Citation: WANG Wei-Yan, ZHANG Xiao-Zhe, YANG Yun-Quan, YANG Yan-Song, PENG Hui-Zuo, LUO He-An. Preparation of La-Ni-Mo-B Amorphous Catalyst and Its Catalytic Properties for Hydrodeoxygenation of Phenol[J]. Acta Physico-Chimica Sinica, ;2012, 28(05): 1243-1251. doi: 10.3866/PKU.WHXB201203081 shu

Preparation of La-Ni-Mo-B Amorphous Catalyst and Its Catalytic Properties for Hydrodeoxygenation of Phenol

1.
School of Chemical Engineering, Xiangtan University, Xiangtan 411105, Hunan Province, P. R. China

Received Date: 1 January 2012
Available Online: 8 March 2012
Fund Project: 湘潭大学资助基金(2011XZX11) (2011XZX11)湖南省教育厅开放基金(10K062)资助项目 (10K062)

Lanthanum-promoted Ni-Mo-B amorphous catalysts were prepared by chemical reduction of the corresponding metal salts with sodium borohydride aqueous solution. Scanning electron microscopy (SEM), X-ray diffraction (XRD), inductively coupled plasma atomic emission spectrometry (ICP-AES), and X-ray photoelectron spectroscopy (XPS) were used to characterize the resulting materials. Phenol was used as model compound to test the hydrodeoxygenation (HDO) activity of the La-Ni-Mo-B amorphous catalysts. Adding lanthanum could decrease the particle size, increase the content of Ni⁰ and promote the reduction of Mo⁶⁺ to Mo⁴⁺ . But excess lanthanum would cover some of the Ni⁰, and Mo⁴⁺ active sites. The high hydrogenation activity was attributed to the amorphous structure of the catalyst and the high content of Ni⁰ and the high degree of deoxygenation was attributed to the high content of MoO₂. The HDO reation of phenol on the La-Ni-Mo-B amorphous catalyst proceeded with a hydrogenation-dehydration route, thus decreasing the aromatic content of the HDO products. Both the conversion and the total deoxygenation degree were up to 99.0%. The deactivation of the La-Ni-Mo-B amorphous catalysts during the HDO reation of phenol at high temperature was mainly caused by the crystallization of the amorphous structure.
- Amorphous catalyst,
- La-Ni-Mo-B,
- Hydrodeoxygenation,
- Phenol,
- Bio-oil
1. [1]
  (1) Bull, T. E.; Turner, J. A. Science 1999, 285, 1209.
2. [2]
  (2) Zakzeski, J.; Bruijnincx, P. C. A.; Jongerius, A. L.; Weckhuysen, B. M. Chem. Rev. 2010, 110, 3552.
3. [3]
  (3) Furimsky, E. Appl. Catal. A: Gen. 2000, 199, 147.
4. [4]
  (4) önal, E. P.; Uzun, B. B.; Pütün, A. E. Fuel Process. Technol. 2011, 92, 879.
5. [5]
  (5) French, R.; Czernik, S. Fuel Process. Technol. 2010, 91, 25.
6. [6]
  (6) Bunch, A. Y.; Wang, X.; Ozkan, U. S. J. Mol. Catal. A: Chem. 2007, 270, 264.
7. [7]
  (7) Senol, O. I.; Ryymin, E. M.; Viljava, T. R.; Krause, A. O. I. J. Mol. Catal. A: Chem. 2007, 277, 107.
8. [8]
  (8) Yang, Y.; Luo, H. a.; Tong, G.; Smith, K. J.; Tye, C. T. Chin. J. Chem. Eng. 2008, 16, 733.
9. [9]
  (9) Ryymin, E. M.; Honkela, M. L.; Viljava, T. R.; Krause, A. O. I. Appl. Catal. A: Gen. 2009, 358, 42.
10. [10]
  (10) Kubicka, D.; Bejblová, M.; Vlk, J. Top. Catal. 2010, 53, 168.
11. [11]
  (11) Badawi, M.; Paul, J. F.; Cristol, S.; Payen, E.; Romero, Y.; Richard, F.; Brunet, S.; Lambert, D.; Portier, X.; Popov, A.; Kondratieva, E.; upil, J. M.; El Fallah, J.; Gilson, J. P.; Mariey, L.; Travert, A.; Maugé, F. J. Catal. 2011, 282, 155.
12. [12]
  (12) Bui, V. N.; Laurenti, D.; Delichère, P.; Geantet, C. Appl. Catal. B: Environ. 2011, 101, 246.
13. [13]
  (13) Romero, Y.; Richard, F.; Brunet, S. Appl. Catal. B: Environ. 2010, 98, 213.
14. [14]
  (14) Yang, Y.; Gilbert, A.; Xu, C. Appl. Catal. A: Gen. 2009, 360, 242.
15. [15]
  (15) Whiffen, V. M. L.; Smith, K. J. Energy Fuels 2010, 24, 4728.
16. [16]
  (16) Li, K.; Wang, R.; Chen, J. Energy Fuels 2011, 25, 854.
17. [17]
  (17) Zhao, H. Y.; Li, D.; Bui, P.; Oyama, S. T. Appl. Catal. A: Gen. 2011, 391, 305.
18. [18]
  (18) Zhao, C.; Kou, Y.; Lemonidou, A. A.; Li, X.; Lercher, J. A. Angew. Chem. Int. Edit. 2009, 48, 3987.
19. [19]
  (19) Crossley, S.; Faria, J.; Shen, M.; Resasco, D. E. Science 2010, 327, 68.
20. [20]
  (20) Li, N.; Huber, G. W. J. Catal. 2010, 270, 48.
21. [21]
  (21) Ruiz, P. E.; Leiva, K.; Garcia, R.; Reyes, P.; Fierro, J. L. G.; Escalona, N. Appl. Catal. A: Gen. 2010, 384, 78.
22. [22]
  (22) nzález-Borja, M. A. n.; Resasco, D. E. Energy Fuels 2011, 25, 4155.
23. [23]
  (23) Nimmanwudipong, T.; Runnebaum, R. C.; Block, D. E.; Gates, B. C. Energy Fuels 2011, 25, 3417.
24. [24]
  (24) Sitthisa, S.; Pham, T.; Prasomsri, T.; Sooknoi, T.; Mallinson, R. G.; Resasco, D. E. J. Catal. 2011, 280, 17.
25. [25]
  (25) Zhu, X.; Lobban, L. L.; Mallinson, R. G.; Resasco, D. E. J. Catal. 2011, 281, 21.
26. [26]
  (26) Wang, Y.; Fang, Y.; He, T.; Hu, H.; Wu, J. Catal. Commun. 2011, 12, 1201.
27. [27]
  (27) Yan, N.; Yuan, Y.; Dykeman, R.; Kou, Y.; Dyson, P. J. Angew. Chem. Int. Edit. 2010, 49, 5549.
28. [28]
  (28) Zhang, W.; Zhang, Y.; Zhao, L.; Wei, W. Energy Fuels 2010, 24, 2052.
29. [29]
  (29) Zhao, C.; Kou, Y.; Lemonidou, A. A.; Li, X.; Lercher, J. A. Chem. Commun. 2010, 46, 412.
30. [30]
  (30) Mei, D.; Karim, A. M.; Wang, Y. J. Phys. Chem. C 2011, 115, 8155.
31. [31]
  (31) Viljava, T. R.; Komulainen, R. S.; Krause, A. O. I. Catal. Today 2000, 60, 83.
32. [32]
  (32) Ferrari, M.; Bosmans, S.; Maggi, R.; Delmon, B.; Grange, P. Catal. Today 2001, 65, 257.
33. [33]
  (33) Bunch, A. Y.; Ozkan, U. S. J. Catal. 2002, 206, 177.
34. [34]
  (34) Senol, O. I.; Viljava, T. R.; Krause, A. O. I. Catal. Today 2005, 106, 186.
35. [35]
  (35) Gandarias, I.; Barrio, V. L.; Requies, J.; Arias, P. L.; Cambra, J. F.; Güemez, M. B. Int. J. Hydrogen Energy 2008, 33, 3485.
36. [36]
  (36) Yang, Y. Q.; Tye, C. T.; Smith, K. J. Catal. Commun. 2008, 9, 1364.
37. [37]
  (37) Zhao, B.; Chou, C. J.; Chen, Y. W. Ind. Eng. Chem. Res. 2010, 49, 1669.
38. [38]
  (38) Li, H.; Zhang, D.; Li, G.; Xu, Y.; Lu, Y.; Li, H. Chem. Commun. 2010, 46, 791.
39. [39]
  (39) Li, H.; Xu, Y.; Yang, H.; Zhang, F.; Li, H. J. Mol. Catal. A: Chem. 2009, 307, 105.
40. [40]
  (40) Chen, Y. W.; Sasirekha, N. Ind. Eng. Chem. Res. 2009, 48, 6248.
41. [41]
  (41) Rajesh, B.; Sasirekha, N.; Lee, S. P.; Kuo, H. Y.; Chen, Y. W. J. Mol. Catal. A: Chem. 2008, 289, 69.
42. [42]
  (42) Zheng, Y. X.; Yao, S. B.; Zhou, S. M. Acta Phys. -Chim. Sin. 2004, 20, 1352. [郑一雄, 姚士冰, 周绍民. 物理化学学报, 2004, 20, 1352.]
43. [43]
  (43) Li, H.; Liu, J.; Xie, S.; Qiao, M.; Dai, W.; Li, H. J. Catal. 2008, 259, 104.
44. [44]
  (44) Tong, D. G.; Chu, W.; Luo, Y. Y.; Ji, X. Y.; He, Y. J. Mol. Catal. A: Chem. 2007, 265, 195.
45. [45]
  (45) Tong, D.; Han, X.; Chu, W.; Chen, H.; Ji, X. Y. Mater. Lett. 2007, 61, 4679.
46. [46]
  (46) Li, H.; Yang, P.; Chu, D.; Li, H. Appl. Catal. A: Gen. 2007, 325, 34.
47. [47]
  (47) Li, H.; Li, H.; Zhang, J.; Dai, W.; Qiao, M. J. Catal. 2007, 246, 301.
48. [48]
  (48) Long, J. Y.; Ma, L.; He, D. H. Acta Phys. -Chim. Sin. 2010, 26, 2719. [龙俊英, 马兰, 贺德华. 物理化学学报, 2010, 26, 2719.]
49. [49]
  (49) Liu, Y. C.; Chen, Y. W. Ind. Eng. Chem. Res. 2006, 45, 2973.
50. [50]
  (50) Li, H.; Wu, Y.; Zhang, J.; Dai, W.; Qiao, M. Appl. Catal. A: Gen. 2004, 275, 199.
51. [51]
  (51) Chen, X.; Wang, S.; Zhuang, J.; Qiao, M.; Fan, K.; He, H. J. Catal. 2004, 227, 419.
52. [52]
  (52) Li, H.; Wu, Y.; Luo, H.; Wang, M.; Xu, Y. J. Catal. 2003, 214, 15.
53. [53]
  (53) Lin, M. H.; Zhao, B.; Chen, Y. W. Ind. Eng. Chem. Res. 2009, 48, 7037.
54. [54]
  (54) Liu, H.; Wang, H.; Shen, J.; Sun, Y.; Liu, Z. Catal. Today 2008, 131, 444.
55. [55]
  (55) Wu, M. X.; Li, W.; Zhang, M. H.; Tao, K. Y. Acta Phys. -Chim. Sin. 2011, 27, 953. [武美霞, 李伟, 张明慧, 陶克毅. 物理化学学报, 2011, 27, 953.]
56. [56]
  (56) Liu, Y. C.; Chen, Y. W. Ind. Eng. Chem. Res. 2006, 45, 2973.
57. [57]
  (57) Shi, Q. J.; Lei, J. X.; Zhang, N. Acta Phys. -Chim. Sin. 2007, 23, 98. [石秋杰, 雷经新, 张宁. 物理化学学报, 2007, 23, 98.]
58. [58]
  (58) Li, H.; Zhang, S.; Luo, H. Mater. Lett. 2004, 58, 2741.
59. [59]
  (59) Hou, Y.; Wang, Y.; He, F.; Han, S.; Mi, Z.; Wu, W.; Min, E. Mater. Lett. 2004, 58, 1267.
60. [60]
  (60) Li, H.; Luo, H.; Zhuang, L.; Dai, W.; Qiao, M. J. Mol. Catal. A: Chem. 2003, 203, 267.
61. [61]
  (61) Wang, W. Y.; Yang, Y. Q.; Luo, H. A.; Peng, H. Z.; He, B.; Liu, W. Y. Catal. Commun. 2011, 12, 1275.
62. [62]
  (62) Wang, W. Y.; Yang, Y. Q.; Luo, H. A.; Hu, T.; Liu, W. Y. Catal. Commun. 2011, 12, 436.
63. [63]
  (63) Wang, W. Y.; Yang, Y. Q.; Bao, J. G.; Luo, H. A. Catal. Commun. 2009, 11, 100.
64. [64]
  (64) Kukula, P.; Gabova, V.; Koprivova, K.; Trtik, P. Catal. Today 2007, 121, 27.
65. [65]
  (65) Parks, G. L.; Pease, M. L.; Burns, A. W.; Layman, K. A.; Bussell, M. E.; Wang, X.; Hanson, J.; Rodriguez, J. A. J. Catal. 2007, 246, 277.
66. [66]
  (66) Wu, Z.; Ge, S. Catal. Commun. 2011, 13, 40.
67. [67]
  (67) Liu, B.; Qiao, M.; Wang, J.; Fan, K. Chem. Commun. 2002, 1236.
68. [68]
  (68) Liu, S. C.; Liu, Z.; Wang, Z.; Wu, Y.; Yuan, P. Chem. Eng. J. 2008, 139, 157.
69. [69]
  (69) Patel, N.; Fernandes, R.; Miotello, A. J. Catal. 2010, 271, 315.
70. [70]
  (70) Suslick, K. S.; Choe, S. B.; Cichowlas, A. A.; Grinstaff, M. W. Nature 1991, 353, 414.
71. [71]
  (71) Lu, L.; Rong, Z.; Du, W.; Ma, S.; Hu, S. ChemCatChem 2009, 1, 369.
72. [72]
  (72) Chen, X.; Li, H.; Dai, W.; Wang, J.; Ran, Y.; Qiao, M. Appl. Catal. A: Gen. 2003, 253, 359.
73. [73]
  (73) Zhang, R.; Li, F.; Shi, Q.; Luo, L. Appl. Catal. A: Gen. 2001, 205, 279.
74. [74]
  (74) Shen, J.; Chen, Y. J. Mol. Catal. A: Chem. 2007, 273, 265.
75. [75]
  (75) Zhang, X.; Ma, A.; Mu, X.; Min, E. Catal. Today 2002, 74, 77.
76. [76]
  (76) Liaw, B. J.; Chiang, S. J.; Chen, S. W.; Chen, Y. Z. Appl. Catal. A: Gen. 2008, 346, 179.
77. [77]
  (77) Meng, Q.; Li, H.; Li, H. J. Phys. Chem. C 2008, 112, 11448.
78. [78]
  (78) Patel, N.; Fernandes, R.; Miotello, A. J. Power Sources 2009, 188, 411.
79. [79]
  (79) Belatel, H.; Al-Kandari, H.; Al-Khorafi, F.; Katrib, A.; Garin, F. Appl. Catal. A: Gen. 2004, 275, 141.
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