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题名: 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
作者: 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
发表日期: 2017-09-01
DOI: 10.1016/j.jcat.2017.07.022
卷: 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
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.
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
语种: 英语
WOS记录号: WOS:000410468300015
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/150024
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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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

Recommended Citation:
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.
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