Ultrastable 3V-PPh3 polymers supported single Rh sites for fixed-bed hydroformylation of olefins
[Display omitted] •The catalyst provided ultrahigh stability for fixed-bed hydroformylation of olefins.•HAADF-STEM and EXAFS indicated the Rh atoms existed in single Rh sites.•The catalyst’s stability originated from strong interaction between Rh and support. The heterogenization of homogeneous cata...
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| Published in | Journal of molecular catalysis. A, Chemical Vol. 404-405; pp. 211 - 217 |
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| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Elsevier B.V
01.08.2015
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| Subjects | |
| Online Access | Get full text |
| ISSN | 1381-1169 1873-314X |
| DOI | 10.1016/j.molcata.2015.05.008 |
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| Abstract | [Display omitted]
•The catalyst provided ultrahigh stability for fixed-bed hydroformylation of olefins.•HAADF-STEM and EXAFS indicated the Rh atoms existed in single Rh sites.•The catalyst’s stability originated from strong interaction between Rh and support.
The heterogenization of homogeneous catalysts is of critical importance for both fundamental research and practical applications. The key obstacle to industrial applications of heterogenized homogeneous catalysts is the long-term stability of the immobilized molecular complexes. We unambiguously demonstrate in this report that the vinyl-functionalized PPh3 polymers supported single Rh sites (Rh/POL–PPh3) catalyst provided not only excellent catalytic activity but also ultrahigh stability for fixed-bed olefins hydroformylation, which is one of the most important industrial homogeneous catalytic processes for the synthesis of aldehydes and alcohols. HAADF-STEM and EXAFS results indicated that the Rh atoms were present in single Rh sites which were strongly coordinated with the exposed phosphorous atoms of the POL–PPh3 support. The Rh/POL-PPh3 catalyst provided high activity and selectivity because it maintained the catalytic functionalities similar to the homogeneous HRh(CO)(PPh3)3 complex, as demonstrated both by 31P MAS NMR and in situ FT-IR experiments. Thus a reaction mechanism, similar to that over the homogeneous HRh(CO)(PPh3)3 complex, was proposed for olefin hydroformylation over the novel Rh/POL–PPh3 catalyst. |
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| AbstractList | [Display omitted]
•The catalyst provided ultrahigh stability for fixed-bed hydroformylation of olefins.•HAADF-STEM and EXAFS indicated the Rh atoms existed in single Rh sites.•The catalyst’s stability originated from strong interaction between Rh and support.
The heterogenization of homogeneous catalysts is of critical importance for both fundamental research and practical applications. The key obstacle to industrial applications of heterogenized homogeneous catalysts is the long-term stability of the immobilized molecular complexes. We unambiguously demonstrate in this report that the vinyl-functionalized PPh3 polymers supported single Rh sites (Rh/POL–PPh3) catalyst provided not only excellent catalytic activity but also ultrahigh stability for fixed-bed olefins hydroformylation, which is one of the most important industrial homogeneous catalytic processes for the synthesis of aldehydes and alcohols. HAADF-STEM and EXAFS results indicated that the Rh atoms were present in single Rh sites which were strongly coordinated with the exposed phosphorous atoms of the POL–PPh3 support. The Rh/POL-PPh3 catalyst provided high activity and selectivity because it maintained the catalytic functionalities similar to the homogeneous HRh(CO)(PPh3)3 complex, as demonstrated both by 31P MAS NMR and in situ FT-IR experiments. Thus a reaction mechanism, similar to that over the homogeneous HRh(CO)(PPh3)3 complex, was proposed for olefin hydroformylation over the novel Rh/POL–PPh3 catalyst. |
| Author | Jiang, Miao Zhu, Hejun Yan, Li Ding, Yunjie Sun, Qi Xiao, Fengshou Liu, Jingyue Liu, Jia Lin, Ronghe Jiang, Zheng |
| Author_xml | – sequence: 1 givenname: Miao surname: Jiang fullname: Jiang, Miao organization: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China – sequence: 2 givenname: Li surname: Yan fullname: Yan, Li organization: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China – sequence: 3 givenname: Yunjie surname: Ding fullname: Ding, Yunjie email: dyj@dicp.ac.cn organization: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China – sequence: 4 givenname: Qi surname: Sun fullname: Sun, Qi organization: Department of Chemistry, Zhejiang University, Hangzhou 310027, China – sequence: 5 givenname: Jia surname: Liu fullname: Liu, Jia organization: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China – sequence: 6 givenname: Hejun surname: Zhu fullname: Zhu, Hejun organization: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China – sequence: 7 givenname: Ronghe surname: Lin fullname: Lin, Ronghe organization: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China – sequence: 8 givenname: Fengshou surname: Xiao fullname: Xiao, Fengshou organization: Department of Chemistry, Zhejiang University, Hangzhou 310027, China – sequence: 9 givenname: Zheng surname: Jiang fullname: Jiang, Zheng organization: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China – sequence: 10 givenname: Jingyue surname: Liu fullname: Liu, Jingyue email: Jingyue.Liu@asu.edu organization: Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China |
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•The catalyst provided ultrahigh stability for fixed-bed hydroformylation of olefins.•HAADF-STEM and EXAFS indicated the Rh atoms existed in... |
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| SubjectTerms | Heterogenized catalysts Hydroformylation Porous organic ligands Rhodium Stability |
| Title | Ultrastable 3V-PPh3 polymers supported single Rh sites for fixed-bed hydroformylation of olefins |
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