Home

Citation: Yuan You-Zhu, Zhang Yu, Chen Zhong, Zhang Hong-Bin, Cai Qi-Rui. Structure and Hydroformylation Performance of Supported Aqueous-phase Rh Catalyst[J]. Acta Physico-Chimica Sinica, ;1998, 14(11): 1013-1019. doi: 10.3866/PKU.WHXB19981110 shu

Structure and Hydroformylation Performance of Supported Aqueous-phase Rh Catalyst

1.
Department of Chemistry,Institute of Physical Chemistry,State Key Laboratory for Physical Chemistry of Solid Surface,Xiamen University,Xiamen 361005

Received Date: 9 February 1998
Available Online: 15 November 1998

The catalytic activity of hydroformylation of 1-hexene over SiO2-supported TPPTSRh(acac)(CO)2 (SAPC) was found to be evidently promoted when a proper amount of water-vapor was introduced into the reactant. Characterization results by using MAS NMR 31p spectra revealed that there were three types of phosphine species in the as-prepared SAPC: uncoordinated ligand TPPTS (over 70 mol%), surface complex {Rh(CO)(TPPTS)2} (chemical shift at δ=32.4, about 15 mol%), and unknown (about 10 mol%). By pre-treatment at 373 K for 2 under dry-snygas or at 333 K for 2 h under wet-syngas, the amount of phosphine species of the surface complex{Rh(CO)(TPPTS)2} was slightly increased to 20-30mol%, accompanying a few changes in ratios of the other phsophine species. When the SAPC was pre-treated at 373 K for 2 h under wet-syngas, however, the phosphine species at chemical shift of 32.4 was increased by over 40 mol% due to the in-situ formation of the surface complex {Rh(CO)(TPPTS)2}. It was found that the peak at δ=32.4 was also a principal one in the MAS NMR 31P spectra of the working SAPC, which demonstrated that the surface complex of {Rh(CO)(TPPTS)2 } would be a catalytic active species for olefin hydroformyaltion. After hydroformylation for 43 h, the deactivation of the catalyst occurred, corresponding to the observations of a broadness in peak ascribed to the surface complex of {An(CO)(TPPTS)z} in the MAS NMR 31P spectra, indicating that there existed de-coordination of the surface complex and oxidation of the ligand TPPTS during the reaction. The results suggest that a proper amount of water-vapor was able to accelerate the formation of active Rh-complex on the catalyst surface and thus increase the catalytic activity, whereas, it could be inevitably to cause the de-coordination of the surface complex and the oxidation of phosphine ligand under the reaction condition, hence leading to the deactivation of the catalyst.
- Hydroformylation,
- Supported aqueous-phase catalyst,
- MAS NMR31P spectroscopy,
- 1-hexene
1. [1]
  Jingzhao Cheng , Shiyu Gao , Bei Cheng , Kai Yang , Wang Wang , Shaowen Cao . Construction of 4-Amino-1H-imidazole-5-carbonitrile Modified Carbon Nitride-Based Donor-Acceptor Photocatalyst for Efficient Photocatalytic Hydrogen Evolution. Acta Physico-Chimica Sinica, 2024, 40(11): 2406026-0. doi: 10.3866/PKU.WHXB202406026
2. [2]
  Bing LIU , Huang ZHANG , Hongliang HAN , Changwen HU , Yinglei ZHANG . Visible light degradation of methylene blue from water by triangle Au@TiO₂ mesoporous catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 941-952. doi: 10.11862/CJIC.20230398
3. [3]
  Xi YANG , Chunxiang CHANG , Yingpeng XIE , Yang LI , Yuhui CHEN , Borao WANG , Ludong YI , Zhonghao HAN . Co-catalyst Ni₃N supported Al-doped SrTiO₃: Synthesis and application to hydrogen evolution from photocatalytic water splitting. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 440-452. doi: 10.11862/CJIC.20240371
4. [4]
  Asif Hassan Raza , Shumail Farhan , Zhixian Yu , Yan Wu . Double S-Scheme ZnS/ZnO/CdS Heterostructure Photocatalyst for Efficient Hydrogen Production. Acta Physico-Chimica Sinica, 2024, 40(11): 2406020-0. doi: 10.3866/PKU.WHXB202406020
5. [5]
  Mian Wei , Chang Cheng , Bowen He , Bei Cheng , Kezhen Qi , Chuanbiao Bie . Inorganic-organic CdS/YBTPy S-scheme photocatalyst for efficient hydrogen production and its mechanism. Acta Physico-Chimica Sinica, 2025, 41(12): 100158-0. doi: 10.1016/j.actphy.2025.100158
6. [6]
  Jiaqi Yang , Xuqiang Hao , Jiejie Jing , Yuqiang Hao , Zhiliang Jin . 3D/2D ReSe₂/ZnCdS S-scheme photocatalyst with efficient interfacial charge separation for optimized hydrogen production. Acta Physico-Chimica Sinica, 2025, 41(10): 100131-0. doi: 10.1016/j.actphy.2025.100131
7. [7]
  Jiali Lei , Juan Wang , Wenhui Zhang , Guohong Wang , Zihui Liang , Jinmao Li . TiO₂/CdIn₂S₄ S-scheme heterojunction photocatalyst promotes photocatalytic hydrogen evolution coupled vanillyl alcohol oxidation. Acta Physico-Chimica Sinica, 2025, 41(12): 100174-0. doi: 10.1016/j.actphy.2025.100174
8. [8]
  Yuanyuan Ping , Wangqing Kong . 光催化碳氢键官能团化合成1-苯基-1,2-乙二醇. University Chemistry, 2025, 40(6): 238-247. doi: 10.12461/PKU.DXHX202408092
9. [9]
  Xuejie Wang , Guoqing Cui , Congkai Wang , Yang Yang , Guiyuan Jiang , Chunming Xu . Research Progress on Carbon-based Catalysts for Catalytic Dehydrogenation of Liquid Organic Hydrogen Carriers. Acta Physico-Chimica Sinica, 2025, 41(5): 100044-0. doi: 10.1016/j.actphy.2024.100044
10. [10]
  Haodong JIN , Qingqing LIU , Chaoyang SHI , Danyang WEI , Jie YU , Xuhui XU , Mingli XU . NiCu/ZnO heterostructure photothermal electrocatalyst for efficient hydrogen evolution reaction. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1068-1082. doi: 10.11862/CJIC.20250048
11. [11]
  Juan WANG , Zhongqiu WANG , Qin SHANG , Guohong WANG , Jinmao LI . NiS and Pt as dual co-catalysts for the enhanced photocatalytic H₂ production activity of BaTiO₃ nanofibers. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1719-1730. doi: 10.11862/CJIC.20240102
12. [12]
  Ying Chen , Ronghua Yan , Weiyan Yin . Research Progress on the Synthesis of Metal Single-Atom Catalysts and Their Applications in Electrocatalytic Hydrogen Evolution Reactions. University Chemistry, 2025, 40(9): 344-353. doi: 10.12461/PKU.DXHX202503066
13. [13]
  Yuying JIANG , Jia LUO , Zhan GAO . Development status and prospects of solid oxide cell high entropy electrode catalysts. Chinese Journal of Inorganic Chemistry, 2025, 41(9): 1719-1730. doi: 10.11862/CJIC.20250124
14. [14]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1953-1964. doi: 10.11862/CJIC.20240028
15. [15]
  Shuang Yang , Qun Wang , Caiqin Miao , Ziqi Geng , Xinran Li , Yang Li , Xiaohong Wu . Ideological and Political Education Design for Research-Oriented Experimental Course of Highly Efficient Hydrogen Production from Water Electrolysis in Aerospace Perspective. University Chemistry, 2024, 39(11): 269-277. doi: 10.12461/PKU.DXHX202403044
16. [16]
  Xue Liu , Lipeng Wang , Luling Li , Kai Wang , Wenju Liu , Biao Hu , Daofan Cao , Fenghao Jiang , Junguo Li , Ke Liu . Research on Cu-Based and Pt-Based Catalysts for Hydrogen Production through Methanol Steam Reforming. Acta Physico-Chimica Sinica, 2025, 41(5): 100049-0. doi: 10.1016/j.actphy.2025.100049
17. [17]
  Zhuoming Liang , Ming Chen , Zhiwen Zheng , Kai Chen . Multidimensional Studies on Ketone-Enol Tautomerism of 1,3-Diketones By ¹H NMR. University Chemistry, 2024, 39(7): 361-367. doi: 10.3866/PKU.DXHX202311029
18. [18]
  Zhanggui DUAN , Yi PEI , Shanshan ZHENG , Zhaoyang WANG , Yongguang WANG , Junjie WANG , Yang HU , Chunxin LÜ , Wei ZHONG . Preparation of UiO-66-NH₂ supported copper catalyst and its catalytic activity on alcohol oxidation. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 496-506. doi: 10.11862/CJIC.20230317
19. [19]
  Huijuan Liao , Yulin Xiao , Dong Xue , Mingyu Yang , Jianyang Dong . Synthesis of 1-Benzyl Isoquinoline via the Minisci Reaction. University Chemistry, 2025, 40(7): 294-299. doi: 10.12461/PKU.DXHX202409092
20. [20]
  Qiangqiang SUN , Pengcheng ZHAO , Ruoyu WU , Baoyue CAO . Multistage microporous bifunctional catalyst constructed by P-doped nickel-based sulfide ultra-thin nanosheets for energy-efficient hydrogen production from water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1151-1161. doi: 10.11862/CJIC.20230454

Get Citation

PDF

XML

Metrics

PDF Downloads(2167)
Abstract views(3569)
HTML views(18)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Address：Zhongguancun North First Street 2,100190 Beijing, PR China Tel: +86-010-82449177-888

DownLoad: Full-Size Img PowerPoint

Return