Journal
APPLIED SURFACE SCIENCE
Volume 425, Issue -, Pages 484-491Publisher
ELSEVIER
DOI: 10.1016/j.apsusc.2017.07.068
Keywords
N-doped carbon; ZIF-67; Polyvinylpyrrolidone; Dicyandiamide; Hydrogenation of phenol
Categories
Funding
- National Key Research and Development Plan [2016YFB0301503]
- Jiangsu Natural Science Foundation for Distinguished Young Scholars [BK20150044]
- National Natural Science Foundation [91534110]
- Jiangsu Province Natural Science Foundation [BK20160978]
- Foundation from State Key Laboratory of Materials-Oriented Chemical Engineering of China [ZK201402, ZK201407]
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Highly efficient Pd@CN catalysts for selective hydrogenation of phenol to cyclohexanone in water were successfully fabricated by loading Pd nanoparticles (NPs) in N-doped carbons (CN) derived from ZIF-67 with dicyandiamide (DICY) as the additional nitrogen source. For comparison, polyvinylpyrrolidone (PVP) was also used as the additional nitrogen source during the ZIF-67 synthesis. The results showed that the PVP and DICY had significantly different impacts on the microstructures of as-obtained CN materials and the catalytic performance of Pd@CN catalysts in the phenol hydrogenation. The addition of DICY had the positive promotion effect on the surface area of the obtained CN materials. Moreover, the introduction of DICY could increase the nitrogen content of CN and then prevent the re-oxidation of Pd NPs during air contact, resulting in higher Pd-0 ratio. In comparison with PVP, the DICY was more suitable as the additional nitrogen source for the formation of CN and Pd@CN (Pd@CND, Pd@CNP). The Pd@CND exhibited superior catalytic activity as compared to Pd@CNP (phenol conversion 96.9% vs. 67.4%). More importantly, the as-prepared Pd@CND catalyst could be reused for four times without catalytic performance reduction. The work would aid the development of Pd@CN catalysts with superior catalytic properties. (C) 2017 Elsevier B.V. All rights reserved.
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