期刊
JOURNAL OF CATALYSIS
卷 397, 期 -, 页码 148-155出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2021.03.031
关键词
Biomass-derived alcohols; Oxidative esterification; Heterogeneous cobalt catalysts; Base-free reaction; Sustainability
资金
- National Natural Science Foundation of China [21978248, 21922513]
- Natural Science Foundation of Fujian Province of China [2019J06005]
The development of active and environmentally friendly non-noble nano-catalysts for transforming biomass-derived platform into value chemicals is highly desired. A low-cost and sustainable cobalt/nitrogen-doped carbon catalyst has been reported to exhibit satisfying activity for the oxidative esterification of various alcohols, with excellent stability and recyclability. The Co/Co-N group synergistically promotes electron transfer, facilitates O-2 adsorption and activation, and reduces energy barrier for oxidation of alcohols to aldehydes, contributing to the overall activity of oxidative esterification.
Developing the active and environmentally friendly non-noble nano-catalysts is highly desired to transform biomass-derived platform into value chemicals. Herein, we report a low-cost and sustainable cobalt/nitrogen-doped carbon catalyst containing both metallic Co and Co-N components exhibits satisfying activity for the oxidative esterification of 5-hydroxymethylfurfural and other investigated alcohols in methanol without the base additive under mild conditions. Experimental results show that an appropriate ratio of Co to Co-N is responsible for the high activity of the Co/Co-N/CN catalysts towards oxidative esterification. Theoretical computational results demonstrate that the Co/Co-N group synergistically promotes electron transfer from the Co adatom to the surface oxygen atoms, facilitates O-2 adsorption and activation on the Co sites, and further reduces the energy barrier for the oxidation of alcohols to aldehydes, all of which contribute to the overall activity of oxidative esterification of alcohols to the corresponding esters. In addition to exhibiting superior intrinsic activity, the as-prepared Co/Co-N/CN catalyst also shows excellent stability and recyclability. (C) 2021 Elsevier Inc. All rights reserved.
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