Herzog Antonia, Bergmann Arno, Jeon Hyo Sang, Timoshenko Janis, Kühl Stefanie, Rettenmaier Clara, Lopez Luna Mauricio, Haase Felix T, Roldan Cuenya Beatriz
Department of Interface Science, Fritz-Haber Institute of the Max-Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.
Angew Chem Int Ed Engl. 2021 Mar 22;60(13):7426-7435. doi: 10.1002/anie.202017070. Epub 2021 Feb 22.
Direct conversion of carbon dioxide into multicarbon liquid fuels by the CO electrochemical reduction reaction (CO RR) can contribute to the decarbonization of the global economy. Here, well-defined Cu O nanocubes (NCs, 35 nm) uniformly covered with Ag nanoparticles (5 nm) were synthesized. When compared to bare Cu O NCs, the catalyst with 5 at % Ag on Cu O NCs displayed a two-fold increase in the Faradaic efficiency for C liquid products (30 % at -1.0 V ), including ethanol, 1-propanol, and acetaldehyde, while formate and hydrogen were suppressed. Operando X-ray absorption spectroscopy revealed the partial reduction of Cu O during CO RR, accompanied by a reaction-driven redispersion of Ag on the CuO 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 CO RR that appear crucial for the C-C coupling and the enhanced yield of liquid products.
通过二氧化碳电化学还原反应(CO₂RR)将二氧化碳直接转化为多碳液体燃料有助于全球经济脱碳。在此,合成了均匀覆盖有银纳米颗粒(5 nm)的明确的氧化铜纳米立方体(NCs,35 nm)。与裸露的氧化铜NCs相比,在氧化铜NCs上含有5原子百分比银的催化剂对C₂液体产物(在-1.0 V时为30%)的法拉第效率提高了两倍,这些产物包括乙醇、1-丙醇和乙醛,同时甲酸盐和氢气受到抑制。原位X射线吸收光谱显示在CO₂RR过程中氧化铜发生了部分还原,同时银在氧化铜NCs上发生了反应驱动的再分散。原位表面增强拉曼光谱数据进一步揭示了CO与铜结合的显著变化,这归因于CO₂RR过程中形成的Ag-Cu位点,这些位点似乎对C-C偶联和液体产物产量的提高至关重要。