Characterization and reactivity of γ-Al2O3 supported Pd–Cu bimetallic nanocatalysts for the selective oxygenization of cyclopentene

引用本文: Wei-Wei Liu, Yi-Si Feng, Guang-Yu Wanga, Wei-Wei Jiang, Hua-Jian Xu. Characterization and reactivity of γ-Al₂O₃ supported Pd–Cu bimetallic nanocatalysts for the selective oxygenization of cyclopentene[J]. Chinese Chemical Letters, 2016, 27(6): 905-909. doi: 10.1016/j.cclet.2016.02.026 shu

Citation: Wei-Wei Liu, Yi-Si Feng, Guang-Yu Wanga, Wei-Wei Jiang, Hua-Jian Xu. Characterization and reactivity of γ-Al₂O₃ supported Pd–Cu bimetallic nanocatalysts for the selective oxygenization of cyclopentene[J]. Chinese Chemical Letters, 2016, 27(6): 905-909. doi: 10.1016/j.cclet.2016.02.026 shu

Characterization and reactivity of γ-Al₂O₃ supported Pd–Cu bimetallic nanocatalysts for the selective oxygenization of cyclopentene

a School of Chemistry and Chemical Engineering, School of Medical Engineering, Hefei University of Technology, Hefei 230009, China;
b Anhui Key Laboratory of Controllable Chemical Reaction & Material Chemical Engineering, Hefei 230009, China;
c Anhui Provincial Laboratory of Heterocyclic Chemistry, Maanshan 243110, China
基金项目:
We are grateful to the financial assistance from the National Natural Science Foundation of China (Nos. 21272050, 21371044, 21472033 and 21571047).

摘要: In this work, Pd-Cu/γ-Al₂O₃ is prepared by the impregnation method and investigated for selective oxygenization of cyclopentene to cyclopentanone. A series of bimetallic Pd-Cu/g-Al₂O₃ nanocatalysts were prepared and the structures characterized by XRD, XPS and TEM. We determined that the obtained Pd-Cu/γ-Al₂O₃ (molar ratio Pd:Cu = 5:1) was an efficient catalyst for the oxygenization of cyclopentene to cyclopentanone with >95% selectivity and >85% conversion (100 ℃, 1 MPa initial O₂ pressure, 7 h).

关键词:

English

Characterization and reactivity of γ-Al₂O₃ supported Pd–Cu bimetallic nanocatalysts for the selective oxygenization of cyclopentene

a School of Chemistry and Chemical Engineering, School of Medical Engineering, Hefei University of Technology, Hefei 230009, China;
b Anhui Key Laboratory of Controllable Chemical Reaction & Material Chemical Engineering, Hefei 230009, China;
c Anhui Provincial Laboratory of Heterocyclic Chemistry, Maanshan 243110, China
Received Date: 01 December 2015
Revised Date: 29 January 2016
Fund Project:
We are grateful to the financial assistance from the National Natural Science Foundation of China (Nos. 21272050, 21371044, 21472033 and 21571047).

Abstract: In this work, Pd-Cu/γ-Al₂O₃ is prepared by the impregnation method and investigated for selective oxygenization of cyclopentene to cyclopentanone. A series of bimetallic Pd-Cu/g-Al₂O₃ nanocatalysts were prepared and the structures characterized by XRD, XPS and TEM. We determined that the obtained Pd-Cu/γ-Al₂O₃ (molar ratio Pd:Cu = 5:1) was an efficient catalyst for the oxygenization of cyclopentene to cyclopentanone with >95% selectivity and >85% conversion (100 ℃, 1 MPa initial O₂ pressure, 7 h).

Key words:

1. [1] C. Sui, G. Lu, X.Y. Li, et al., Selective oxidation of cyclopentene catalyzed by Pd(CH₃COO)₂-NPMoV under oxygen a atmosphere, React. Kinet. Catal. Lett. 94 (2008) 191-198.
2. [2] C. Sui, X.Y. Li, Z.P. Qu, Research progress of cyclopentanone synthesis, Chem. Ind. Eng. Prog. 27 (2008) 809-813.
3. [3] K. Takehira, T. Hayakawa, H. Orita, M. Shimizu, Mono-oxygenation of cyclopentene by molecular oxygen catalyzed by PdCl₂-CuCl₂ in ethanol, J. Mol. Catal. 53 (1989) 15-21.
4. [4] K. Takehira, H. Orita, I.H. Oh, et al., Palladium(II)-catalyzed oxidation of cyclopentene in the presence of copper (II) chloride and molecular oxygen, J. Mol. Catal. 42 (1987) 247-255.
5. [5] J.J. Mao, Y.X. Liu, Z. Chen, D.S. Wang, Y.D. Li, Bimetallic Pd-Cu nanocrystals and their tunable catalytic properties, Chem. Commun. 50 (2014) 4588-4591.
6. [6] F. Cárdenas-Lizana, S. Gómez-Quero, C. Amorim, M.A. Keane, Gas phase hydrogenation of p-chloronitrobenzene over Pd-Ni/Al₂O₃, Appl. Catal., A: Gen. 473 (2014) 41-50.
7. [7] H. Yang, D. Shi, S.F. Ji, D.N. Zhang, X.F. Liu, Nanosized Pd assembled on superparamagnetic core-shell microspheres: synthesis, characterization and recyclable catalytic properties for the Heck reaction, Chin. Chem. Lett. 25 (2014) 1265-1270.
8. [8] N.S. Babu, N. Lingaiah, P.S.S. Prasad, Characterization and reactivity of Al₂O₃ supported Pd-Ni bimetallic catalysts for hydrodechlorination of chlorobenzene, Appl. Catal., B: Environ. 111-112 (2012) 309-316.
9. [9] S.J.S. Basha, P. Vijayan, C. Suresh, D. Santhanaraj, K. Shanthi, Effect of order of impregnation of Mo and Ni on the hydrodenitrogenation activity of NiO-MoO₃/AlMCM-41 catalyst, Ind. Eng. Chem. Res. 48 (2009) 2774-2780.
10. [10] J.A. Bergwerff, T. Visser, B.R.G. Leliveld, et al., Envisaging the physicochemical processes during the preparation of supported catalysts: Raman microscopy on the impregnation of Mo onto Al₂O₃ extrudates, J. Am. Chem. Soc. 126 (2004) 14548-14556.
11. [11] Y. Qiu, L. Xin, W.Z. Li, Electrocatalytic oxygen evolution over supported small amorphous Ni-Fe nanoparticles in alkaline electrolyte, Langmuir 30 (2014) 7893-7901.
12. [12] Y.S. Feng, J. Hao, W.W. Liu, et al., Characterization and reactivity of γ-Al₂O₃ supported Pd-Ni bimetallic nanocatalysts for selective hydrogenation of cyclopentadiene, Chin. Chem. Lett. 26 (2015) 709-713.
13. [13] Y.S. Feng, C. Liu, Y.M. Kang, et al., Selective hydrogenolysis of glycerol to 1,2-propanediol catalyzed by supported bimetallic PdCu-KF/γ-Al₂O₃, Chem. Eng. J. 281 (2015) 96-101.
14. [14] J.X. Zhou, L.Y. Guo, X.W. Guo, J.B. Mao, S.G. Zhang, Selective hydrogenolysis of glycerol to propanediol on supported Cu-containing bimetallic catalysis, Green Chem. 12 (2010) 1835-1843.
15. [15] R. Morrish, A.J. Muscat, Nanoporous silver with controllable optical properties formed by chemical dealloying in supercritical CO₂, Chem. Mater. 21 (2009) 3865-3870.
16. [16] X.Q. Pan, Y.B. Zhang, Z.Z. Miao, X.G. Yang, A novel PdNi/Al₂O₃ catalyst prepared by galvanic deposition for low temperature methane combustion, J. Energy Chem. 22 (2013) 610-616.
17. [17] X.Q. Pan, Y.B. Zhang, B. Zhang, et al., Influence of electronic effect on methane catalytic combustion over PdNi/Al₂O₃, Chem. Res. Chin. Univ. 29 (2013) 952-955.

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 1591
HTML全文浏览量: 30

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

Characterization and reactivity of γ-Al₂O₃ supported Pd–Cu bimetallic nanocatalysts for the selective oxygenization of cyclopentene

English

Characterization and reactivity of γ-Al₂O₃ supported Pd–Cu bimetallic nanocatalysts for the selective oxygenization of cyclopentene

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处