FeMn、FeMnNa和FeMnK催化剂上合成气制低碳烯烃的比较

doi:10.3866/PKU.WHXB201408051

Acta Phys. -Chim. Sin. ›› 2014, Vol. 30 ›› Issue (10): 1932-1940.doi: 10.3866/PKU.WHXB201408051

• CATALYSIS AND SURFACE SCIENCE • Previous Articles Next Articles

Comparison of FeMn, FeMnNa and FeMnK Catalysts for the Preparation of Light Olefins from Syngas

LI Jiang-Bing^1,2, MA Hong-Fang¹, ZHANG Hai-Tao¹, SUN Qi-Wen³, YING Wei-Yong¹, FANG Ding-Ye¹

1. State Key Laboratory of Chemical Engineering, Engineering Research Center of Large Scale Reactor Engineering and Technology of the Ministry of Education, East China University of Science and Technology, Shanghai 200237, P. R. China;
2. Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832003, The Xinjiang Uygur Autonomous Region, P. R. China;
3. State Key Laboratory of Coal Liquefaction and Coal Chemical Technology, Shanghai 201203, P. R. China

Received:2014-06-20 Revised:2014-08-04 Published:2014-09-30
Contact: YING Wei-Yong E-mail:wying@ecust.edu.cn
Supported by:
The project was supported by the Major State Basic Research Program of China (2010CB736203) and National High-Tech R&D Program of China (2011AA05A204).

Abstract

Abstract:

The influence of sodium and potassium promoters on the structure and reaction behavior of an FeMn catalyst toward light olefin synthesis from syngas was investigated by N₂ adsorption, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), H₂ temperature-programmed reduction (H₂-TPR), CO/CO₂ temperature-programmed desorption (CO/CO₂-TPD), Mössbauer spectroscopy (MES) and CO+H₂ reaction. We found that an increase in manganese improves the dispersion of the active Fe component and light olefin selectivity; however, excessive enrichment with the Mn promoter on the catalyst surface suppresses CO conversion. Potassium and sodium inhibit the reduction of the catalyst in H₂ and improve the adsorption of CO₂ and CO because of the enhanced surface basicity of the catalysts. After reduction with syngas (n_H₂/n_CO=20) and reaction with syngas (n_H₂/n_CO=3.5), the analysis of the bulk structure was compared with those of the FeMn, FeMnNa, and FeMnK catalysts. The results show that FeC_x is found in relatively high levels in the FeMnK catalysts because of the stronger alkalinity and adsorbability of CO. However, Fischer-Tropsch synthesis (FTS) results indicate that sodium and potassium improved the selectivity toward light olefins. The best catalytic performance was achieved by the FeMnNa catalyst. Its CO conversion and light olefins selectivity were 96.2% and 30.5% (molar fraction), respectively.

Key words: Light olefin, Fischer-Tropsch synthesis, FeMn catalyst, Sodium promoter, Potassium promoter

LI Jiang-Bing, MA Hong-Fang, ZHANG Hai-Tao, SUN Qi-Wen, YING Wei-Yong, FANG Ding-Ye. Comparison of FeMn, FeMnNa and FeMnK Catalysts for the Preparation of Light Olefins from Syngas[J]. Acta Phys. -Chim. Sin. 2014, 30(10), 1932-1940. doi: 10.3866/PKU.WHXB201408051

References

(1) Janardanarao, M. Ind. Eng. Chem. Res. 1990, 29, 1735. doi: 10.1021/ie00105a001
(2) Ma,W. P.; Ding, Y. J.; Luo, H. Y.; Lin, P. Z.; Lin, L.W. Chinese Journal of Catalysis 2001, 22, 279. [马文平, 丁云杰, 罗洪原, 林培滋, 林励吾. 催化学报, 2001, 22, 279.] (3) Mirzaei, A. A.; Habibpour, R.; Kashi, E. Appl. Catal. A-Gen. 2005, 296, 222. doi: 10.1016/j.apcata.2005.08.033
(4) Dry, M. E.; Shingles, T.; Botha, C. S. V. H. J. Catal. 1970, 17, 341. doi: 10.1016/0021-9517(70)90109-0
(5) Lohitharn, N.; Goodwin, J. G., Jr. J. Catal. 2008, 260, 7. doi: 10.1016/j.jcat.2008.08.011
(6) Botes, F. G.; Govender, N. S. Energ. Fuel. 2007, 21, 3095. doi: 10.1021/ef7003464
(7) Ngantsoue-Hoc,W.; Zhang, Y. Q.; O’Brien, R. J.; Luo, M.; Davis, B. H. Appl. Catal. A-Gen. 2002, 236, 77. doi: 10.1016/S0926-860X(02)00278-8
(8) Wang, C.; Zhao, H. B.;Wang, H.; Liu, L. T.; Xiao, C. X.; Ma, D. Catal. Today 2012, 183, 143. doi: 10.1016/j.cattod.2011.10.020
(9) Dry, M. E.; Oosthuizen, G. J. J. Catal. 1968, 11, 18. doi: 10.1016/0021-9517(68)90004-3
(10) Yang, Y.; Xiang, H.W.; Xu, Y. Y.; Li, Y.W. Appl. Catal. A-Gen. 2004, 266, 181. doi: 10.1016/j.apcata.2004.02.018
(11) An, X.;Wu, B. S.; Hou,W. J.;Wan, H. J.; Tao, Z. C.; Li, T. Z.; Zhang, Z. X.; Xiang, H.W.; Li, Y.W.; Xu, B.; Yi, F. J. Mol. Catal. A: Chem. 2007, 263, 266. doi: 10.1016/j.molcata.2006.09.003
(12) Abbot, J.; Clark, N. J.; Baker, B. G. Appl. Catal. A-Gen. 1986, 26, 141. doi: 10.1016/S0166-9834(00)82547-6
(13) Galvis, H. M. T.; Bitter, J. H.; Khare, C. B.; Ruitenbeek, M.; Dugulan, A. I.; Jong, K. P. D. Science 2012, 335, 835. doi: 10.1126/science.1215614
(14) Zhang, J. L.; Ma, L. H.; Fan, S. B.; Zhao, T. S.; Sun, Y. H. Fuel2013, 109, 116. doi: 10.1016/j.fuel.2012.12.081
(15) Qian,W. X.; Zhang, H. T.; Ying,W. Y.; Fang, D. Y. J. Nat. Gas Chem. 2011, 20, 389. doi: 10.1016/S1003-9953(10)60203-4
(16) Herranz, T.; Rojas, S.; Pérez-Alonso, F. J.; Ojeda, M.; Terreros, P.; Fierro, J. L. G. Appl. Catal. A-Gen. 2006, 311, 66. doi: 10.1016/j.apcata.2006.06.007
(17) Tao, Z. C.; Yang, Y.;Wan, H. J.; Li, T. Z.; An, X.; Xiang, H.W.; Li, Y.W. Catal. Lett. 2007, 114, 161. doi: 10.1007/s10562-007-9060-6
(18) Cao, C. J.; Liu, X. G.; Ju, X. R.; Chen, X. R. Acta Phys. -Chim. Sin. 2013, 29, 2475. [曹崇江, 刘晓庚, 鞠兴荣, 陈晓荣. 物理化学学报, 2013, 29, 2475.] doi: 10.3866/PKU.WHXB201310101
(19) Leith, I. R.; Howden, M. G. Appl. Catal. 1988, 37, 75. doi: 10.1016/S0166-9834(00)80752-6
(20) An, X.;Wu, B. S.;Wan, H. J.; Li, T. Z.; Tao, Z. C.; Xiang, H. W.; Li, Y.W. Catal. Commun. 2007, 8, 1957. doi: 10.1016/j.catcom.2007.03.016
(21) Wang, H. L.; Yang, Y.; Xu, J.;Wang, H.; Ding, M. Y.; Li, Y.W. J. Mol. Catal. A: Chem. 2010, 326, 29. doi: 10.1016/j.molcata.2010.04.009
(22) Motjope, T. R.; Dlamini, H. T.; Hearne, G. R.; Coville, N. J. Catal. Today 2002, 71, 335. doi: 10.1016/S0920-5861(01)00460-6
(23) Yang, Y.; Xiang, H.W.; Tian, L.;Wang, H.; Zhang, C. H.; Tao, Z. C.; Xu, Y. Y.; Zhong, B.; Li, Y.W. Appl. Catal. A-Gen. 2005, 284, 105. doi: 10.1016/j.apcata.2005.01.025
(24) Jung, H.; Thomson,W. J. J. Catal. 1992, 134, 654. doi: 10.1016/0021-9517(92)90350-Q
(25) Tao, Z. C.; Yang, Y.; Zhang, C. H.; Li, T. Z.;Wang, J. H.;Wan, H. J.; Xiang, H.W.; Li, Y.W. Catal. Commun. 2006, 7, 1061. (26) Dry, R. E.; Shingles, T.; Bboshoff, L. J.; Oosthuizen, G. J. J. Catal. 1969, 15, 190. doi: 10.1016/0021-9517(69)90023-2
(27) Miller, D. G.; Moskovits, M. The Journal of Physical Chemistry 1988, 92, 6081. doi: 10.1021/j100332a047
(28) Zhang, X. J.; Liu, Y.; Liu, G. Q.; Tao, K.; Jin, Q.; Meng, F. Z.; Wang, D.; Tsubaki, N. Fuel 2012, 92, 122. doi: 10.1016/j.fuel.2011.07.041

[1]	Xueling Lang, Shutao Lei, Bolong Li, Xiaohong Li, Bing Ma, Chen Zhao. Approaches for the Synthesis of High-Melting Waxes: A Review [J]. Acta Phys. -Chim. Sin., 2022, 38(10): 2204045-.
[2]	XU Ke, CHENG Yi, SUN Bo, PEI Yan, YAN Shi-Run, QIAO Ming-Hua, ZHANG Xiao-Xin, ZONG Bao-Ning. Fischer-Tropsch Synthesis over Skeletal Co@HZSM-5 Core-Shell Catalysts [J]. Acta Phys. -Chim. Sin., 2015, 31(6): 1137-1144.
[3]	CAO Chong-Jiang, LIU Xiao-Geng, JU Xing-Rong, CHEN Xiao-Rong. Design, Synthesis and Characterization of Pt/Fe Bimetallic Fischer-Tropsch Catalyst [J]. Acta Phys. -Chim. Sin., 2013, 29(11): 2475-2480.
[4]	YAO Fang-Fang, WU Bao-Shan, ZHOU Li-Ping, GAO Jun-Hu, LI Ying, LI Yong-Wang. Effect of Alcohol Addition on Fischer-Tropsch Synthesis over Cobalt-Based Catalysts [J]. Acta Phys. -Chim. Sin., 2013, 29(05): 1063-1072.
[5]	HU Xiao-Yan, LI Chun-Yi, YANG Chao-He. Catalytic Cracking Behavior of n-Heptane over HZSM-5 Catalyst [J]. Acta Phys. -Chim. Sin., 2010, 26(12): 3291-3298.
[6]	WAN Hai-Jun; WU Bao-Shan; AN Xia; TAO Zhi-Chao; LI Ting-Zhen; XIANG Hong-Wei; LI Yong-Wang. Structural Properties, Reduction and Carburization Behaviors of Fe/Cu/K/Al₂O₃ Catalyst for Fischer-Tropsch Synthesis [J]. Acta Phys. -Chim. Sin., 2007, 23(08): 1151-1156.
[7]	ZHANG Cheng-Hua;YANG Yong;TAO Zhi-Chao;LI Ting-Zhen;WAN Hai-Jun;XIANG Hong-Wei;LI Yong-Wang . Effects of Cu and K on Co-precipitated FeMn/SiO2 Catalysts for Fischer-Tropsch Synthesis [J]. Acta Phys. -Chim. Sin., 2006, 22(11): 1310-1316.
[8]	CHANG Jie; TENG Bo-tao; XIANG Hong-wei; LI Yong-wang; SUN Yu-han. UBI-QEP Analysis for the Mechanism of Fischer-Tropsch Synthesis [J]. Acta Phys. -Chim. Sin., 2005, 21(11): 1223-1228.
[9]	Zhu Yi-Xiang, Chai Yun-Zhou, Liu Zheng-Yang, Huang Su-Mei, Cheng Xiang-Ming. XRD Characterization of Interaction between Potassium Promoter and Magnetite [J]. Acta Phys. -Chim. Sin., 2000, 16(02): 126-132.
[10]	Chen Kai-Dong,Yan Qi-Jie. Influence of Ceria on the Structure and Catalytic Property of F-T Synthesis Fe/ZrO₂ Catalysts [J]. Acta Phys. -Chim. Sin., 1996, 12(11): 990-994.
[11]	Bian Guo-Zhu; Jiang Ming; Fu Yi-Lu; Ji Ming-Rong. Chemical States and Composition of the Surface Species of K-MoO₃/γ-Al₂O₃ Catalysts [J]. Acta Phys. -Chim. Sin., 1993, 9(05): 650-656.

Comparison of FeMn, FeMnNa and FeMnK Catalysts for the Preparation of Light Olefins from Syngas

PDF

Like

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 11

Metrics

Recommended 0