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Conversion of fructose into 5-hydroxymethylfurfural catalyzed by recyclable sulfonic acid-functionalized metal-organic frameworks
Chen, Jinzhu1; Li, Kegui1,3; Chen, Limin2; Liu, Ruliang1,3; Huang, Xing1,2; Ye, Daiqi2
2014
发表期刊GREEN CHEMISTRY
卷号16期号:5页码:2490-2499
摘要A series of sulfonic acid-functionalized metal-organic frameworks (MOF-SO3H) were prepared by postsynthetic modification (PSM) of the organic linkers within the MOF with chlorosulfonic acid. The obtained MOF-SO3H, including sulfonic acid-functionalized MIL-101(Cr) [MIL-101(Cr)-SO3H], UIO-66(Zr) [UIO-66(Zr)-SO3H], and MIL-53(Al) [MIL-53(Al)-SO3H], have been systematically studied as solid acids in fructose transformation to 5-hydroxymethylfurfural (HMF). With MIL-101(Cr)-SO3H as catalyst, a HMF yield of 90% with a full fructose conversion was obtained at 120 degrees C for 60 min in DMSO. The concentration of -SO3H in MOF-SO3H as well as the contribution of Bronsted acidity of MOF-SO3H parallels its -SO3H grafting rate. Under a lower -SO3H grafting level, a good linear correlation between catalytic activity, in terms of turnover frequency, and sulfonic acid-site density of MOF-SO3H was found. Moreover, the sulfonic acid groups, which function as the catalytic sites, are equivalent in all MOF-SO3H for fructose-to-HMF transformation, regardless of precursor MOFs. Both conversions of fructose and selectivities towards HMF increase with the sulfonic acid-site density of MOF-SO3H at an initial stage of fructose-to-HMF transformation. Kinetics studies reveal that the MIL-101(Cr)-SO3H promoted fructose-to-HMF transformation may follow pseudo-first-order kinetics with observed activation energy of 55 kJ mol(-1) under the investigated conditions. Moreover, MIL-101(Cr)-SO3H behaves as a heterogeneous catalyst and can be easily recovered and reused. The research highlights a good prospect for catalytic application of MOF-derived solid acid catalysts for biomass carbohydrate valorization.
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
DOI10.1039/c3gc42414f
研究领域[WOS]Chemistry
关键词[WOS]IONIC LIQUIDS ; DEHYDRATION ; BIOMASS ; FUELS ; CHEMICALS ; EFFICIENT ; CELLULOSE ; ENCAPSULATION ; KINETICS ; MIL-101
收录类别SCI
语种英语
WOS类目Chemistry, Multidisciplinary
WOS记录号WOS:000335005200018
引用统计
被引频次:101[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.giec.ac.cn/handle/344007/10751
专题中国科学院广州能源研究所
作者单位1.Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangzhou 510640, Guangdong, Peoples R China
2.S China Univ Technol, Coll Environm & Energy, Guangdong Prov Key Lab Atmospher Environm & Pollu, Guangzhou 510006, Guangdong, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
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GB/T 7714
Chen, Jinzhu,Li, Kegui,Chen, Limin,et al. Conversion of fructose into 5-hydroxymethylfurfural catalyzed by recyclable sulfonic acid-functionalized metal-organic frameworks[J]. GREEN CHEMISTRY,2014,16(5):2490-2499.
APA Chen, Jinzhu,Li, Kegui,Chen, Limin,Liu, Ruliang,Huang, Xing,&Ye, Daiqi.(2014).Conversion of fructose into 5-hydroxymethylfurfural catalyzed by recyclable sulfonic acid-functionalized metal-organic frameworks.GREEN CHEMISTRY,16(5),2490-2499.
MLA Chen, Jinzhu,et al."Conversion of fructose into 5-hydroxymethylfurfural catalyzed by recyclable sulfonic acid-functionalized metal-organic frameworks".GREEN CHEMISTRY 16.5(2014):2490-2499.
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