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Selective Hydrogenation of Biomass-Based 5-Hydroxymethylfurfural over Catalyst of Palladium Immobilized on Amine-Functionalized Metal-Organic Frameworks
Chen, Jinzhu1; Liu, Ruliang1,3; Guo, Yuanyuan1; Chen, Limin2; Gao, Hui1
2015-02-01
发表期刊ACS CATALYSIS
卷号5期号:2页码:722-733
摘要A catalyst of palladium [Pd/MIL-101(Al)-NH2] supported on amine-functionalized Metal Organic Frameworks (MOFs) allows selective hydrogenation of biomass-based 5-hydroxymethylfurfural (HMF) to 2,5-dihydroxymethyl-tetrahydrofuran (DHMTHF) with 2,5-dihydroxymethylfuran (DHMF) as an observed "intermediate". The Pd/MIL-101(Al)-NH2 was prepared by using a direct anionic exchange approach and subsequent gentle reduction. The presence of free amine moieties in the frameworks of MIL-101(AI)-NH2 is suggested to play a key role on the formation of uniform and well-dispersed palladium nanoparticles on the support. The adsorption experiments reveal that the amine-functionalized MOF supports show preferential adsorption to hydrogenation intermediate DHMF than in the case of reactant HMF owing to an enhanced hydrophilic nature of DHMF as well as improved hydrogen bonding interactions between DHMF and the MOP support, which promotes a further hydrogenation of DHMF to DHMTHF upon the in situ formation of DHMF over Pd/MIL-101(A1)-NH2. Moreover, our results also indicate that the observed high selectivity toward DHMTHF form HMF is closely related to the cooperation between the metallic site and the free amine moiety on the MOF support. Under the optimal conditions, a maximum DHMTHF yield of 96% with a full conversion of HMF is obtained by using Pd/MIL-101(Al)-NH2 (Pd 3.0 wt %) catalyst at a low reaction temperature of 30 degrees C in aqueous medium. The research thus highlights new perspectives for aluminum-based and amine-functionalized MOP material for biomass transformation.
文章类型Article
关键词Biomass Hydrogenation 5-hydroxymethylfurfural Palladium Metal-organic Frameworks
WOS标题词Science & Technology ; Physical Sciences
DOI10.1021/cs5012926
研究领域[WOS]Chemistry
关键词[WOS]CROSS-COUPLING REACTION ; CARBOHYDRATE DEHYDRATION ; PHOSPHOTUNGSTIC ACID ; RENEWABLE RESOURCES ; SUPPORTED PALLADIUM ; CYCLIC ETHERS ; CONVERSION ; NANOPARTICLES ; EFFICIENT ; HYDROGENOLYSIS
收录类别SCI
语种英语
WOS类目Chemistry, Physical
WOS记录号WOS:000349275300028
引用统计
被引频次:57[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/344007/10797
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, Guangzhou 510006, Guangdong, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
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Chen, Jinzhu,Liu, Ruliang,Guo, Yuanyuan,et al. Selective Hydrogenation of Biomass-Based 5-Hydroxymethylfurfural over Catalyst of Palladium Immobilized on Amine-Functionalized Metal-Organic Frameworks[J]. ACS CATALYSIS,2015,5(2):722-733.
APA Chen, Jinzhu,Liu, Ruliang,Guo, Yuanyuan,Chen, Limin,&Gao, Hui.(2015).Selective Hydrogenation of Biomass-Based 5-Hydroxymethylfurfural over Catalyst of Palladium Immobilized on Amine-Functionalized Metal-Organic Frameworks.ACS CATALYSIS,5(2),722-733.
MLA Chen, Jinzhu,et al."Selective Hydrogenation of Biomass-Based 5-Hydroxymethylfurfural over Catalyst of Palladium Immobilized on Amine-Functionalized Metal-Organic Frameworks".ACS CATALYSIS 5.2(2015):722-733.
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