，表面组成依赖性 d 带中心可以调节CO 结合强度，调节CO 后续反应途径，从而调节产物选择性。进一步调整施加的电势会改变参与电子的能量，从而控制 ECO RR 对所需产物的选择性。然后提供一个主要区域图，并提出一个指标来评估*CO 后续反应的热力学优势，作为双金属合金可控 ECO RR 产物选择性的可靠理论指导。
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