Citation: WANG Zhan-Qi, ZHOU Zhi-Ming, ZHANG Rui, LI Li, CHENG Zhen-Min. Selective Hydrogenation of Phenylacetylene over Pd-Cu/γ-Al₂O₃ Catalysts[J]. Acta Physico-Chimica Sinica, ;2014, 30(12): 2315-2322. doi: 10.3866/PKU.WHXB201410152 shu

Selective Hydrogenation of Phenylacetylene over Pd-Cu/γ-Al₂O₃ Catalysts

1.
1. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China;
2. Engineering Research Center of Large Scale Reactor Engineering and Technology, Ministry of Education, East China University of Science and Technology, Shanghai 200237, P. R. China;
3. Institute of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, P. R. China

Received Date: 20 August 2014
Available Online: 15 October 2014
Fund Project: 教育部新世纪优秀人才支持计划(NCET-13-0801) (NCET-13-0801)中央高校基本科研业务费(222201313011)资助 (222201313011)

A two-step method combining colloid synthesis and incipient wetness impregnation was developed for the preparation of bimetallic Pd-Cu/γ-Al₂O₃ catalysts, with the aim of increasing the selectivity to styrene in the selective hydrogenation of phenylacetylene. The structural properties of the catalysts were characterized using high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), CO-pulse chemisorption, N₂ physisorption, and inductively coupled plasma atomic emission spectrometry (ICPAES). The effects of changing the Cu/Pd molar ratio, the Pd loading, and the order in which the Pd and Cu were introduced into the catalysts on the catalytic activity and selectivity were investigated. The results showed that Pd-Cu/γ-Al₂O₃ exhibited much higher selectivity toward styrene than Pd/γ-Al₂O₃. In particular, Pd-Cu/γ-Al₂O₃ with a Pd loading of 0.3%(w) and a Cu/Pd molar ratio of 0.6 displayed excellent performance at 40℃under 0.1 MPa H₂, with a high selectivity of 95% at a conversion of 90%, and a selectivity of approximately 82%, even at conversions of higher than 99%. The increased selectivity of Pd-Cu/γ- Al₂O₃ was ascribed mainly to the geometrical effects of the Pd-Cu bimetallic alloys, rather than the electronic effects, since no electron transfer occurred between Pd and Cu.
- Pd-Cu/γ-Al₂O₃,
- Selective hydrogenation,
- Phenylacetylene,
- Styrene,
- Structureperformance relationship
1. [1]
  
  (1) Galobardes, M.; Maurer, B. R. Selective Hydrogenation of Phenylacetylene in the Presence of Styrene. U.S. Patent 4822936, 1989-04-18.
2. [2]
  (2) Xiao, J.; Yang,W.; Chen, Y. H.; Chen, X. H. Ind. Catal. 2004, 12, 7. [肖剑, 杨伟, 陈祎华, 陈秀宏. 工业催化, 2004, 12, 7.]
3. [3]
  (3) Li, C.; Shao, Z.; Pang, M.;Williams, C. T.; Liang, C. Catal. Today 2012, 186, 69. doi: 10.1016/j.cattod.2011.09.005
4. [4]
  (4) Panpranot, J.; Phandinthong, K.; Sirikajorn, T.; Arai, M.; Praserthdam, P. J. Mol. Catal. A: Chem. 2007, 261, 29. doi: 10.1016/j.molcata.2006.07.053
5. [5]
  (5) Na-Chiangmai, C.; Tiengchad, N.; Kittisakmontree, P.; Mekasuwandumrong, O.; Powell, J.; Panpranot, J. Catal. Lett. 2011, 141, 1149. doi: 10.1007/s10562-011-0593-3
6. [6]
  (6) Hu, J.; Zhou, Z.; Zhang, R.; Li, L.; Cheng, Z. J. Mol. Catal. A: Chem. 2014, 381, 61. doi: 10.1016/j.molcata.2013.10.008
7. [7]
  (7) Tao, F. F. Chem. Soc. Rev. 2012, 41, 7977. doi: 10.1039/c2cs90093a
8. [8]
  (8) Guczi, L.; Schay, Z.; Stefler, G.; Liotta, L. F.; Deganello, G.; Venezia, A. M. J. Catal. 1999, 182, 456. doi: 10.1006/jcat.1998.2344
9. [9]
  (9) Domínguez-Domínguez, S.; Berenguer-Murcia, Á.; Cazorla-Amorós, D.; Linares-Solano, Á. J. Catal. 2006, 243, 74. doi: 10.1016/j.jcat.2006.06.027
10. [10]
  (10) Yoshida, H.; Zama, T.; Fujita, S.; Panpranot, J.; Arai, M. RSC Advances 2014, 4, 24922. doi: 10.1039/c4ra02220c
11. [11]
  (11) Shao, Z.; Li, C.; Liang, C. H. J. Mol. Catal. 2014, 28, 47. [邵正锋, 李闯, 梁长海. 分子催化, 2014, 28, 47.]
12. [12]
  (12) Kyriakou, G.; Boucher, M. B.; Jewell, A. D.; Lewis, E. A.; Lawton, T. J.; Baber, A. E.; Tierney, H. L.; Flytzani- Stephanopoulos, M.; Sykes, E. C. H. Science 2012, 335, 1209. doi: 10.1126/science.1215864
13. [13]
  (13) Boucher, M. B.; Zugic, B.; Cladaras, G.; Kammert, J.; Marcinkowski, M. D.; Lawton, T. J.; Sykes, E. C. H.; Flytzani-Stephanopoulos, M. Phys. Chem. Chem. Phys. 2013, 15, 12187. doi: 10.1039/c3cp51538a
14. [14]
  (14) Kim, S. K.; Lee, J. H.; Ahn, I. Y.; Kim,W.; Moon, S. H. Appl. Catal. A 2011, 401, 12. doi: 10.1016/j.apcata.2011.04.048
15. [15]
  (15) Weerachawanasak, P.; Mekasuwandumrong, O.; Arai, M.; Fujita, S.; Praserthdam, P.; Panpranot, J. J. Catal. 2009, 262, 199. doi: 10.1016/j.jcat.2008.12.011
16. [16]
  (16) Molnár, Á.; Sárkány, A.; Varga, M. J. Mol. Catal. A: Chem. 2001, 173, 185. doi: 10.1016/S1381-1169(01)00150-9
17. [17]
  (17) Shao, Z.; Li, C.; Chen, X.; Pang, M.;Wang, X.; Liang, C. ChemCatChem 2010, 2, 1555. doi: 10.1002/cctc.v2.12
18. [18]
  (18) Mao, J.; Liu, Y.; Chen, Z.;Wang, D.; Li, Y. Chem. Commun. 2014, 50, 4588. doi: 10.1039/c4cc01051e
19. [19]
  (19) Sitthisa, S.; Pham, T.; Prasomsri, T.; Sooknoi, T.; Mallinson, R. G.; Resasco, D. E. J. Catal. 2011, 280, 17. doi: 10.1016/j.jcat.2011.02.006
20. [20]
  (20) Jeroro, E.; Hyman, M. P.; Vohs, J. M. Phys. Chem. Chem. Phys. 2009, 11, 10457. doi: 10.1039/b913220a
21. [21]
  (21) Pattamakomsan, K.; Ehret, E.; Morfin, F.; Gélin, P.; Jugnet, Y.; Prakash, S.; Bertolini, J. C.; Panpranot, J.; Aires, F. J. C. S. Catal. Today 2011, 164, 28. doi: 10.1016/j.cattod.2010.10.013
22. [22]
  (22) Venezia, A. M.; Liotta, L. F.; Deganello, G.; Schay, Z.; Guczi, L. J. Catal. 1999, 182, 449. doi: 10.1006/jcat.1998.2343
23. [23]
  (23) Skoda, F.; Astier, M. P.; Pajonk, G. M.; Primet, M. Catal. Lett. 1994, 29, 159.
24. [24]
  (24) Strohmeier, B. R.; Levden, D. E.; Field, R. S.; Hercules, D. M. J. Catal. 1985, 94, 514. doi: 10.1016/0021-9517(85)90216-7
25. [25]
  (25) Leviness, S.; Nair, V.;Weiss, A. H.; Schay, Z.; Guczi, L. J. Mol. Catal. 1984, 25, 131. doi: 10.1016/0304-5102(84)80037-1
1. [1]
  Chengqian Mao , Yanghan Chen , Haotong Bai , Junru Huang , Junpeng Zhuang . Photodimerization of Styrylpyridinium Salt and Its Application in Silk Screen Printing. University Chemistry, 2024, 39(5): 354-362. doi: 10.3866/PKU.DXHX202312014
2. [2]
  Peng YUE , Liyao SHI , Jinglei CUI , Huirong ZHANG , Yanxia GUO . Effects of Ce and Mn promoters on the selective oxidation of ammonia over V₂O₅/TiO₂ catalyst. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 293-307. doi: 10.11862/CJIC.20240210
3. [3]
  Jun LUO , Baoshu LIU , Yunchang ZHANG , Bingkai WANG , Beibei GUO , Lan SHE , Tianheng CHEN . Europium(Ⅲ) metal-organic framework as a fluorescent probe for selectively and sensitively sensing Pb²⁺ in aqueous solution. Chinese Journal of Inorganic Chemistry, 2024, 40(12): 2438-2444. doi: 10.11862/CJIC.20240240
4. [4]
  Baitong Wei , Jinxin Guo , Xigong Liu , Rongxiu Zhu , Lei Liu . Theoretical Study on the Structure, Stability of Hydrocarbon Free Radicals and Selectivity of Alkane Chlorination Reaction. University Chemistry, 2025, 40(3): 402-407. doi: 10.12461/PKU.DXHX202406003
5. [5]
  Bin HE , Hao ZHANG , Lin XU , Yanghe LIU , Feifan LANG , Jiandong PANG . Recent progress in multicomponent zirconium?based metal-organic frameworks. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2041-2062. doi: 10.11862/CJIC.20240161
6. [6]
  Yi Li , Zhaoxiang Cao , Peng Liu , Xia Wu , Dongju Zhang . Revealing the Coloration and Color Change Mechanisms of the Eriochrome Black T Indicator through Computational Chemistry and UV-Visible Absorption Spectroscopy. University Chemistry, 2025, 40(3): 132-139. doi: 10.12461/PKU.DXHX202405154
7. [7]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
8. [8]
  Lihui Jiang , Wanrong Dong , Hua Yang , Yongqing Xia , Hongjian Peng , Jun Yuan , Xiaoqian Hu , Zihan Zeng , Yingping Zou , Yiming Luo . Study on Extraction of p-Hydroxyacetophenone. University Chemistry, 2024, 39(11): 259-268. doi: 10.12461/PKU.DXHX202402056
9. [9]
  Hongyi LI , Aimin WU , Liuyang ZHAO , Xinpeng LIU , Fengqin CHEN , Aikui LI , Hao HUANG . Effect of Y(PO₃)₃ double-coating modification on the electrochemical properties of Li[Ni_0.8Co_0.15Al_0.05]O₂. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1320-1328. doi: 10.11862/CJIC.20230480
10. [10]
  Yongqing Kuang , Jie Liu , Jianjun Feng , Wen Yang , Shuanglian Cai , Ling Shi . Experimental Design for the Two-Step Synthesis of Paracetamol from 4-Hydroxyacetophenone. University Chemistry, 2024, 39(8): 331-337. doi: 10.12461/PKU.DXHX202403012
11. [11]
  Wenlong LI , Xinyu JIA , Jie LING , Mengdan MA , Anning ZHOU . Photothermal catalytic CO₂ hydrogenation over a Mg-doped In₂O_3-x catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 919-929. doi: 10.11862/CJIC.20230421
12. [12]
  Shihui Shi , Haoyu Li , Shaojie Han , Yifan Yao , Siqi Liu . Regioselectively Synthesis of Halogenated Arenes via Self-Assembly and Synergistic Catalysis Strategy. University Chemistry, 2024, 39(5): 336-344. doi: 10.3866/PKU.DXHX202312002
13. [13]
  Yunhao Zhang , Yinuo Wang , Siran Wang , Dazhen Xu . Progress in Selective Construction of Functional Aromatics from Nitrogenous Cycloalkanes. University Chemistry, 2024, 39(11): 136-145. doi: 10.3866/PKU.DXHX202401083
14. [14]
  Peiran ZHAO , Yuqian LIU , Cheng HE , Chunying DUAN . A functionalized Eu³⁺ metal-organic framework for selective fluorescent detection of pyrene. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 713-724. doi: 10.11862/CJIC.20230355
15. [15]
  Xilin Zhao , Xingyu Tu , Zongxuan Li , Rui Dong , Bo Jiang , Zhiwei Miao . Research Progress in Enantioselective Synthesis of Axial Chiral Compounds. University Chemistry, 2024, 39(11): 158-173. doi: 10.12461/PKU.DXHX202403106
16. [16]
  Jiakun BAI , Ting XU , Lu ZHANG , Jiang PENG , Yuqiang LI , Junhui JIA . A red-emitting fluorescent probe with a large Stokes shift for selective detection of hypochlorous acid. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1095-1104. doi: 10.11862/CJIC.20240002
17. [17]
  .
  CCS Chemistry | 超分子活化底物为自由基促进高效选择性光催化氧化
  . CCS Chemistry, 2025, 7(10.31635/ccschem.025.202405229): -.
18. [18]
  Qiang ZHAO , Zhinan GUO , Shuying LI , Junli WANG , Zuopeng LI , Zhifang JIA , Kewei WANG , Yong GUO . Cu₂O/Bi₂MoO₆ Z-type heterojunction: Construction and photocatalytic degradation properties. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 885-894. doi: 10.11862/CJIC.20230435
19. [19]
  Tianqi Bai , Kun Huang , Fachen Liu , Ruochen Shi , Wencai Ren , Songfeng Pei , Peng Gao , Zhongfan Liu . 石墨烯厚膜热扩散系数与微观结构的关系. Acta Physico-Chimica Sinica, 2025, 41(3): 2404024-. doi: 10.3866/PKU.WHXB202404024
20. [20]
  Junjie Zhang , Yue Wang , Qiuhan Wu , Ruquan Shen , Han Liu , Xinhua Duan . Preparation and Selective Separation of Lightweight Magnetic Molecularly Imprinted Polymers for Trace Tetracycline Detection in Milk. University Chemistry, 2024, 39(5): 251-257. doi: 10.3866/PKU.DXHX202311084

Get Citation

PDF

XML

Metrics

PDF Downloads(334)
Abstract views(501)
HTML views(11)

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

Selective Hydrogenation of Phenylacetylene over Pd-Cu/γ-Al2O3 Catalysts

Metrics

通讯作者: 陈斌, bchen63@163.com

Selective Hydrogenation of Phenylacetylene over Pd-Cu/γ-Al₂O₃ Catalysts