Citation: Yuan Pei, Chen Jian, Pan Deng, Bao Xiaojun. Adsorption and Reaction Kinetic Studies of the Heterogeneous Catalytic Hydrogenation for Polystyrene[J]. Acta Chimica Sinica, ;2016, 74(7): 603-611. doi: 10.6023/A16030117 shu

Adsorption and Reaction Kinetic Studies of the Heterogeneous Catalytic Hydrogenation for Polystyrene

Yuan Pei ^a,*,, ,
Chen Jian ^a ,
Pan Deng ^b ,
Bao Xiaojun ^b

a.
State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249
b.
The Key Laboratory of Catalysis, China University of Petroleum, Beijing 102249

Corresponding author: Yuan Pei, yuanpei@cup.edu.cn
Received Date: 4 March 2016

Fund Project: China National Petroleum Corp. 2012B-2805The National Natural Science Foundation of China 21106182The National Natural Science Foundation of China 21576290

Figures(10)

We applied silica hollow microspheres with through holes in the shell as supports to prepare Pd-based supported catalyst (Pd/SHMs) for heterogeneous catalytic hydrogenation of polystyrene (PS) and also systematically studied the adsorption and reaction behavior of PS molecules over Pd/SHMs. The dynamic adsorption and reaction models of PS molecules under different temperatures have been established and the partially hydrogenated products were also comprehensively analyzed. The result shows that both the adsorption capacity and saturation time are increased as the temperature increasing and this hydrogenation reaction is confirmed to be a first-order reaction and the activation energy is calculated to be 58.3 kJ·mol^-1. After separating and purifying three samples with different hydrogenation degrees, we further analyzed the partially hydrogenated products and the results show that they are all actually comprised of two kinds of substances with different properties, one with high hydrogenation conversion rate (ca. 85%) and the other with low hydrogenation ratio (ca. 25%). It is proved that PS heterogeneous hydrogenation process exists secondary adsorption and competitive adsorption phenomenon, and obeys the Blocky mechanism. This work lays the foundation for PS adsorption and hydrogenation reaction and is also favorable for the understanding of the adsorption and catalytic process for other unsaturated polymers over heterogeneous catalysts.
- hydrogenation,
- adsorption,
- kinetics,
- supported catalyst,
- unsaturated polymer
1. [1]
  Singha, N. K.; Bhattacharjee, S.; Sivaram, S. Rubber Chem. Technol. 1997, 70, 311.
2. [2]
  Xu, Z. D.; Hadjichristidis, N.; Carella, J. M.; Fetters, L. J. Macromolecules 1983, 16, 925. doi: 10.1021/ma00240a019
3. [3]
  Dondos, A.; Staikos, G. Colloid Polym. Sci. 1995, 273, 626. doi: 10.1007/BF00652254
4. [4]
  Garcia Escribiano, P.; Canovas, M. J.; Ojeda, M. C.; Del Rio, C.; Sanchez, F.; Acosta, J. L. Polym. Int. 2011, 60, 493. doi: 10.1002/pi.v60.3
5. [5]
  Wei, Z. L.; Wu, J. L.; Pan, Q. M.; Rempel, G. L. Macromol. Rapid Commun. 2005, 26, 1768. doi: 10.1002/(ISSN)1521-3927
6. [6]
  Monroy-Barreto, M.; Acosta, J. L.; Del Rio, C.; Ojeda, M. C.; Munoz, M.; Aguilar, J. C. J. Power Sources 2010, 195, 8052. doi: 10.1016/j.jpowsour.2010.06.105
7. [7]
  Jin, M.; Liao, M.; Zhai, J.; Jiang, L. Acta Chim. Sinica 2008, 66, 145.
8. [8]
  Xu, L.; Li, W.; Yang, M. Acta Chim. Sinica 2007, 65, 1917.
9. [9]
  Zhang, S.; Bai, Y.; Peng, J.; Hu, Y.; Lai, G. Prog. Chem. 2013, 25, 707.
10. [10]
  Przybyszewska, M.; Zaborski, M. Composite Interfaces 2009, 16, 131. doi: 10.1163/156855409X402920
11. [11]
  Yoon, K.; Kim, K. O.; Schaefer, M.; Yoon, D. Y. Polymer 2012, 53, 2290. doi: 10.1016/j.polymer.2012.02.047
12. [12]
  Choi, M.; Kim, Y.; Ha, C. Prog. Polym. Sci. 2008, 33, 581. doi: 10.1016/j.progpolymsci.2007.11.004
13. [13]
  Gehlsen, M. D.; Bates, F. S. Macromolecules 1993, 26, 4122. doi: 10.1021/ma00068a009
14. [14]
  Huang, H.; Fan, Y.; Tao, S.; Gao, H. New Chem. Mater. 2013, 41, 178.
15. [15]
  Ness, J. S.; Brodil, J. C.; Bates, F. S.; Hahn, S. F.; Hucul, D. A.; Hillmyer, M. A. Macromolecules 2001, 35, 602.
16. [16]
  Dong, L. B.; Turgman-Cohen, S.; Roberts, G. W.; Kiserow, D. J. Ind. Eng. Chem. Res. 2010, 49, 11280. doi: 10.1021/ie1011905
17. [17]
  Xu, D.; Carbonell, R. G.; Kiserow, D. J.; Roberts, G. W. Ind. Eng. Chem. Res. 2003, 42, 3509. doi: 10.1021/ie0301841
18. [18]
  Hucul, D. A.; Hahn, S. F. Adv. Mater. 2000, 12, 1855. doi: 10.1002/(ISSN)1521-4095
19. [19]
  Aylward, F.; Sawistowka, M.; Arthur, F.; Robert, C. B.; Shirley, H. Chem. Rev. 1965, 65, 51. doi: 10.1021/cr60233a002
20. [20]
  Parent, J. S.; Mcmanus, N. T.; Rempel, G. L. Ind. Eng. Chem. Res. 1996, 35, 4417. doi: 10.1021/ie9506680
21. [21]
  Martin, P.; Mcmanus, N. T.; Rempel, G. L. J. Mol. Catal. A: Chem. 1997, 126, 115. doi: 10.1016/S1381-1169(97)00102-7
22. [22]
  Bhattacharjee, S.; Bhowmick, A. K.; Avasthi, B. N. J. Polym. Sci. Part A: Polym. Chem. 1992, 30, 471. doi: 10.1002/pola.1992.080300314
23. [23]
  Bond, G. C. Heterogeneous Catalysis: Principles and Applications, 2nd Ed., Clarendon Press, Oxford, 1987, p. 120.
24. [24]
  Bussard, A.; Dooley, K. M. AIChE J. 2008, 54, 1064. doi: 10.1002/(ISSN)1547-5905
25. [25]
  Zhou, H.; Qiang, M.; Li, J.; Li, Y.; Wang, J. Polym. Mater. Sci. Eng. 2011, 27, 73.
26. [26]
  Almusaiteer, K. A. Top. Catal. 2012, 55, 498. doi: 10.1007/s11244-012-9821-3
27. [27]
  Hutchings, G. J. J. Mater. Chem. 2009, 19, 1222. doi: 10.1039/B812300B
28. [28]
  Fang, F.; Satulovsky, J.; Szleifer, I. Biophys. J. 2005, 89, 1516. doi: 10.1529/biophysj.104.055079
29. [29]
  Rosedale, J. H.; Bates, F. S. J. Am. Chem. Soc. 1988, 110, 3542. doi: 10.1021/ja00219a032
30. [30]
  Huang, H.; Zhou, J.; Ying, Q.; Tao, S. Mod. Chem. Ind. 2014, 34, 70.
31. [31]
  Cassano, G. A.; Vallés, E. M.; Quinzani, L. M. Polymer 1998, 39, 5573. doi: 10.1016/S0032-3861(97)10080-5
32. [32]
  Tsukagoshi, T.; Kondo, Y.; Yoshino, N. Colloids Surf. B-Biointerfaces 2007, 54, 101. doi: 10.1016/j.colsurfb.2006.10.004
33. [33]
  Linse, P.; Kallrot, N. Macromolecules 2010, 43, 2054. doi: 10.1021/ma902338m
34. [34]
  Kawaguchi, M.; Anada, S.; Nishikawa, K.; Kurata, N. Macromolecules 1992, 25, 1588. doi: 10.1021/ma00031a035
35. [35]
  Kawaguchi, M.; Sakata, Y.; Anada, S.; Kato, T.; Takahashi, A. Langmuir 1994, 10, 538. doi: 10.1021/la00014a033
36. [36]
  Rybicka, J.; Sikorski, A. Macromol. Theory Simul. 2010, 19, 135.
37. [37]
  Scheutjens, J. M. H. M.; Fleer, G. J. J. Phys. Chem. 1979, 83, 1619. doi: 10.1021/j100475a012
38. [38]
  Scheutjens, J. M. H. M.; Fleer, G. J. J. Phys. Chem. 1980, 84, 178. doi: 10.1021/j100439a011
39. [39]
  Doi, Y.; Yano, A.; Soga, K.; Burfield, D. R. Macromolecules 1986, 19, 2409. doi: 10.1021/ma00163a013
40. [40]
  Tangthongkul, R.; Prasassarakich, P.; Mcmanus, N. T.; Rempel, G. L. J. Appl. Polym. Sci. 2004, 91, 3259. doi: 10.1002/(ISSN)1097-4628
41. [41]
  Hinchiranan, N.; Charmondusit, K.; Prasassarakich, P.; Rempel, G. L. J. Appl. Polym. Sci. 2006, 100, 4219. doi: 10.1002/(ISSN)1097-4628
42. [42]
  Pan, D.; Shi, G.; Zhang, T.; Yuan, P.; Fan, Y.; Bao, X. J. Mater. Chem. A 2013, 1, 9597. doi: 10.1039/c3ta11824j
43. [43]
  Dijt, J. C.; Cohen Stuart, M. A.; Fleer, G. J. Macromolecules 1994, 27, 3207. doi: 10.1021/ma00090a014
44. [44]
  Kislenko, V. N.; Berlin, A. A.; Kawaguchi, M.; Kato, T. Langmuir 1996, 12, 768. doi: 10.1021/la950478u
45. [45]
  Tóth, J. Adsorption: Theory, Modeling, and Analysis, Marcel Dekker, New York, 2002, p. 26.
46. [46]
  Whittier, R. E. MS Thesis, North Carolina State University, Raleigh, 2004.
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