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Tuning of Silver Catalyst Mesostructure Promotes Selective Carbon Dioxide Conversion into Fuels
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2016-11-10 , DOI: 10.1002/anie.201607942 Youngmin Yoon 1 , Anthony Shoji Hall 1, 2 , Yogesh Surendranath 1
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2016-11-10 , DOI: 10.1002/anie.201607942 Youngmin Yoon 1 , Anthony Shoji Hall 1, 2 , Yogesh Surendranath 1
Affiliation
An electrode's performance for catalytic CO2 conversion to fuels is a complex convolution of surface structure and transport effects. Using well‐defined mesostructured silver inverse opal (Ag‐IO) electrodes, it is demonstrated that mesostructure‐induced transport limitations alone serve to increase the turnover frequency for CO2 activation per unit area, while simultaneously improving reaction selectivity. The specific activity for catalyzed CO evolution systematically rises by three‐fold and the specific activity for catalyzed H2 evolution systematically declines by ten‐fold with increasing mesostructural roughness of Ag‐IOs. By exploiting the compounding influence of both of these effects, we demonstrate that mesostructure, rather than surface structure, can be used to tune CO evolution selectivity from less than 5 % to more than 80 %. These results establish electrode mesostructuring as a powerful complementary tool for tuning both catalyst selectivity and efficiency for CO2 conversion into fuels.
中文翻译:
银催化剂介观结构的调整促进选择性二氧化碳转化为燃料
电极将CO 2催化转化为燃料的性能是表面结构和传输效应的复杂综合。通过使用定义明确的介孔结构银反蛋白石(Ag-IO)电极,证明了介孔结构引起的输运限制本身可以增加单位面积CO 2活化的周转频率,同时提高反应选择性。催化的CO逸出的比活性系统地提高了三倍,催化的H 2的比活性随着AgIOs的细观结构粗糙度的增加,其演化系统地下降了十倍。通过利用这两种影响的复合影响,我们证明了介观结构而不是表面结构可用于将CO生成选择性从不到5%调整到超过80%。这些结果确立了电极介孔结构作为调节催化剂选择性和CO 2转化成燃料的效率的有力补充工具。
更新日期:2016-11-10
中文翻译:
银催化剂介观结构的调整促进选择性二氧化碳转化为燃料
电极将CO 2催化转化为燃料的性能是表面结构和传输效应的复杂综合。通过使用定义明确的介孔结构银反蛋白石(Ag-IO)电极,证明了介孔结构引起的输运限制本身可以增加单位面积CO 2活化的周转频率,同时提高反应选择性。催化的CO逸出的比活性系统地提高了三倍,催化的H 2的比活性随着AgIOs的细观结构粗糙度的增加,其演化系统地下降了十倍。通过利用这两种影响的复合影响,我们证明了介观结构而不是表面结构可用于将CO生成选择性从不到5%调整到超过80%。这些结果确立了电极介孔结构作为调节催化剂选择性和CO 2转化成燃料的效率的有力补充工具。