期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 27, 页码 24140-24153出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b06789
关键词
cobalt phosphide; porous organic polymer; vanillin; hydrodeoxygenation (HDO); biofuel; ATR-IR
资金
- Council of Scientific and Industrial Research (CSIR), New Delhi
- IICT-RMIT PhD Program
- Department of Science and Technology, India [GAP-0522]
- IISc Bangalore
- ICTP Trieste
Hydrodeoxygenation (HDO) is a promising route for the upgrading of bio-oils to eco-friendly biofuel produced from lignocellulose. Herein, we report the sequential synthesis of a hybrid nanocatalyst CoxP@POP, where substoichiometric CoxP nanoparticles are distributed in a porous organic polymer (POP) via solid-state phosphidation of the Co3O4@POP nanohybrid system. We also explored the catalytic activity of the above two nanohybrids toward the HDO of vanillin, a typical compound of lignin-derived bio-oil to 2-methoxy-4-methylphenol, which is a promising future biofuel. The CoxP@POP exhibited superior catalytic activity and selectivity toward desired product with improved stability compared to the Co3O4@POP. Based on advanced sample characterization results, the extraordinary selectivity of CoxP@POP is attributed to the strong interaction of the cation of the CoxP nanoparticle with the POP matrix and the consequent modifications of the electronic states. Through attenuated total reflectance-infrared spectroscopy, we have also observed different interaction strengths between vanillin and the two catalysts. The decreased catalytic activity of Co3O4@POP compared to CoxP@POP catalyst could be attributed to the stronger adsorption of vanillin over the Co3O4@POP catalyst. Also from kinetic investigation, it is clearly demonstrated that the Co3O4@POP has higher activation energy barrier than the CoxP@POP, which also reflects to the reduction of the overall efficiency of the Co3O4@POP catalyst. To the best of our knowledge, this is the first approach in POP-encapsulated cobalt phosphide catalyst synthesis and comprehensive study in establishing the structure-activity relationship in significant step-forwarding in promoting biomass refining.
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