Efficient aerobic oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran on manganese oxide catalysts

doi:10.1016/j.jcat.2014.05.003

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	Efficient aerobic oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran on manganese oxide catalysts
	Nie, Junfang; Liu, Haichao
刊名	JOURNAL OF CATALYSIS
	2014-07-01
卷号	316 页码:57-66
关键词	Biomass 5-hydroxymethylfurfural Aerobic Oxidation Manganese Oxide Reaction Mechanism 2 5-diformylfuran
ISSN号	0021-9517
DOI	10.1016/j.jcat.2014.05.003
英文摘要	A cryptomelane-type manganese oxide octahedral molecular sieve with a (2 x 2, 4.6 angstrom x 4.6 angstrom) tunnel size (OMS-2) efficiently catalyzed aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) with a high yield of 97.2% at 383 K and 0.5 MPa O-2 in N,N-dimethylformamide. OMS-2 was superior to other MnO2 catalysts with different morphologies, including OMS-1, OMS-6, and OMS-7 with various tunnel sizes, amorphous MnO2 and bimessite-type MnO2, apparently due to its (2 x 2) tunnel structure and consequently high reducibility and oxidizability. Kinetic and isotopic studies on OMS-2 showed near half-order dependence of the activities on HMF and O-2 concentrations and marked kinetic isotope effects for deuterated HMF at its methylene group. These results, together with the similar initial rates under aerobic and anaerobic conditions, suggest that HMF oxidation to DFF on OMS-2 proceeds via a redox mechanism involving kinetically-relevant steps of C-H bond cleavage in adsorbed alcoholate intermediate, derived from quasi-equilibrated dissociation of HMF, using lattice oxygen and reoxidation of Mn3+ to Mn4+ by dissociative chemisorption of O-2. (C) 2014 Elsevier Inc. All rights reserved.
语种	英语
出版者	ACADEMIC PRESS INC ELSEVIER SCIENCE
WOS记录号	WOS:000340853800006
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/53111]
专题	中国科学院化学研究所
通讯作者	Liu, Haichao
作者单位	Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, State Key Lab Struct Chem Stable & Unstable Speci, Beijing 100871, Peoples R China
推荐引用方式 GB/T 7714	Nie, Junfang,Liu, Haichao. Efficient aerobic oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran on manganese oxide catalysts[J]. JOURNAL OF CATALYSIS,2014,316:57-66.
APA	Nie, Junfang,&Liu, Haichao.(2014).Efficient aerobic oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran on manganese oxide catalysts.JOURNAL OF CATALYSIS,316,57-66.
MLA	Nie, Junfang,et al."Efficient aerobic oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran on manganese oxide catalysts".JOURNAL OF CATALYSIS 316(2014):57-66.