Mesostructure-Induced Selectivity in CO2 Reduction Catalysis

被引:451
作者
Hall, Anthony Shoji [1 ]
Yoon, Youngmin [1 ]
Wuttig, Anna [1 ]
Surendranath, Yogesh [1 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
基金
美国国家科学基金会;
关键词
CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; COPPER; ELECTROREDUCTION; DEPOSITION; CONVERSION;
D O I
10.1021/jacs.5b08259
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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.
引用
收藏
页码:14834 / 14837
页数:4
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