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Role of MoO3 on a Rhodium Catalyst in the Selective Hydrogenolysis of Biomass-Derived Tetrahydrofurfuryl Alcohol into 1,5-Pentanediol
Guan, Jing1; Peng, Gongming1; Cao, Quan1,2; Mu, Xindong1
2014-11-06
发表期刊JOURNAL OF PHYSICAL CHEMISTRY C
卷号118期号:44页码:25555-25566
摘要Selective hydrogenolysis of biomass-derived tetrahydrofurfuryl alcohol (THFA) to produce 1,5-pentanediol (1,5-PeD) is accomplished by a binary catalyst consisting of MoO3 and supported Rh nanoparticles; a 1,5-PeD selectivity up to 80% is achieved in the present work. Moreover, a very interesting phase-transfer behavior for MoO3 during the reaction is observed with the assistance of different characterization techniques. In this process, MoO3 dissolves partially in the liquid phase under the reaction conditions and is transformed into the soluble hydrogen molybdenum oxide bronzes (HxMoO(3)) in the presence of H-2, which are recognized as the genuinely active sites for the CO bond breaking of THFA. Density functional theory (DFT) calculations were then carried out to simulate the plausible mechanisms and highlight the role of Mo in the ring-opening process of THFA in more detail. We propose that the formation of 1,5-PeD takes place in a two consecutive reactions. THFA first undergoes acid-catalyzed ring-opening process to form the key intermediate 5-hydroxypentanal with the homogeneous catalysis of dissolved HxMoO(3). The intermediate is then quickly hydrogenated into 1,5-PeD under the heterogeneous catalysis of Rh. The concerted hydrogen-transferring-opening mechanism plausibly explains the high reaction selectivity toward 1,5-PeD in the hydrogenolysis of THFA and is verified by the reactivity trends of related substrates.
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
DOI10.1021/jp508313y
关键词[WOS]AQUEOUS-PHASE HYDRODEOXYGENATION ; TOTAL-ENERGY CALCULATIONS ; AUGMENTED-WAVE METHOD ; C-O BOND ; ETHYLENE-GLYCOL ; BIO-OIL ; CHEMOSELECTIVE HYDROGENOLYSIS ; UNSATURATED-HYDROCARBONS ; MOLYBDENUM TRIOXIDE ; CYCLIC ETHERS
收录类别SCI
语种英语
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science
WOS类目Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号WOS:000344579300029
引用统计
被引频次:29[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.qibebt.ac.cn/handle/337004/6176
专题绿色化学催化团队
作者单位1.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, CAS Key Lab Biobased Mat, Qingdao 266101, Shandong, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
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Guan, Jing,Peng, Gongming,Cao, Quan,et al. Role of MoO3 on a Rhodium Catalyst in the Selective Hydrogenolysis of Biomass-Derived Tetrahydrofurfuryl Alcohol into 1,5-Pentanediol[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2014,118(44):25555-25566.
APA Guan, Jing,Peng, Gongming,Cao, Quan,&Mu, Xindong.(2014).Role of MoO3 on a Rhodium Catalyst in the Selective Hydrogenolysis of Biomass-Derived Tetrahydrofurfuryl Alcohol into 1,5-Pentanediol.JOURNAL OF PHYSICAL CHEMISTRY C,118(44),25555-25566.
MLA Guan, Jing,et al."Role of MoO3 on a Rhodium Catalyst in the Selective Hydrogenolysis of Biomass-Derived Tetrahydrofurfuryl Alcohol into 1,5-Pentanediol".JOURNAL OF PHYSICAL CHEMISTRY C 118.44(2014):25555-25566.
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