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Design of Pd{111}-TiO_2 interface for enhanced catalytic efficiency towards formic acid decomposition

Science China Chemistry 2018年第9期61卷 1123-1127页

作者： Yang You Hao Huang Song Xia Zijian Cai panyiming liu Chengming Wang Ran Long Li Song Yujie Xiong Hefei National Laboratory for Physical Sciences at the Microscale Collaborative Innovation Center of Chemistry for Energy MaterialsSchool of Chemistry and Materials Science and National Synchrotron Radiation Laboratory University of Science and Technology of China

Supports are commonly implemented in the industrial application of heterogeneous catalysts to improve the stability and recyclability of *** supported catalysts often show the enhanced activity and selectivity in various catalytic ***,the specific contributions of electronic and steric effects to a catalytic system often remain elusive due to the lack of well-defined model *** this work,two types of uniform Pd nanocrystals covered by{111}facets in tetrahedral and octahedral shapes,respectively,are synthesized with identical chemical environment and loaded on Ti O_2supports to form hybrid structures(Pd{111}-Ti O_2)towards the application of formic acid *** observation suggests that the polarization effect at the interface of Pd-Ti O_2enhances its activity in formic acid ***,the Pd tetrahedrons-Ti O_2hybrid structure whose Pd{111}-Ti O_2interface possesses a larger angle shows higher catalytic activity,owing to the reduced steric effect as compared to Pd octahedrons-Ti O_*** study reveals the nature of interface effects in formic acid decomposition,and provides a guidance for the related catalyst design.

关键词： palladium facet formic acid decomposition interface

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Tandem nanocatalyst design: putting two step-reaction sites into one location towards enhanced hydrogen transfer reactions

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Science China Materials 2019年第9期62卷 1297-1305页

作者： Yang You Hao Huang Keke Mao Song Xia Di Wu Canyu Hu Chao Gao panyiming liu Ran Long Xiaojun Wu Yujie Xiong Hefei National Laboratory for Physical Sciences at the Microscale Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) School of Chemistry and Materials Science and National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230026 China School of Energy and Environment Science Anhui University of Technology Maanshan 243032 China

Efficient tandem reactions on a single catalytic nanostructure would be beneficial to improving chemical transformation efficiency and reducing safety implications. It is imperative to identify the active sites for each single step reaction so that the entire reaction process can be optimized by designing and integrating the sites. Herein, hydrogen transfer reaction is taken as a proof-of-concept demonstration to show that the spatial integration of active sites is important to the catalytic efficiency of the entire process in tandem reactions. We identified specific active sites (i.e., various sites at faces versus corners and edges) for formic acid decomposition and alkene/nitrobenzene hydrogenation-the two steps in hydrogen transfer reactions, by employing three different shapes of Pd nanocrystals in tunable sizes. The investigation reveals that the decomposition of formic acid occurs preferentially at the edge sites of cubic nanocrystal and the plane sites of octahedral/ tetrahedral nanocrystals, while the hydrogenation takes place mainly at the edge sites of both cubic and octahedral/ tetrahedral nanocrystals. The consistency of active edge sites during different step reactions enables cubic nanocrystals to exhibit a higher activity than octahedral nanocrystals in hydrogen transfer reactions, although octahedrons offer comparable activities to cubes in formic acid decomposition and hydrogenation reactions. Guided by these findings, we further improved the overall performance of tandem catalysis by specifically promoting the limiting step through nanocatalyst design. This work provides insights into the rational design of heterogeneous nanocatalysts in tandem reactions.

关键词： hydrogen transfer reaction palladium tandem reaction reactive site hydrogenation

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