文献类型：期刊文献

英文题名：Self-Etherification of 5-Hydroxymethylfurfural to 5,5′(Oxy-bis(methylene))bis-2-furfural over Hierarchically Micromesoporous ZSM-5: The Role of Br?nsted- and Lewis-Acid Sites

作者：Yang, Jie[1]; Huai, Liyuan[1]; Gan, Jiang[1,2]; Hu, Hualei[1]; Zhou, Shenghu[3]; Zhang, Jian[1,2]

机构：[1] Ningbo Institute of Materials Technology & Engineering Chinese Academy of Sciences, 1219 Zhongguan West Road, Ningbo, 315201, China; [2] University of Chinese Academy of Sciences, Beijing, 100049, China; [3] Shanghai Key Laboratory of Multiphase Materials Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China

年份：2022

卷号：61

期号：1

起止页码：987

外文期刊名：Industrial and Engineering Chemistry Research

收录：EI(收录号：20220111417129)

语种：英文

外文关键词：Aldehydes - Activation energy - Catalyst selectivity - Furfural - Catalyst activity - Density functional theory

摘要：The 5,5′(oxy-bis(methylene))bis-2-furfural (OBMF) formation from the 5-hydroxymethylfurfural (HMF) self-etherification over zeolites is an important reaction for the synthesis of value-added chemicals from biomass resources. However, there is still a lack of knowledge about the reaction mechanism and the roles of different acid sites that impedes the exploitation of zeolite catalysts for efficient OBMF production. In the present study, the ZSM-5 (HPZ) catalysts of four hierarchically micromesopores were successfully synthesized in different Si/Al ratios by adjusting the amount of Al in the solvent evaporation with the assistance of a dry gel conversion method. The kinetics of OBMF formation from HMF self-etherification was investigated. The apparent activation energy and the conversion reaction order were calculated to be 104.6 kJ/mol and 0.65, respectively. The intrinsic activity comparison of four catalysts and density functional theory (DFT) calculations showed that HMF adsorption and etherification benefit from Br?nsted-acid sites. Besides, the DFT results suggested that the etherification proceeds via a concerted step, instead of the sequential pathways, thus leading to the high selectivity of OBMF on hierarchically micromesoporous ZSM-5 (HPZ) catalysts. ? 2021 American Chemical Society