Nature Communications, 2014; 5: 4948.
Dohyung Kim, Joaquin Resasco, Yi Yu, Abdullah Mohamed Asiri, Peidong Yang.
Department of Materials Science and Engineering, University of California, Berkeley, California 94720, USA &
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California 94720, USA &
Department of Chemistry, University of California, Berkeley, California 94720, USA &
Center of Excellence for Advanced Materials Research (CEAMR), King Abdulaziz University, P.O. Box 80203, Jeddah 21589, Saudi Arabia &
Kavli Energy Nanosciences Institute, Berkeley, California 94720, USA.
Highly efficient and selective electrochemical reduction of carbon dioxide represents one of the biggest scientific challenges in artificial photosynthesis, where carbon dioxide and water are converted into chemical fuels from solar energy. However, our fundamental understanding of the reaction is still limited and we do not have the capability to design an outstanding catalyst with great activity and selectivity a priori. Here we assemble uniform gold–copper bimetallic nanoparticles with different compositions into ordered monolayers, which serve as a well-defined platform to understand their fundamental catalytic activity in carbon dioxide reduction. We find that two important factors related to intermediate binding, the electronic effect and the geometric effect, dictate the activity of gold–copper bimetallic nanoparticles. These nanoparticle monolayers also show great mass activities, outperforming conventional carbon dioxide reduction catalysts. The insights gained through this study may serve as a foundation for designing better carbon dioxide electrochemical reduction catalysts.
The Authors discovered that geometric and electronic effects synergistically played an important role in carbon dioxide reduction reaction. They control the binding strength of the reaction intermediates, which influences the efficiency and selectivity of the catalyst in the reduction process. They assembled gold–copper bimetallic nanoparticles with varying compositions into ordered monolayers, which enabled better analysis of the catalytic activity in reduction reaction. The results observed in the study could hold good for other catalysts in achieving exceptional advancements in electrochemical carbon dioxide reduction.