Citation: Na Huo, Hong Ma, Xinhong Wang, Tianlong Wang, Gang Wang, Ting Wang, Leilei Hou, Jin Gao, Jie Xu. High-efficiency oxidative esterification of furfural to methylfuroate with a non-precious metal Co-N-C/MgO catalyst[J]. Chinese Journal of Catalysis, ;2017, 38(7): 1148-1154. doi: 10.1016/S1872-2067(17)62841-9 shu

High-efficiency oxidative esterification of furfural to methylfuroate with a non-precious metal Co-N-C/MgO catalyst

Na Huo ^a,b, ,
Hong Ma ^b ,
Xinhong Wang ^a ,
Tianlong Wang ^a,b ,
Gang Wang ^a,b ,
Ting Wang ^a,b ,
Leilei Hou ^a,b ,
Jin Gao ^b ,
Jie Xu ^b

a School of Textile and Material Engineering, Dalian Polytechnic University, Dalian 116034, Liaoning, China;
b State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, Dalian 116023, Liaoning, China

Received Date: 7 March 2017
Revised Date: 15 April 2017

Fund Project: This work was supported by the National Natural Science Foundation of China (21233008, 21643013, 21690084), the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020300), and the Youth Innovation Promotion Association CAS (2013121).

From both fundamental and practical perspectives, the production of chemicals from biomass re-sources using high-efficiency non-precious metal catalysts is important. However, many processes require addition of stoichiometric or excess quantities of base, which leads to high energy consump-tion, leaching problems, and side reactions. In this study, we investigated the high-efficiency oxida-tive esterification of furfural to methylfuroate by molecular oxygen with a Co-N-C/MgO catalyst. The catalyst was prepared by direct pyrolysis of a cobalt(Ⅱ) phenanthroline complex on MgO at 800℃ under N₂ atmosphere. From furfural, 93.0% conversion and 98.5% selectivity toward methylfuroate were achieved under 0.5 MPa O₂ with reaction at 100℃ for 12 h without a basic additive. The con-version and selectivity were much higher than those obtained with cobalt catalysts produced by pyrolysis of a cobalt(Ⅱ) phenanthroline complex on activated carbon or typical basic supports, in-cluding NaX, NaY, and CaO. X-ray photoelectron spectroscopy, X-ray diffraction, transmission elec-tron microscopy, and experimental results revealed that the high efficiency of Co-N-C/MgO for pro-duction of methylfuroate was closely related to the cobalt-nitrogen-doped carbon species and its catalytic ability in hydrogen abstraction. In contrast, Co-N-C(HCl) that synthesized by removing MgO with HCl from Co-N-C/MgO, as the catalyst produced mainly an acetal as a condensation prod-uct, and chloride ions had a negative effect on the oxidative esterification. Although the catalytic performance of the cobalt-nitrogen-doped carbon species was greatly affected by HCl treatment, it could be recovered to a great extent by addition of MgO. Moreover, changes in the oxygen pressure hardly affected the oxidative esterification of furfural with Co-N-C/MgO. This study not only pro-vides an effective approach to prepare methylfuroate, but also for designing high-performance non-precious metal catalysts for the oxidative esterification of biomass-derived compounds.
- Catalysis,
- Cobalt-nitrogen-doped carbon,
- Furfural,
- Methylfuroate,
- MgO,
- Oxidative esterification
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