Reactant enrichment in hollow void of Pt NPs@MnOx nanoreactors for boosting hydrogenation performance  

作　　者：Yanfu Ma Liwei Wang Wantong Zhao Tianyi Liu Haitao Li Wenhao Luo Qike Jiang Wei Liu Qihua Yang Jun Huang Riguang Zhang Jian Liu GQMax Lu Can Li 

机构地区：[1]State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics(DICP),Chinese Academy of Sciences,Dalian116023,China [2]Center of Materials Science and Optoelectronics Engineering,University of Chinese Academy of Sciences,Beijing 100049,China [3]State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology.Taiyuan 030024,China [4]DICP-Surrey Joint Centre for Future Materials,Department of Chemical and Process Engineering,University of Surrey,GuildfordGU27XH,UK [5]CAS Key Laboratory of Science and Technology on Applied Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian116023,China [6]School of Chemistry and Chemical Engineering,Inner Mongolia University,Hohhot010021,China [7]Division of Energy Research Resources,Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academyof Sciences,Dalian116023,China [8]Key Laboratory of the Ministry of Education for Advanced Catalysis Materials,Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces,Institute of Physical Chemistry,Zhejiang Normal University,Jinhua321004,China [9]Laboratory for Catalysis Engineering,School of Chemical and Biomolecular Engineering,Sydney Nano Institute,The University of Sydney.Sydney 2006.Australia [10]University of Surrey,Guildford GU27XH,UK

出　　处：《National Science Review》2023年第10期109-117,共9页国家科学评论（英文版）

基　　金：supported by the National Natural Science Foundation of China(21905271 and 62227815);the China Postdoctoral Science Foundation(2021M703142);supported by the Shanghai Science and Technology Committee(19DZ2270100)。

摘　　要：In confined mesoscopic spaces,the unraveling of a catalytic mechanism with complex mass transfer and adsorption processes such as reactant enrichment is a great challenge.In this study,a hollow nanoarchitecture of MnOx-encapsulated Pt nanoparticles was designed as a nanoreactor to investigate the reactant enrichment in a mesoscopic hollow void.By employing advanced characterization techniques,we found that the reactant-enrichment behavior is derived from directional diffusion of the reactant driven through the local concentration gradient and this increased the amount of reactant.Combining experimental results with density functional theory calculations,the superior cinnamyl alcohol(COL)selectivity originates from the selective adsorption of cinnamaldehyde(CAL)and the rapid formation and desorption of COL in the MnOx shell.The superb performance of 95%CAL conversion and 95%COL selectivity is obtained at only 0.5 MPa H2 and 40 min.Our findings showcase that a rationally designed nanoreactor co uld boost catalytic performance in chemoselective hydrogenation,which can be of great aid and potential in various application scenarios.

关 键 词：reactant enrichment nanoreactor effect selective hydrogenation hollow nanostructure mesoporousmaterials 

分 类 号：TQ052[化学工程]