Aqueous CO 2 Reduction at Very Low Overpotential on Oxide-Derived Au Nanoparticles

作者：Yihong Chen, Christina Li, Matthew W. Kanan · 发表于：Journal of the American Chemical Society · 年份：2012 · DOI：10.1021/ja309317u · 被引用次数：1664 · 研究领域：CO2 Reduction Techniques and Catalysts、Catalytic Processes in Materials Science、Electrocatalysts for Energy Conversion

Carbon dioxide reduction is an essential component of many prospective technologies for the renewable synthesis of carbon-containing fuels. Known catalysts for this reaction generally suffer from low energetic efficiency, poor product selectivity, and rapid deactivation. We show that the reduction of thick Au oxide films results in the formation of Au nanoparticles ("oxide-derived Au") that exhibit highly selective CO(2) reduction to CO in water at overpotentials as low as 140 mV and retain their activity for at least 8 h. Under identical conditions, polycrystalline Au electrodes and several other nanostructured Au electrodes prepared via alternative methods require at least 200 mV of additional overpotential to attain comparable CO(2) reduction activity and rapidly lose their activity. Electrokinetic studies indicate that the improved catalysis is linked to dramatically increased stabilization of the CO(2)(•-) intermediate on the surfaces of the oxide-derived Au electrodes.