Yang Yisen, Zhang Jianling, Tan Zhonghao, Yang Jie, Wang Sha, Li Meiling, Su Zhuizhui
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P.R. China.
School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, P.R. China.
Angew Chem Int Ed Engl. 2024 Nov 18;63(47):e202408873. doi: 10.1002/anie.202408873. Epub 2024 Oct 17.
The acidic electrocatalytic conversion of CO to multi-carbon (C) oxygenates is of great importance in view of enhancing carbon utilization efficiency and generating products with high energy densities, but suffering from low selectivity and activity. Herein, we synthesized Ag-Cu alloy catalyst with highly rough surface, by which the selectivity to C oxygenates can be greatly improved. In a strongly acidic condition (pH=0.75), the maximum C products Faradaic efficiency (FE) and C oxygenates FE reach 80.4 % and 56.5 % at -1.9 V versus reversible hydrogen electrode, respectively, with a ratio of FE to FE up to 2.36. At this condition, the C oxygenates partial current density is as high as 480 mA cm. The in situ spectra, control experiments and theoretical calculations indicate that the high generation of C oxygenates over the catalyst originates from its large surface roughness and Ag alloying.
将CO酸性电催化转化为多碳（C）含氧化合物对于提高碳利用效率和生成具有高能量密度的产物具有重要意义，但存在选择性和活性较低的问题。在此，我们合成了具有高度粗糙表面的Ag-Cu合金催化剂，通过该催化剂可大大提高对C含氧化合物的选择性。在强酸性条件（pH = 0.75）下，相对于可逆氢电极，在-1.9 V时，最大C产物法拉第效率（FE）和C含氧化合物FE分别达到80.4%和56.5%，FE与FE的比率高达2.36。在此条件下，C含氧化合物的分电流密度高达480 mA cm。原位光谱、对照实验和理论计算表明，催化剂上C含氧化合物的高生成源于其大的表面粗糙度和Ag合金化。
