容碳的SiW20-Al/Zr10催化剂用于甘油脱水制丙烯醛

doi:10.1016/S1872-2067(17)62891-2

摘要/Abstract

摘要：

将一系列负载型硅钨酸催化剂用于甘油脱水制丙烯醛反应中.表征结果表明，最终所得催化剂具有高的热稳定性、大的孔径、强的L酸位和大的比表面积.X射线光电子能谱中清晰地出现归属于W（W 4f=35.8 eV），Al（Al 2p=74.9 eV）和Zr（Zr 3d=182.8 eV）元素的谱峰.在SiW₂₀-Al/Zr₁₀催化剂上丙烯醛选择性最高，为87.3%，此时甘油转化率为97%.由于高浓度L酸位的存在，显著降低了催化剂表面积碳量，因而该催化剂即使反应40 h之后仍具有较高地催化生成丙烯醛的活性和选择性.响应面方法表明，在以下优化条件下反应甘油转化率和丙烯醛选择性分别达87.7%和97.0%：催化剂用量0.5 wt%，进料甘油浓度10 wt%，反应温度300 ℃.传质限制评估结果显示，当颗粒尺寸d_P<20 μm时，反应不存在内外扩散限制.综上可见，强L酸催化剂有望用于甘油脱水制丙烯醛反应中.

关键词: 甘油, 脱水, 丙烯醛, 多相催化, 杂多酸

Abstract:

Glycerol dehydration to acrolein over a series of supported silicotungstic acid catalysts (SiW_x-Al/Zr_y) was investigated. Characterization results showed that the final catalyst had high thermal stability, a large pore diameter, strong Lewis acidic sites, and a large specific surface area. X-ray photoelectron survey spectra clearly showed peaks attributable to W (W 4f = 35.8 eV), Al₂O₃(Al 2p = 74.9 eV), and ZrO₂ (Zr 3d = 182.8 eV). The highest acrolein selectivity achieved was 87.3% at 97% glycerol conversion over the SiW₂₀-Al/Zr₁₀ catalyst. The prepared catalysts were highly active and selective for acrolein formation even after 40 h because of the presence of high concentrations of Lewis acidic sites, which significantly reduced the amount of coke on the catalyst surface. Response surface methodology optimization showed that 87.7% acrolein selectivity at 97.0% glycerol conversion could be obtained under the following optimal reaction conditions: 0.5 wt% catalyst, reaction temperature 300 ℃, and feed glycerol concentration 10 wt%. Evaluation of a mass-transfer-limited regime showed the absence of internal and external diffusions over pellets of diameter d_P<20 μm. These results show that glycerol dehydration over a strong Lewis acid catalyst is a promising method for acrolein production.

Key words: Glycerol, Dehydration, Acrolein, Heterogeneous catalysis, Heteropoly acid

Amin Talebian-Kiakalaieh, Nor Aishah Saidina Amin. 容碳的SiW₂₀-Al/Zr₁₀催化剂用于甘油脱水制丙烯醛[J]. 催化学报, 2017, 38(10): 1697-1710.

Amin Talebian-Kiakalaieh, Nor Aishah Saidina Amin. Coke-tolerant SiW₂₀-Al/Zr₁₀ catalyst for glycerol dehydration to acrolein[J]. Chinese Journal of Catalysis, 2017, 38(10): 1697-1710.

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参考文献

[1] D. Yun, T. Y. Kim, D. S. Park, Y. S. Yun, J. W. Han, J. Yi, ChemSusChem, 2014, 7, 2193-2201.
[2] K. N. Papageridis, G. Siakavelas, N. D. Charisiou, D. G. Avraam, L. Tzounis, K. Kousi, M. A. Goula, Fuel Process. Technol., 2016, 152, 156-175.
[3] T. Jedsukontorn, V. Meeyoo, N. Saito, M. Hunsom, Chin. J. Catal., 2016, 37, 1975-1081.
[4] S. Lopez-Pedrajas, R. Estevez, R. Navarro, D. Luna, F. M. Bautista, J. Mol. Catal. A, 2016, 421, 92-101.
[5] M. R. Nanda, Y. Zhang, Z. Yuan, W. Qin, H. S. Ghaziaskar, C. Xu, Renew. Sustain Energy Rev., 2016, 56, 1022-1031.
[6] A. Chieregato, M. D. Soriano, F. Basile, G. Liosi, S. Zamaro, P. Concepcion, F. Cavani, J. M. Lopez Nieto, Appl. Cat. B, 2014, 150, 151-37.
[7] A. Galadima, O. Muraza, J. Taiwan. Inst. Chem. Eng., 2016, 67, 29-44.
[8] L. T. Phi Trinh, J. W. Lee, H. J. Lee, Biomass Bioenergy, 2016, 94, 39-45.
[9] G. D. Yadav, R. V. Sharma, S. O. Katole, Ind. Eng. Chem. Res., 2013, 52, 10133-10144.
[10] M. A. Goula, N. D. Charisiou, K. N. Papageridis, G. Siakavelas, Chin. J. Catal., 2016, 37, 1949-1965.
[11] J. Y. Hu, X. Y. Liu, B. Wang, Y. Pei, K. N. Fan, Chin. J. Catal., 2012, 33, 1266-1275.
[12] J. M. Thomas, ChemSusChem, 2014, 7, 1801-1832.
[13] G. W. Keulks, L. D. Krenzke, T. M. Notermann, Adv. Catal., 1978, 27, 183-225.
[14] G. Srinivasa Rao, N. Pethan Rajan, M. Hari Sekhar, S. Ammaji, K. V. R. Chary, J. Mol. Catal. A, 2014, 395, 486-493.
[15] R. Liu, T. F. Wang, C. Liu, Y. Lin, Chin. J. Catal., 2013, 34, 2174-2182.
[16] L. L. Ning, Y. J. Ding, W. M. Chew, L. F. Gong, R. H. Lin, Y. Lu, Q. Xin, Chin. J. Catal., 2008, 29, 212-214.
[17] B. Katryniok, S. Paul, M. Capron, C. Lancelot, V. Bellere-Beca, P. Rey, F. Dumeignil, Green Chem., 2010, 12, 1922-1925.
[18] C. S. Carrico, F. T. Cruz, M. B. dos Santos, D. S. Oliveira, H. O. Pastore, H. M. C. Andrade, A. J. S. Mascarenhas, J. Catal., 2016, 334, 34-41.
[19] L. G. Possato, R. N. Diniz, T. Garetto, S. H. Pulcinelli, C. V. Santilli, L. Martins, J. Catal., 2013, 300, 102-112.
[20] L. H. Vieira, K. T. G. Carvalho, E. A. Urquieta-Gonzalez, S. H. Pulcinelli, C. V. Santilli, L. Martins, J. Mol. Catal. A, 2016, 422, 148-157.
[21] H. M. Gan, X. G. Zhao, B. N. Song, L. Guo, R. Zhang, C. Chen, J. Z. Chen, W. W. Zhu, Z. S. Hou, Chin. J. Catal., 2014, 35, 1148-1156.
[22] A. S. Ivanova, E. V. Korneeva, V. M. Bondareva, T. S. Glazneva, J. Mol. Catal. A, 2015, 408, 98-106.
[23] L. Q. Shen, H. B. Yin, A. L. Wang, X. F. Lu, C. H. Zhang, F. Chen, Y. T. Wang, H. J. Chen, J. Ind. Eng. Chem., 2014, 20, 759-766.
[24] A. Alhanash, E. F. Kozhevnikova, I. V. Kozhevnikov, Appl. Catal. A, 2010, 378, 11-18.
[25] M. Misono, Chem. Commun., 2001, 1141-1152.
[26] H. Atia, U. Armbruster, A. Martin, J. Catal., 2008, 258, 71-82.
[27] M. Dalil. M. Edake, C. Sudeau, J. L. Dubios, G. S. Patience. Appl. Catal. A, 2016, 522, 80-89.
[28] S. B. A. Hamid, N. A. Daud, D. D. Suppiah, W. A. Yehya, P. Sudarsanam, S. K. Bhargava, Polyhedron, 2016, 120, 154-161.
[29] D. Stosic, S. Bennici, S. Sirotin, C. Calais, J. L. Couturier, J. L. Dubois, A. Travert, A. Auroux, Appl. Catal. A, 2012, 447-448, 124-134.
[30] Y. L. Gu, N. Y. Cui, Q. J. Yu, C. Y. Li, Q. K. Cui, Appl. Catal. A, 2012, 429-430, 9-16.
[31] D. Stosic, S. Bennici, J. L. Couturiei, J. L. Dubois, A. Auroux, Catal. Commun., 2012, 17, 23-28.
[32] M. H. Haider, N. F. Dummer, D. Zhang, P. Miedziak, T. E. Davies, S. H. Taylor, D. J. Willock, D. W. Knight, D. Chadwick, G. J. Hutchings, J. Catal., 2012, 286, 206-213.
[33] A. Talebian-Kiakalaieh, N. A. S. Amin, Z. Y. Zakaria, J. Ind. Eng. Chem., 2016, 34, 300-312.
[34] A. Talebian-Kiakalaieh, N. A. S. Amin, Catal. Today, 2015, 256, 315-324.
[35] S. H. Zhu, Y. L. Zhu, S. L. Hao, H. Y. Zheng, T. Mo, Y. W. Li, Green Chem., 2012, 14, 2607-2616.
[36] S. H. Zhu, Y. N. Qiu, Y. L. Zhu, S. L. Hao, H. Y. Zheng, Y. W. Li, Catal. Today, 2013, 212, 120-126.
[37] S. Erfle, U. Armbruster, U. Bentrup, A. Martin, A. Bruckner, Appl. Catal. A, 2011, 391, 102-109.
[38] M. G. Kulkarni, R. Gopinath, L. C. Meher, A. K. Dalai, Green Chem., 2006, 8, 1056-1062.
[39] L. Q. Shen, Y. H. Feng, H. B. Yin, A. L. Wang, L. B. Yu, T. S. Jiang, Y. T. Shen, Z. A. Wu, J. Ind. Eng. Chem., 2011, 17, 484-492.
[40] Z. Obali, T. Dogu, Chem. Eng. J., 2008, 138, 548-555.
[41] B. M. Reddy, P. M. Sreekanth, Y. Yamada, T. Kobayashi, J. Mol. Catal. A, 2005, 227, 81-89.
[42] K. M. Reddy, N. S. Babu, P. S. S. Prasad, N. ingaiah, Catal. Commun., 2008, 9, 2525-2531.
[43] N. K. Nag, J. Phys. Chem., 1987, 91, 2324-2327.
[44] L. R. Pizzio, M. N. Blanco. Microporous Mesporous Mater., 2007, 103, 40-47.
[45] C. S. Carrico, F. T. Cruz, M. B. Santos, H. O. Pastore, H. M. C. Andrade, A. J. M. Mascarenhas, Microporous Mesporous Mater, 2013, 181, 74-82.
[46] A. A. Babad-Zakhryapin, N. S. Gorunov, Izv. AN SSSR, Seri. Khim., 1963, 14-16.
[47] Y. Leng, J. Wang, P. P. Jiang. Catal. Commun., 2012, 27, 101-104.
[48] P. Kar, B. G. Misra, Chem. Eng. J., 2013, 223, 647-656.
[49] S. H. Zhu, Z. Q. Gao, Y. L. Zhu, Y. F. Zhu, X. M. Xiang, C. X. Hu, Y. W. Li, Appl. Catal. B, 2013, 140-141, 60-67.
[50] G. D. Yadav, D. P. Tekale, Catal. Today, 2014, 237, 54-61.
[51] J. A. Cecilia, C. Garcia-Sancho, J. M. Merida-Robles, J. Santamaria Goczalez, R. Moreno-Tost, P. Maireles-Torres, Appl. Catal. A, 2016, 516, 30-40.
[52] W. Yan, G. J. Suppes, Ind. Eng. Chem. Res., 2009, 48, 3279-3283.
[53] W. Suprun, M. Lutecki, T. Haber, H. Papp, J. Mol. Catal. A, 2009, 309, 71-78.
[54] L. M. Cheng, X. P. Ye, Catal. Lett., 2009, 130, 100-107.
[55] E. Tsukuda, S. Sato, R. Takahashi, T. Sodesawa, Catal. Commun., 2007, 8, 1349-1353.
[56] I. V. Kozhevnikov, Chem. Rev., 1998, 98, 171-198.
[57] P. G. Menon, J. Mol. Catal., 1990, 59, 207-220.
[58] Y. C. Yang, H. S. Weng, J. Mol. Catal A, 2009, 304, 65-70.
[59] A. Talebian-Kiakalaieh, N. A. S. Amin, J. Taiwan Inst. Chem. Eng., 2016, 59, 11-17.
[60] M. M. Ballari, R. Brandi, O. Alfano, A. Cassano, Chem. Eng. J., 2008, 136, 242-255.
[61] T. L. Ma, Z. Yun, W. Xu, L. G. Chen, L. Li, J. F. Ding, R. Shao, Chem. Eng. J., 2016, 294, 343-352.

容碳的SiW₂₀-Al/Zr₁₀催化剂用于甘油脱水制丙烯醛

Coke-tolerant SiW₂₀-Al/Zr₁₀ catalyst for glycerol dehydration to acrolein

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