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Evaluation of the collaboration between intrinsic activity and diffusion: a descriptor for alkene epoxidation
1Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials, Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM), Fudan University Shanghai 200433 P. R. China zhangyh@fudan.edu.cn yitang@fudan.edu.cn.
Abstract:
The systemic evaluation of the collaboration between intrinsic activity of active sites and the substrate/product diffusion rate is a key challenge for rational optimization of reaction performance in alkene epoxidation. Herein, we constructed a series of TS-1 catalysts with adjustable local microenvironments around active sites to explore their performance in alkene epoxidation. This was achieved by controlling the contributions of classical and non-classical routines during the crystallization process. Based on the characterization of active sites, product diffusion and their alkene epoxidation activity, we proposed a descriptor, R a/d, for quantitative evaluation of the collaboration between intrinsic activity and product diffusion in TS-1 catalysts. This descriptor successfully explains the catalytic performance of various TS-1 catalysts including commercial TS-1 and guides further improvement of TS-1 in different alkene epoxidations. The optimal R a/d is found in various epoxidations, corresponding to peak epoxidation performance across different substrates due to the well-balanced intrinsic activity and diffusion rate.
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