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

Author:

Ma Yanfu1,Wang Liwei12,Zhao Wantong3,Liu Tianyi14,Li Haitao1,Luo Wenhao56ORCID,Jiang Qike7,Liu Wei7ORCID,Yang Qihua8,Huang Jun9ORCID,Zhang Riguang3,Liu Jian1246ORCID,Lu G Q Max10,Li Can1

Affiliation:

1. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics (DICP), Chinese Academy of Sciences , Dalian 116023 , 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 , Guildford GU2 7XH , UK

5. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023 , China

6. School of Chemistry and Chemical Engineering, Inner Mongolia University , Hohhot 010021 , China

7. Division of Energy Research Resources, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023 , 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 , Jinhua 321004 , 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 GU2 7XH , UK

Abstract

ABSTRACT 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 could boost catalytic performance in chemoselective hydrogenation, which can be of great aid and potential in various application scenarios.

Funder

National Natural Science Foundation of China

China Postdoctoral Science Foundation

Shanghai Science and Technology Committee

Publisher

Oxford University Press (OUP)

Subject

Multidisciplinary

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