Citation: LI Jian-Mei, LIU Jian, REN Li-Wei, LIU Qing-Long, ZHAO Zhen, WEI Yue-Chang, DUAN Ai-Jun, JIANG Gui-Yuan. Selective Oxidation of Ethane to Aldehydes over Potassium-Promoted SBA-15-Supported Molybdenum Oxide Catalysts[J]. Acta Physico-Chimica Sinica, ;2014, 30(9): 1736-1744. doi: 10.3866/PKU.WHXB201407091 shu

Selective Oxidation of Ethane to Aldehydes over Potassium-Promoted SBA-15-Supported Molybdenum Oxide Catalysts

1.
State Key Laboratory of Heavy Oil, College of Science, China University of Petroleum, Beijing 102249, P. R. China

Received Date: 16 April 2014
Available Online: 9 July 2014
Fund Project:

Potassium-modified SBA-15-supported molybdenum oxide catalysts were prepared using a twostep impregnation method. The physical and chemical properties of the catalysts were characterized using N2- adsorption-desorption, X-ray diffraction (XRD), transmission electron microscope (TEM), UV-visible (UV-Vis) spectroscopy, Raman spectroscopy, NH₃ temperature-programmed desorption (NH₃-TPD), CO₂ temperatureprogrammed desorption (CO₂-TPD), and H₂ temperature-programmed reduction (H₂-TPR). The results showed that potassium addition resulted in the formation of new potassium molybdates, and the states of molybdenum species varied with changes in the K/Mo molar ratio. The addition of potassium to Mo_0.75/SBA-15 effectively improved the activity of catalysts and the selectivity to the total aldehydes (formaldehyde, acetaldehyde, and acrolein), especially for acetaldehyde in the selective oxidation of ethane. The turn-over frequency (TOF) and product selectivity depended strongly on the potassium content. The maximum selectivity and yield of aldehydes were obtained by varying the K/Mo molar ratio. At 575 ℃, the maximum yield of aldehydes reached 8.5%(molar fraction) over K_0.25-Mo_0.75/SBA-15 catalyst. The formation of new potassium-molybdates promoted the activities and selectivities of the catalysts.
- Selective oxidation of ethane,
- K-modified catalyst,
- Molybdenum oxide,
- Aldehyde,
- SBA-15 mesoporous material
1. [1]
  
  (1) Lou, Y.;Wang, H.; Zhang, Q.;Wang, Y. J. Catal. 2007, 24, 245.
2. [2]
  (2) Nieto, J. M. L.; Solsona, B.; Concepcion, P.; Ivars, F.; Dejoz, A.; Vazquez, M. J. Catal. Today 2010, 157, 291. doi: 10.1016/j.cattod.2010.01.046
3. [3]
  (3) Liu, J.; Yu, L.; Zhao, Z.; Chen, Y.; Xu, C.; Duan, A.; Jiang, G. J. Catal. 2012, 285, 134. doi: 10.1016/j.jcat.2011.09.029
4. [4]
  (4) Zhao, Z.; Yamada, Y.; Teng, Y.; Ueda, A.; Nakagawa, K.; Kobayashi, T. J. Catal. 2000, 190, 215. doi: 10.1006/jcat.1999.2740
5. [5]
  (5) Zhao, Z.; Yamada, Y.; Ueda, A.; Sakurai, H.; Kobayashi, T. Appl. Catal. A 2000, 196, 37. doi: 10.1016/S0926-860X(99)00451-2
6. [6]
  (6) Zhang, Z.; Zhao, Z.; Xu, C.; Duan, A.; Sha, S.; Zhang, Y.; Dou, T. Chem. Lett. 2005, 34, 1080. doi: 10.1246/cl.2005.1080
7. [7]
  (7) Bañares, M. A.; Spencer, N. D.; Jones, M. D.;Wachs, I. E. J. Catal. 1994, 146, 204. doi: 10.1016/0021-9517(94)90023-X
8. [8]
  (8) Liu, J.; Zhao, Z.; Xu, C.; Duan, A.; Zhu, L.;Wang, X. Appl. Catal. B 2005, 61, 36. doi: 10.1016/j.apcatb.2005.04.006
9. [9]
  (9) Liu, J.; Zhao, Z.; Xu, C.; Duan, A.; Jiang, G. J. Phys. Chem. C 2008, 112, 5930.
10. [10]
  (10) Kobayashi, T. Catal. Today 2001, 71, 69. doi: 10.1016/S0920-5861(01)00439-4
11. [11]
  (11) Watson, R. B.; Ozkan, U. S. J. Catal. 2000, 191, 12. doi: 10.1006/jcat.1999.2781
12. [12]
  (12) Koc, S. N.; Gurdag, G.; Geissler, S.; Guraya, M.; Orbay, M.; Muhler, M. J. Mol. Catal. A 2005, 225, 197. doi: 10.1016/j.molcata.2004.09.009
13. [13]
  (13) Erdöhelyi, A.; Fodor, K.; Solymosi, F. J. Catal. 1997, 166, 244. doi: 10.1006/jcat.1997.1519
14. [14]
  (14) Erdöhelyi, A.; Máté, F.; Solymosi, F. Catal. Lett. 1991, 8, 229. doi: 10.1007/BF00764121
15. [15]
  (15) MacGiolla, C. E.; Mulhall, E.; Hoek, R.; Hodnett, B. K. Catal. Today 1989, 4, 383. doi: 10.1016/0920-5861(89)85034-5
16. [16]
  (16) Watson, R. B.; Ozkan, U. S. J. Phys. Chem. B 2002, 106, 6930. doi: 10.1021/jp025512+
17. [17]
  (17) Yoon, Y. S.; Ueda,W.; Moro-oka, Y. Catal. Lett. 1995, 35, 57. doi: 10.1007/BF00807004
18. [18]
  (18) Jurapatrakorn, J.; Coles, M. P.; Tilley, T. D. Chem. Mater. 2005, 17, 1818.
19. [19]
  (19) Fournier, J.; Louis, C.; Che, M.; Chaquin, P.; Masure, D. J. Catal. 1989, 119, 400. doi: 10.1016/0021-9517(89)90170-X
20. [20]
  (20) Williams, C. C.; Ekerdt, J. G.; Jehng, J. M.; Hardcastle, F. D.; Turek, A. M.;Wachs, I. E. J. Phys. Chem. 1991, 95, 8781. doi: 10.1021/j100175a067
21. [21]
  (21) Boer, M.; Dillen, A. J.; Koningsberger, D. C.; Geus, J.W.; Vuurman, M. A.;Wachs, I. E. Catal. Lett. 1991, 11, 227. doi: 10.1007/BF00764089
22. [22]
  (22) Desikan, A. N.; Huang, L.; Oyama, S.T. J. Phys. Chem. 1991, 95, 10050. doi: 10.1021/j100177a080
23. [23]
  (23) Zhang,W.; Desikan, A.; Oyama, S. T. J. Phys. Chem. 1995, 99, 14486. doi: 10.1021/j100039a041
24. [24]
  (24) Melero, J. A.; Iglesias, J.; Arsuaga, J. M.; Sainz-Pardo, J.; Frutos, P. S. Blazquez 2007, 331, 84.
25. [25]
  (25) Shupyk, I.; Piquemal, J. Y.; Briot, E.; Vaulay, M. J.; Connan, C.; Truong, S.; Zaitsev, V.; Bozon-Verduraz, F. Appl. Catal. A 2007, 325, 140. doi: 10.1016/j.apcata.2007.03.033
26. [26]
  (26) Takenaka, S.; Tanaka, T.; Funabiki, T.; Yoshida, S. J. Phys. Chem. B 1998, 102, 2960. doi: 10.1021/jp980134n
27. [27]
  (27) Verbruggen, N. F. D.; Mestl, G.; Hippel, L. M. J.; Lengeler, B.; Knozinger, H. Langmuir 1994, 10, 3063. doi: 10.1021/la00021a033
28. [28]
  (28) Verbruggen, N. F. D.; Hippel, L. M. J.; Mestl, G.; Lengeler, B.; Knoezinger, H. Langmuir 1994, 10, 3073. doi: 10.1021/la00021a034
29. [29]
  (29) Jede, E. J.; Requejo, F. G.; Pawelec, B.; Fierro, J. L. G. J. Phys. Chem. B 2002, 106, 7824. doi: 10.1021/jp014648p
30. [30]
  (30) Feng, L.; Li, X.; Dadyburjor, D. B.; Kugler, E. L. J. Catal. 2000, 190, 1. doi: 10.1006/jcat.1999.2744
31. [31]
  (31) Zhao, Z.; Liu, J.; Xu, C.; Duan, A.; Kobayashi, T.;Wachs, I. E. Topics in Catalysis 2006, 38, 309. doi: 10.1007/s11244-006-0030-9
32. [32]
  (32) Naraschewski, F. N.; Kumar1, C. P.; Jentys, A.; Lercher, J. A. Appl. Catal. A 2011, 39, 163.
1. [1]
  Xiaotian ZHU , Fangding HUANG , Wenchang ZHU , Jianqing ZHAO . Layered oxide cathode for sodium-ion batteries: Surface and interface modification and suppressed gas generation effect. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 254-266. doi: 10.11862/CJIC.20240260
2. [2]
  Lina Guo , Ruizhe Li , Chuang Sun , Xiaoli Luo , Yiqiu Shi , Hong Yuan , Shuxin Ouyang , Tierui Zhang . 层状双金属氢氧化物的层间阴离子对衍生的Ni-Al₂O₃催化剂光热催化CO₂甲烷化反应的影响. Acta Physico-Chimica Sinica, 2025, 41(1): 2309002-. doi: 10.3866/PKU.WHXB202309002
3. [3]
  Ping ZHANG , Chenchen ZHAO , Xiaoyun CUI , Bing XIE , Yihan LIU , Haiyu LIN , Jiale ZHANG , Yu'nan CHEN . Preparation and adsorption-photocatalytic performance of ZnAl@layered double oxides. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1965-1974. doi: 10.11862/CJIC.20240014
4. [4]
  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
5. [5]
  Xin Han , Zhihao Cheng , Jinfeng Zhang , Jie Liu , Cheng Zhong , Wenbin Hu . Design of Amorphous High-Entropy FeCoCrMnBS (Oxy) Hydroxides for Boosting Oxygen Evolution Reaction. Acta Physico-Chimica Sinica, 2025, 41(4): 100033-. doi: 10.3866/PKU.WHXB202404023
6. [6]
  Yaping ZHANG , Tongchen WU , Yun ZHENG , Bizhou LIN . Z-scheme heterojunction β-Bi₂O₃ pillared CoAl layered double hydroxide nanohybrid: Fabrication and photocatalytic degradation property. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 531-539. doi: 10.11862/CJIC.20240256
7. [7]
  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
8. [8]
  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
9. [9]
  Zhiquan Zhang , Baker Rhimi , Zheyang Liu , Min Zhou , Guowei Deng , Wei Wei , Liang Mao , Huaming Li , Zhifeng Jiang . Insights into the Development of Copper-based Photocatalysts for CO₂ Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2406029-. doi: 10.3866/PKU.WHXB202406029
10. [10]
  Bing WEI , Jianfan ZHANG , Zhe CHEN . Research progress in fine tuning of bimetallic nanocatalysts for electrocatalytic carbon dioxide reduction. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 425-439. doi: 10.11862/CJIC.20240201
11. [11]
  Chuanming GUO , Kaiyang ZHANG , Yun WU , Rui YAO , Qiang ZHAO , Jinping LI , Guang LIU . Performance of MnO₂-0.39IrO_x composite oxides for water oxidation reaction in acidic media. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1135-1142. doi: 10.11862/CJIC.20230459
12. [12]
  Xueyu Lin , Ruiqi Wang , Wujie Dong , Fuqiang Huang . 高性能双金属氧化物负极的理性设计及储锂特性. Acta Physico-Chimica Sinica, 2025, 41(3): 2311005-. doi: 10.3866/PKU.WHXB202311005
13. [13]
  Junli Liu . Practice and Exploration of Research-Oriented Classroom Teaching in the Integration of Science and Education: a Case Study on the Synthesis of Sub-Nanometer Metal Oxide Materials and Their Application in Battery Energy Storage. University Chemistry, 2024, 39(10): 249-254. doi: 10.12461/PKU.DXHX202404023
14. [14]
  Xiaofeng Zhu , Bingbing Xiao , Jiaxin Su , Shuai Wang , Qingran Zhang , Jun Wang . Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides. Acta Physico-Chimica Sinica, 2024, 40(12): 2407005-. doi: 10.3866/PKU.WHXB202407005
15. [15]
  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
16. [16]
  .
  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): -.
17. [17]
  Hailian Tang , Siyuan Chen , Qiaoyun Liu , Guoyi Bai , Botao Qiao , Fei Liu . Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions. Acta Physico-Chimica Sinica, 2025, 41(4): 100036-. doi: 10.3866/PKU.WHXB202408004
18. [18]
  Endong YANG , Haoze TIAN , Ke ZHANG , Yongbing LOU . Efficient oxygen evolution reaction of CuCo₂O₄/NiFe-layered bimetallic hydroxide core-shell nanoflower sphere arrays. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 930-940. doi: 10.11862/CJIC.20230369
19. [19]
  Yan LIU , Jiaxin GUO , Song YANG , Shixian XU , Yanyan YANG , Zhongliang YU , Xiaogang HAO . Exclusionary recovery of phosphate anions with low concentration from wastewater using a CoNi-layered double hydroxide/graphene electronically controlled separation film. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1775-1783. doi: 10.11862/CJIC.20240043
20. [20]
  Caixia Lin , Zhaojiang Shi , Yi Yu , Jianfeng Yan , Keyin Ye , Yaofeng Yuan . Ideological and Political Design for the Electrochemical Synthesis of Benzoxathiazine Dioxide Experiment. University Chemistry, 2024, 39(2): 61-66. doi: 10.3866/PKU.DXHX202309005

Get Citation

PDF

XML

Metrics

PDF Downloads(471)
Abstract views(670)
HTML views(47)

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