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Design of Hollow Nanoreactors for Size- and Shape-Selective Catalytic Semihydrogenation Driven by Molecular Recognition |
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| Authors: | Yutong Pi Linxia Cui Prof Wenhao Luo Dr Haitao Li Dr Yanfu Ma Dr Na Ta Xinyao Wang Prof Rui Gao Prof Dan Wang Prof Qihua Yang Prof Jian Liu |
| Institution: | 1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, 116023 Dalian, China
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, 100049 Beijing, China These authors contributed equally to this work.;2. School of Chemistry and Chemical Engineering, Inner Mongolia University, 235 West University Street, 010021 Hohhot, China These authors contributed equally to this work.;3. School of Chemistry and Chemical Engineering, Inner Mongolia University, 235 West University Street, 010021 Hohhot, China;4. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, 116023 Dalian, China;5. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, 116023 Dalian, China Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, 100049 Beijing, China;6. State Key Laboratory of Biochemical Engineering, Key Laboratory of Science and Technology on Particle Materials, Institute of Process Engineering, Chinese Academy of Sciences, 100190 Beijing, China;7. 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, 321004 Jinhua, China |
| Abstract: | Mimicking the structures and functions of cells to create artificial organelles has spurred the development of efficient strategies for production of hollow nanoreactors with biomimetic catalytic functions. However, such structure are challenging to fabricate and are thus rarely reported. We report the design of hollow nanoreactors with hollow multishelled structure (HoMS) and spatially loaded metal nanoparticles. Starting from a molecular-level design strategy, well-defined hollow multishelled structure phenolic resins (HoMS-PR) and carbon (HoMS-C) submicron particles were accurately constructed. HoMS-C serves as an excellent, versatile platform, owing to its tunable properties with tailored functional sites for achieving precise spatial location of metal nanoparticles, internally encapsulated (Pd@HoMS-C) or externally supported (Pd/HoMS-C). Impressively, the combination of the delicate nanoarchitecture and spatially loaded metal nanoparticles endow the pair of nanoreactors with size–shape-selective molecular recognition properties in catalytic semihydrogenation, including high activity and selectivity of Pd@HoMS-C for small aliphatic substrates and Pd/HoMS-C for large aromatic substrates. Theoretical calculations provide insight into the pair of nanoreactors with distinct behaviors due to the differences in energy barrier of substrate adsorption. This work provides guidance on the rational design and accurate construction of hollow nanoreactors with precisely located active sites and a finely modulated microenvironment by mimicking the functions of cells. |
| Keywords: | Hollow Structure Hydrogenation Nanoreactor Polymer Supported Catalyst |