期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 42, 页码 18374-18379出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202007297
关键词
heterogeneous catalysis; hollow nanoreactors; hydrogenation; shape-selective catalysis; void-confinement effects
资金
- National Natural Science Foundation of China [21872159]
- QIBEBT [QIBEBT ZZBS201802]
- DNL Cooperation Fund, CAS [DNL180402]
Nanoreactors with hollow structures have attracted great interest in catalysis research due to their void-confinement effects. However, the challenge in unambiguously unraveling these confinement effects is to decouple them from other factors affecting catalysis. Here, we synthesize a pair of hollow carbon sphere (HCS) nanoreactors with presynthesized PdCu nanoparticles encapsulated inside of HCS (PdCu@HCS) and supported outside of HCS (PdCu/HCS), respectively, while keeping other structural features the same. Based on the two comparative nanoreactors, void-confinement effects in liquid-phase hydrogenation are investigated in a two-chamber reactor. It is found that hydrogenations over PdCu@HCS are shape-selective catalysis, can be accelerated (accumulation of reactants), decelerated (mass transfer limitation), and even inhibited (molecular-sieving effect); conversion of the intermediate in the void space can be further promoted. Using this principle, a specific imine is selectively produced. This work provides a proof of concept for fundamental catalytic action of the hollow nanoreactors.
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