Mesokinetics as a Tool Bridging the Microscopic-to-Macroscopic Transition to Rationalize Catalyst Design

作者：Wenyao Chen, Gang Qian, Ying Wan, De Chen, Xinggui Zhou, Weikang Yuan, Xuezhi Duan · 发表于：Accounts of Chemical Research · 年份：2022 · DOI：10.1021/acs.accounts.2c00483 · 被引用次数：98 · 研究领域：Catalytic Processes in Materials Science、Electrocatalysts for Energy Conversion、Catalysis and Hydrodesulfurization Studies

Conspectus Heterogeneous catalysis is the workhorse of the chemical industry, and a heterogeneous catalyst possesses numerous active sites working together to drive the conversion of reactants to desirable products. Over the decades, much focus has been placed on identifying the factors affecting the active sites to gain deep insights into the structure-performance relationship, which in turn guides the design and preparation of more active, selective, and stable catalysts. However, the molecular-level interplay between active sites and catalytic function still remains qualitative or semiquantitative, ascribed to the difficulty and uncertainty in elucidating the nature of active sites for its controllable manipulation. Hence, bridging the microscopic properties of active sites and the macroscopic catalytic performance, that is, microscopic-to-macroscopic transition, to afford a quantitative description is intriguing yet challenging, and progress toward this promises to revolutionize catalyst design and preparation. In this Account, we propose mesokinetics modeling, for the first time enabling a quantitative description of active site characteristics and the related mechanistic information, as a versatile tool to guide rational catalyst design. Exemplified by a pseudo-zero-order reaction, the kinetics derivation from the Pt particle size-sensitive catalytic activity and size-insensitive activation energy suggests only one type of surface site as the dominant active site, in wh...