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Operando Investigation of Ag‐Decorated Cu2O Nanocube Catalysts with Enhanced CO2 Electroreduction toward Liquid Products
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-01-26 , DOI: 10.1002/anie.202017070
Antonia Herzog 1 , Arno Bergmann 1 , Hyo Sang Jeon 1 , Janis Timoshenko 1 , Stefanie Kühl 1 , Clara Rettenmaier 1 , Mauricio Lopez Luna 1 , Felix T Haase 1 , Beatriz Roldan Cuenya 1
Affiliation  

Direct conversion of carbon dioxide into multicarbon liquid fuels by the CO2 electrochemical reduction reaction (CO2RR) can contribute to the decarbonization of the global economy. Here, well‐defined Cu2O nanocubes (NCs, 35 nm) uniformly covered with Ag nanoparticles (5 nm) were synthesized. When compared to bare Cu2O NCs, the catalyst with 5 at % Ag on Cu2O NCs displayed a two‐fold increase in the Faradaic efficiency for C2+ liquid products (30 % at −1.0 VRHE), including ethanol, 1‐propanol, and acetaldehyde, while formate and hydrogen were suppressed. Operando X‐ray absorption spectroscopy revealed the partial reduction of Cu2O during CO2RR, accompanied by a reaction‐driven redispersion of Ag on the CuOx NCs. Data from operando surface‐enhanced Raman spectroscopy further uncovered significant variations in the CO binding to Cu, which were assigned to Ag−Cu sites formed during CO2RR that appear crucial for the C−C coupling and the enhanced yield of liquid products.

中文翻译:


Ag 修饰的 Cu2O 纳米立方体催化剂增强 CO2 电还原液体产物的操作研究



通过CO 2电化学还原反应(CO 2 RR)将二氧化碳直接转化为多碳液体燃料可以促进全球经济的脱碳。在这里,合成了均匀覆盖有银纳米颗粒(5 nm)的清晰的 Cu 2 O 纳米立方体(NC,35 nm)。与裸露的 Cu 2 O NC 相比,Cu 2 O NC 上含有 5 at% Ag 的催化剂显示 C 2+液体产物的法拉第效率增加了一倍(-1.0 V RHE时为 30%),包括乙醇、 1-丙醇和乙醛,而甲酸盐和氢被抑制。原位X射线吸收光谱揭示了CO 2 RR过程中Cu 2 O的部分还原,并伴随着反应驱动的Ag在CuO x NC上的再分散。原位表面增强拉曼光谱的数据进一步揭示了 CO 与 Cu 结合的显着变化,这些变化被分配给 CO 2 RR 过程中形成的 Ag−Cu 位点,这对于 C−C 耦合和提高液体产物的产率至关重要。
更新日期:2021-03-17
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