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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2017,Vol.33>> Issue(8)>> 1672-1680     doi: 10.3866/PKU.WHXB201704143         中文摘要
Article
Influences of Cu Content on the Cu/Co/Mn/Al Catalysts Derived from Hydrotalcite-Like Precursors for Higher Alcohols Synthesis via Syngas
LIAO Pei-Yi1,2, ZHANG Chen1,2, ZHANG Li-Jun1, YANG Yan-Zhang2, ZHONG Liang-Shu2, GUO Xiao-Ya1, WANG Hui2, SUN Yu-Han2
1 School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, P. R. China;
2 Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, P. R. China
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A series of Cu/Co/Mn/Al catalysts derived from hydrotalcite precursors with different Cu/Co molar ratios (0, 0.1, 0.5, 1.0, and 2.0) were prepared and used for the synthesis of higher alcohols from syngas. N2 physical adsorption desorption, inductively coupled plasma atomic emission spectrometry (ICP-AES), X-ray diffraction (XRD), scanning electron microscopy (SEM), hydrogen temperature-programmed reduction (H2-TPR), thermogravimetry (TG), and high-resolution transmission electron microscopy (HRTEM) techniques were employed to investigate the physical and chemical properties of the Cu/Co/Mn/Al catalysts. The results show that the optimum Cu content can increase specific surface area, improve reducibility, and form regular layered structure to provide more uniform distribution of active sites, thereby enhancing catalytic activity and alcohol selectivity. When the Cu/Co molar ratio was 0.5, the yield of alcohol and the alcohol selectivity reached the maximum values of 0.071 g·g-1·h-1 and 35.9%, respectively.



Keywords: Higher alcohols synthesis   Layered-double hydroxide   Cu/Co/Mn/Al catalyst   Cu/Co molar ratio   Syngas conversion  
Received: 2016-12-28 Accepted: 2017-03-27 Publication Date (Web): 2017-04-14
Corresponding Authors: WANG Hui, SUN Yu-Han Email: wanghh@sari.ac.cn;yhsun@sari.ac.cn

Fund: The project was supported by the National Natural Science Foundation of China (21403278), China Shenhua Coal to Liquid and Chemical Company Limited, Shanxi Lu'an Coal Corporation Limited, and Shell Global Solutions International B. V.

Cite this article: LIAO Pei-Yi, ZHANG Chen, ZHANG Li-Jun, YANG Yan-Zhang, ZHONG Liang-Shu, GUO Xiao-Ya, WANG Hui, SUN Yu-Han. Influences of Cu Content on the Cu/Co/Mn/Al Catalysts Derived from Hydrotalcite-Like Precursors for Higher Alcohols Synthesis via Syngas[J]. Acta Phys. -Chim. Sin., 2017,33 (8): 1672-1680.    doi: 10.3866/PKU.WHXB201704143

(1) Pan, X. L.; Fan, Z. L.; Chen, W. Nat. Mater. 2007, 6, 507. doi: 10.1038/nmat1916
(2) Spivey, J. J.; Egbebi, A. Chem. Soc. Rev. 2007, 36, 1514. doi: 10.1039/b414039g
(3) Subramani, V.; Gangwal, S. K. Energy Fuels. 2008, 22, 814. doi: 10.1021/ef700411x
(4) Gupta, M.; Smith, M. L. ACS Catal. 2011, 1, 641. doi: 10. 1021/cs2001048
(5) Fang, K. G.; Li, D. B.; Lin, M. G. Catal. Today. 2009, 147, 133. doi: 10.1016/j.cattod.2009.01.038
(6) Choi, Y. M.; Liu, P. J. Am. Chem. Soc. 2009, 131, 13054. doi: 10.1021/jacs.5b12087
(7) Prieto, G.; Concepción, P. J. Catal. 2011, 280, 274. doi: 10.1016/j.jcat.2011.03.025
(8) Yang, N. Y.; Medford, A. J.; Liu, X.Y. J. Am. Chem. Soc. 2016, 138, 3705. doi: 10.1021/jacs.5b12087
(9) Sun, J.; Wan, S. L.; Wang, F. Ind. Eng. Chem. Res. 2015, 54, 7841. doi: 10.1021/acs.iecr.5b01927.
(10) Epling, W. S.; Minahan, D. M. J. Catal. 1998, 175, 175. doi: 10.1006/jcat.1998.2005
(11) Xu, M. T.; Gines, M. J. L.; Hilmen, A. M. J. Catal. 1997, 171, 130. doi: 10.1006/j cat.1997.1777
(12) Xiang, M. L.; Li, D. B.; Li, W. H. Catal. Commun. 2007, 8, 503. doi: 10.1016/j.catcom.2006.08.049
(13) Shou, H.; Ferrari, D. ACS Catal. 2012, 2, 1408. doi: 10.1021/cs300083b
(14) Thao, N. T.; Niaki, M. H. Z. J. Catal. 2007, 245, 348. doi: 10.1016/j.jcat.2006.10.026
(15) Subramanian, N. D.; Balaji, G. Catal. Today. 2009, 147, 100. doi: 10.1016/j.cattod.2009.02.027
(16) Xu, H. Y.; Chu, W.; Deng, S. Y. Acta Phys. -Chim. Sin. 2010, 26, 345. [徐慧远, 储伟, 邓思玉. 物理化学学报, 2010, 26, 345.] doi: 10.3866/PKU.WHXB20100228
(17) Xiao, K.; Qi, X. Z. Catal. Sci. Technol. 2013, 3, 1591. doi: 10.1039/c3cy00063j
(18) Wang, J. J.; Chernavskii, P. A. J. Catal. 2012, 286, 51. doi: 10.1016/j.jcat. 2011.10.012
(19) Yang, Y. Z.; Qi, X. Z.; Wang, X. X. Catal. Today. 2016, 270, 101. doi:10.1016/j.cattod.2015.06.014
(20) Prieto, G. Z.; Beijer, S. Angew. Chem. Int. Ed. 2014, 53, 6397. doi: 10.1002/anie.201402680
(21) Liu, Y. J.; Zuo, Z. J. Fuel. Process. Technol. 2016, 144, 186. doi: 10.1016/j.fuproc.2016.01.005
(22) Xiang, Y. Z.; Chitry, V. J. Am. Chem. Soc. 2013, 135, 7114. doi: 10.1021/ja402512r
(23) Duan, X. Chem. Soc. Rev. 2014, 43, 7040. doi: 10.1039/c4cs00160e
(24) Gao, W.; Zhao, Y. F.; Liu, J. M. Catal. Sci. Technol. 2013, 31, 324. doi: 10.1039/c3cy00025g
(25) Grey, C. P. Science 2008, 321, 113. doi: 10.1126/science. 1157581.
(26) Ma, K. Y.; Cheng, J. P. J. Alloy. Compd. 2016, 679, 277. doi: 10.1016/j.jallcom.2016.04.059
(27) Yuan, Z.; Wang, L.; Wang, J. Appl. Catal. B: Environ. 2011, 101, 431. doi: 10. 1016/j.apcatb.2010.10.013
(28) Xia, S.; Nie, R.; Lu, X. J. Catal. 2012, 296, 1. doi: 10.1016/j.jcat.2012.12.008.
(29) Anton, J.; Nebel, J. Appl. Catal. A: Gen. 2015, 505, 326. doi: 10.1016/j.apcata.2015.07.002
(30) Su, J. J.; Zhang, Z. P. J. Catal. 2016, 336, 94. doi: 10.1016/j.jcat.2016.01.015
(31) Gao, P.; Li, F.; Zhan, H. J. J. Catal. 2013, 298, 51. doi: 10. 1016/j.jcat.2012.10.030
(32) Wang, J. J.; Chernavskii, P. A. J. Catal. 2012 , 286, 51. doi: 10.1016/j.jcat.2011.10.012
(33) Deng, S. Y.; Chu. W. J. Nat. Gas. Chem. 2008, 17, 369
(34) Alejandre. A.; Medina, F.; Salagre, P. Chem. Mater. 1999, 11, 939. doi: 10.1021/cm980500f
(35) Smith, M. L.; Campos. A.; Spivey, J. J. Catal. Today. 2012, 182, 60. doi: 10.1016 /j.cattod.2011.07.026
(36) Frantisek, K.; Tomas, R.; Jana, D. J. Solid State Chem. 2006, 179, 812. doi: 10.1016/j.jssc.2005.12.004
(37) Pei, Y.; Jian, S.; Chen, Y. RSC Adv. 2015, 5, 76330. doi: 10.1039/c5ra10804g
(38) Byoung, K. K.; Dae, S. P.; Yang, S. Y. Catal. Commu. 2012, 24, 90. doi: 10.1016/j.catcom.2012.03.029
(39) Ning, X.; An. Z.; He. J. J. Catal. 2016, 340, 236. doi:10.1016/j.jcat.2016.05.014
(40) Xu, Z. P.; Zeng, H. C. J. Phys. Chem. B. 2000, 104, 10206. doi: 10.1021/jp001963n
(41) Cheng. J.; Yu. J. J.; Wang. X. P. Energy Fuels 2008, 22, 2131. doi: 10.1021/cs200294d
(42) Velu, S.; Sabde, D. P. Chem. Mater. 1998, 10, 3451. doi: 10.1021/cm980185x
(43) Trujillano, R.; Holgado. M. J. Phys. B 2006, 373, 267. doi: 10.1103/Phys.RevB.73.012203
(44) Behrens. M.; Kasatkin. I. Chem. Mater. 2010, 22, 386. doi: 10.1021/cm9029165
(45) Gao, P; Yang, H. J. CO 2Util. 2016, 16, 32. doi: 10.1016/j.jcou.2016.06.001
(46) Cheng, X. F.; Wu, B. S. J. Mol. Catal. A: Chem. 2010, 329, 103. doi: 10.1016/j.molcata.2010.06.024
(47) Laan, G. P. V. Catal. Rev. 1999, 41, 255. doi: 10.1081/CR-100101170
(48) Matsuzaki, T.; Takeuchi, K.; Hanaoka, T. Catal. Today 1996, 28, 251. doi: 10.1016/0920-5861(95)00245-6

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