Tuning Catalytic Selectivity at the Mesoscale via Interparticle Interactions

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• 作者：Hemma Mistry ; Farzad Behafarid ; Rulle Reske ; Ana Sofia Varela ; Peter Strasser ; Beatriz Roldan Cuenya
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：February 5, 2016
• 年：2016
• 卷：6
• 期：2
• 页码：1075-1080
• 全文大小：417K
• ISSN：2155-5435

文摘

The selectivity of heterogeneously catalyzed chemical reactions is well-known to be dependent on nanoscale determinants, such as surface atomic geometry and composition. However, principles to control the selectivity of nanoparticle (NP) catalysts by means of mesoscopic descriptors, such as the interparticle distance, have remained largely unexplored. We used well-defined copper catalysts to deconvolute the effect of NP size and distance on product selectivity during CO₂ electroreduction. Corroborated by reaction-diffusion modeling, our results reveal that mesoscale phenomena such as interparticle reactant diffusion and readsorption of intermediates play a defining role in product selectivity. More importantly, this study uncovers general principles of tailoring NP activity and selectivity by carefully engineering size and distance. These principles provide guidance for the rational design of mesoscopic catalyst architectures in order to enhance the production of desired reaction products.