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Xantphos doped Rh/POPs-PPh3 catalyst for highly selective long-chain olefins hydroformylation: Chemical and DFT insights into Rh location and the roles of Xantphos and PPh3
Li, Cunyao1; Sun, Keju3; Wang, Wenlong1; Yan, Li1; Sun, Xueping5; Wang, Yuqing1; Xiong, Kai4; Zhan, Zhuangping4; Jiang, Zheng5; Ding, Yunjie1,2
关键词Heterogeneous Hydroformylation Long-chain Olefins Porous Organic Polymers Linear-regioselectivity
刊名JOURNAL OF CATALYSIS
2017-09-01
DOI10.1016/j.jcat.2017.07.022
353页:123-132
收录类别SCI
文章类型Article
WOS标题词Science & Technology ; Physical Sciences ; Technology
类目[WOS]Chemistry, Physical ; Engineering, Chemical
研究领域[WOS]Chemistry ; Engineering
关键词[WOS]SUPERCRITICAL CARBON-DIOXIDE ; GAS-PHASE HYDROFORMYLATION ; FIXED-BED HYDROFORMYLATION ; MODIFIED RH/SIO2 CATALYSTS ; IONIC LIQUID ; TETRAPHOSPHORUS LIGANDS ; RHODIUM CATALYST ; REGIOSELECTIVE HYDROFORMYLATION ; ASYMMETRIC HYDROFORMYLATION ; PROPYLENE CARBONATE
英文摘要Vinyl functionalized Xantphos ligand (denoted as 4v-Xantphos) was newly synthesized and successfully doped into the PPh3 based porous organic polymers (POPs) through the solvothermal synthesis technique. After proper coordination with Rh precursor, the resultant Xantphos doped Rh/POPs-PPh3 catalysts exhibited high activity (TOF: 300-500 h(-1)), chemoselectivity (87-91%) and regioselectivity (about 90:10) in the hydroformylation of long-chain olefins (C6-C12). As a representative substrate, hydroformylation of 1-octene could be easily realized in a fixed bed reactor for more than 400 h with high efficiency employing Xantphos doped Rh/POPs-PPh3 catalyst, which represented a rare successful example that realized heterogenization of homogeneous hydrofromylation catalysts as well as the regioselectivity-control at the same time without leaching of rhodium. Interestingly, the hydroformylation reaction data indicated that the Rh species tend to coordinate with the exposed P atom from Xantphos rather than that from PPh3 ligand in the Xantphos doped catalyst frame. More importantly, the HAADF-STEM and EXAFS characterizations indicated that Rh species demonstrated as single site dispersion in Xantphos doped Rh/POPs-PPh3 catalyst, thus endowed the catalyst with high activity. Detailed DFT calculations revealed that the unique location of single site dispersed Rh species (Rh species coordinated with both of Xantphos and PPh3 in the catalyst frame simultaneously) was responsible for the high linear regioselectivity and stability of the catalysts, the roles of Xantphos and PPh3 were further elucidated in details. (C) 2017 Elsevier Inc. All rights reserved.
语种英语
WOS记录号WOS:000410468300015
引用统计
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/150024
专题中国科学院大连化学物理研究所
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
3.Yanshan Univ, Coll Environm & Chem Engn, Key Lab Appl Chem, Qinhuangdao 066004, Peoples R China
4.Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, Xiamen 361005, Peoples R China
5.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
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Li, Cunyao,Sun, Keju,Wang, Wenlong,et al. Xantphos doped Rh/POPs-PPh3 catalyst for highly selective long-chain olefins hydroformylation: Chemical and DFT insights into Rh location and the roles of Xantphos and PPh3[J]. JOURNAL OF CATALYSIS,2017,353:123-132.
APA Li, Cunyao.,Sun, Keju.,Wang, Wenlong.,Yan, Li.,Sun, Xueping.,...&Ding, Yunjie.(2017).Xantphos doped Rh/POPs-PPh3 catalyst for highly selective long-chain olefins hydroformylation: Chemical and DFT insights into Rh location and the roles of Xantphos and PPh3.JOURNAL OF CATALYSIS,353,123-132.
MLA Li, Cunyao,et al."Xantphos doped Rh/POPs-PPh3 catalyst for highly selective long-chain olefins hydroformylation: Chemical and DFT insights into Rh location and the roles of Xantphos and PPh3".JOURNAL OF CATALYSIS 353(2017):123-132.
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