Mesostructure-Induced Selectivity in CO2 Reduction Catalysis

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• 作者：Anthony Shoji Hall ; Youngmin Yoon ; Anna Wuttig ; Yogesh Surendranath
• 刊名：Journal of the American Chemical Society
• 出版年：2015
• 出版时间：December 2, 2015
• 年：2015
• 卷：137
• 期：47
• 页码：14834-14837
• 全文大小：288K
• ISSN：1520-5126

文摘

Gold inverse opal (Au-IO) thin films are active for CO₂ reduction to CO with high efficiency at modest overpotentials and high selectivity relative to hydrogen evolution. The specific activity for hydrogen evolution diminishes by 10-fold with increasing porous film thickness, while CO evolution activity is largely unchanged. We demonstrate that the origin of hydrogen suppression in Au-IO films stems from the generation of diffusional gradients within the pores of the mesostructured electrode rather than changes in surface faceting or Au grain size. For electrodes with optimal mesoporosity, 99% selectivity for CO evolution can be obtained at overpotentials as low as 0.4 V. These results establish electrode mesostructuring as a complementary method for tuning selectivity in CO₂-to-fuels catalysis.