χ-氧化铝的添加对纯的和修饰的γ-氧化铝上H2S氧化反应性能的影响

doi:10.1016/S1872-2067(18)63016-5

摘要/Abstract

摘要：

考察了γ-Al₂O₃，（γ+χ）-Al₂O₃和α-Al₂O₃的结构性质和酸性对其催化H₂S直接氧化反应性能（活性、选择性和稳定性）的影响.采用红外光谱（FTIR）与氨-程序升温脱附（NH₃-TPD）方法对氧化铝作用下H₂S转化为S的反应性能与其酸性进行了比较.结果显示，H₂S吸附主要发生在弱Lewis酸位.含有χ相和/或Mg²⁺修饰的γ-Al₂O₃样品具有更高浓度的弱Lewis酸位，并表现出更高的催化活性.当氧化铝样品用硫酸溶液处理后，表现出强Lewis酸位性质，且Lewis酸位点数量显著下降.而当用HCl对氧化铝进行修饰时，其对Lewis酸位强度的影响很小，保持着弱Lewis酸位的性质，且其Lewis酸位数量与未修饰的样品相比增加了二倍，但处理过的样品中含有Al-Cl键.用硫酸盐和氯离子修饰过的氧化铝样品在H₂S氧化反应中的催化性能均较低.

关键词: 氧化铝, χ-Al₂O₃, 硫化氢氧化, 酸性质, 路易斯酸位, 红外光谱, 氨-程序升温脱附

Abstract:

The influence of the textural and acidic properties of γ-Al₂O₃, (γ+χ)-Al₂O₃, and α-Al₂O₃ on the catalytic activity, selectivity, and stability of direct H₂S oxidation has been studied. A comparison of the H₂S-to-S conversion effectiveness of aluminas with their acidic properties (identified by Fourier transform infrared spectroscopy and temperature programmed desorption of NH₃) shows that H₂S adsorption occurs predominantly on weak Lewis acid sites (LAS). γ-Alumina samples containing a χ-phase and/or modified Mg²⁺ ions have a greater concentration of weak LAS and exhibit greater catalytic activity. When alumina is treated with a sulfuric acid solution, strong LAS appear and the number of LAS decreases significantly. Modification of alumina with hydrochloric acid has a limited effect on LAS strength. Weak LAS are retained and double in number compared to that present in the unmodified alumina, but the treated sample has Al-Cl bonds. Alumina samples modified by sulfate and chloride anions exhibit poor catalytic activity in H₂S oxidation.

Key words: Alumina, χ-Al₂O₃, Hydrogen sulfide oxidation, Acidic property, Lewis acid sites, Fourier transform infrared spectroscopy, NH₃-temperature programmed desorption

Svetlana A. Yashnik, Vadim V. Kuznetsov, Zinfer R. Ismagilov. χ-氧化铝的添加对纯的和修饰的γ-氧化铝上H₂S氧化反应性能的影响[J]. 催化学报, 2018, 39(2): 258-274.

Svetlana A. Yashnik, Vadim V. Kuznetsov, Zinfer R. Ismagilov. Effect of χ-alumina addition on H₂S oxidation properties of pure and modified γ-alumina[J]. Chinese Journal of Catalysis, 2018, 39(2): 258-274.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(18)63016-5

https://www.cjcatal.com/CN/Y2018/V39/I2/258

参考文献

[1] A. Melchor, E. Garbowski, M. V. Mathieu, M. Primet, J. Chem. Soc., Faraday Trans. 1, 1986, 82, 1893-1901.
[2] F. Arena, F. Frusterl, N. Mondeller, N. Giordano, A. Parmaliana, J. Chem. Soc., Faraday Trans. 1992, 88, 3353-3356.
[3] B. Ducourty, G. Szabo, J. P. Dath, J. P. Gilson, J. M. Goupil, D. Cornet, Appl. Catal. A, 2004, 269, 203-214.
[4] G. Clet, J. M. Goupil, G. Szabo, D. Cornet, J. Mol. Catal. A, 1999, 148, 253-264.
[5] G. Clet, J. M. Goupil, G. Szabo, D. Cornet, Appl. Catal. A, 2000, 202, 37-46.
[6] R. S. Drago, E. E. Getty, J. Am. Chem. Soc., 1988, 110, 3311-3312.
[7] J. Thomson, G. Webb, J. M. Winfield, J. Mol. Catal., 1991, 68, 347-354.
[8] S. V. Tsybulya, G. N. Kryukova, Physical Review B, 2008, 77, 024112/1-024112/13.
[9] S. A. Yashnik, A. V. Ishchenko, L. S. Dovlitova, Z. R. Ismagilov, Top. Catal., 2017, 60, 52-72.
[10] Z. R. Ismagilov, M. A. Kerzhentsev, Catal. Rev. Sci. Eng., 1990, 32, 51-102.
[11] Z. R. Ismagilov, N. M. Dobrynkin, S. R. Khairulin, F. R. Ismagilov, Oil & Gas J., 1994, 7, 81-82.
[12] B. W. Gamson, R. H. Elkins, Chem. Eng. Progr., 1953, 49, 203-215.
[13] J. Klein, K. D. Henning, Fuel, 1984, 63, 1064-1067.
[14] Z. L. Pan, H. S. Weng, H. Y. Feng, J. M. Smith, AIChE J., 1984, 30, 1021-1025.
[15] A. B. Verver, W. P. M. Van Swaaij, Appl. Catal., 1985, 14, 185-206.
[16] R. J. A. M. Terorde, P. J. Van den Brink, L. M. Visser, A. J. van Dillen, J. W. Geus, Catal. Today, 1993, 17, 217-224.
[17] V. I. Marshneva, V. V. Mokrinskii, Kinet. Catal., 1988, 29, 989-993.
[18] M. V. Batygina, N. M. Dobrynkin, O. A. Kirichenko, S. R. Khairulin, Z. R. Ismagilov, React. Kinet. Catal. Lett., 1992, 48, 55-63.
[19] K. T. Li, C. S. Yen, N. S. Shyu, Appl. Catal. A, 1997, 156, 117-123.
[20] Z. R. Ismagilov, M. A. Kerzhentsev, S. R. Khairulin, V. V. Kuznetsov, Chem. Sustainable Development, 1999, 7, 375-381.
[21] J. H. Uhm, M. Y. Shin, J. Zhidong, J. S. Chung, Appl. Catal. B, 1999, 22, 293-303.
[22] E. Laperdrix, G. Costentin, O. Saur, J. C. Lavalley, C. Nedez, S. Sav-in-Pocet, J. Nougayrede, J. Catal., 2000, 189, 63-69.
[23] N. Keller, C. Pham-Huu, M. J. Ledoux, Appl. Catal. A, 2001, 217, 205-217.
[24] S. Yasyerlia, G. Dogua, I. Ara, T. Dogu, Chem. Eng. Sci., 2004, 59, 4001-4009.
[25] P. Nguyen, D. Edouard, J. M. Nhut, M. J. Ledoux, C. Pham, C. Pham-Huu, Appl. Catal. B, 2007, 76, 300-310.
[26] M. D. Soriano, J. Jimenez-Jimenez, P. Concepcion, A. Jimenez-Lopez, E. Rodr?guez-Castellon, J. M. Lopez Nieto, Appl. Catal. B, 2009, 92, 271-279.
[27] M. Leon, J. Jimenez-Jimenez, A. Jimenez-Lopez, E. Rodr?guez-Castellon, D. Soriano, J. M. Lopez Nieto, Solid State Sci., 2010, 12, 996-1001.
[28] V. Palma, D. Barba, P. Ciambelli, Chem. Eng. Trans., 2012, 29, 631-636.
[29] X. Zhang, G. Y. Dou, Z. Wang, L. Li, Y. F. Wang, H. L. Wang, Z. P. Hao. J. Hazard. Mater., 2013, 260, 104-111.
[30] A. Reyes-Carmona, D. Soriano, J. M. Lopez Nieto, D. J. Jones, J. Jimenez-Jimenez, A. Jimenez-Lopez, E. Rodriguez-Castellon, Catal. Today, 2013, 210, 117-123.
[31] V. Palma, D. Barba, Int. J. Hydrogen Energy, 2014, 39, 21524-21530.
[32] M. D. Soriano, J. A. Cecilia, A. Natoli, J. Jimenez-Jimenez, J. M. Lopez Nieto, E. Rodriguez-Castellon, Catal. Today, 2015, 254, 36-42.
[33] N. A. Koryabkina, Z. R. Ismagilov, R. A. Shkrabina, E. M. Moroz, V. A. Ushakov, Appl. Catal., 1991, 72, 63-69.
[34] P. H. Berben, A. Scholten, M. K. Titulaer, N. Brahma, W. J. J. van der Wal, J. W. Geus, Stud. Surf. Sci. Catal., 1987, 34, 303-316.
[35] P. J. Van den Brink, Study of the reaction of hydrogen sulfide oxidation on vanadia catalysts, Ph. D Thesis, University of Utrecht, Utrecht, The Netherlands, 1992.
[36] M. N. Shepeleva, R. A. Shkrabina, Z. R. Ismagilov, Technol. Today, 1990, 3, 150-162.
[37] Z. R. Ismagilov, R. A. Shkrabina, N. A. Koryabkina, Catal. Today, 1999, 47, 51-71.
[38] E. Paukshtis, R. I. Soltanov, E. N. Yurchenko, React. Kinet. Catal. Lett., 1981, 16, 93-96.
[39] R. I. Soltanov, E. A. Paukshtis, E. N. Yurchenko, Kinet. Catal., 1982, 23, 135-141.
[40] E. A. Paukshtis, Infrared Spectroscopy of Heterogeneous Acid-Base Catalysis (in Russian), 1992, Nauka, Novosibirsk.
[41] E. Paukshtis, P. I. Soltanov, E. N. Yurchenko, K. Iratova, Collection Czechoslovak Chem. Commun., 1982, 47, 2044-2060.
[42] E. Baumgarten, R. Wagner, C. Lentes-Wagner, Fresenius Z. Anal. Chem., 1989, 334, 246-251.
[43] G. Della Gatta, B. Fubini, G. Ghiotti, C. Morterra, J. Catal., 1976, 43, 90-98.
[44] A. Zecchina, E. Escalona Platero, C. Otero Arean, J. Catal., 1987, 107, 244-247.
[45] G. Busca, V. Lorenzelli, V. Sanchez Escribano, R. Guidetti, J. Catal., 1991, 131, 167-177.
[46] H. Knözinger, P. Ratnasamy, Catal. Rev. Sci. Eng., 1978, 17, 31-70.
[47] M. Digne, P. Sautet, P. Raybaud, P. Euzen, H. Toulhoat, J. Catal., 2002, 211, 1-5
[48] E. V. Kul'ko, A. S. Ivanova, A. A. Budneva, E. A. Paukshtis, Kinet. Catal., 2005, 46, 132-137.
[49] T. Montanari, L. Castoldi, L. Lietti, G, Busca, Appl. Catal. A, 2011, 400, 61-69.
[50] V. V. Yuschenko, Russian Journal of Physical Chemistry A, 1997, 71, 628-632.
[51] R. H. Perry, D. W. Green, J. O. Malonay (Eds.), Perry's Chemical Engineering Handbook, 7th Edition, McGraw-Hill Companies, New York, 1997, pp. 2-7.
[52] M. Yu. Smirnova, G. A. Urguntsev, A. B. Ayupov, A. A. Vedyagin, G. V. Echevsky. Appl. Catal. A, 2008, 344, 107-113.
[53] S. A. Yashnik, Z. R. Ismagilov, I. V. Koptyug, I. P. Andrievskaya, A. A. Matveev, J. A. Moulijn, Catal. Today, 2005, 105, 507-515.
[54] S. A. Yashnik, I. P. Andrievskaya, O. V. Pashke, Z. R. Ismagilov, J. A. Moulijn, Catal. Ind., 2007, 1, 35-46.
[55] O. Saur, M. Bensitel, A. B. M. Saad, J. C. Lavalley, C. P. Tripp, B. A. Morrowt, J. Catal., 1986, 99, 104-110.
[56] V. V. Danilevich, L. A. Isupova, E. A. Paukshtis, V. A. Ushakov, Kinet. Catal., 2014, 55(3), 372-379.
[57] G. C. Bond, Heterogeneous Catalysis, Principles and Applications, 2^nd ed, Oxford Science publications, Oxford, 1987, 140.
[58] C. N. Satterfield, Mass Transfer in Heterogeneous Catalysis, M. I. T Press, Cambridge, 1970, 267.
[59] A. Wheeler, Adv. Catal., 1951, 3, 249-327.
[60] M. Steijns, P. Mars, Ind. Chem. Prod. Res. Dev., 1977, 16, 35-39.
[61] M. Steijns, P. Kooprian, B. Nieuwenhuijse, P. Mars, J. Catal., 1976, 42, 96-106.
[62] A. V. Mashkina, Heterogeneous Catalysis in Chemistry of Organic Sulfur Compounds, Novosibirsk, Nayka, 1977, 237.
[63] T. S. Yang, T. H. Chang, C. T. Yeh, J. Mol. Catal. A, 1997, 115, 339-347.
[64] G. A. H. Mekhemer, M. I. Zaki, Surf. Sci., 2016, 652, 269-277.
[65] T. V. Reshetenko, S. R. Khairulin, Z. R. Ismagilov, V. V. Kuznetsov, Intern. J. Hydrogen Energy, 2002, 27, 387-394.
[66] A. V. Mashkina, E. A. Paukshtis, V. N. Yakovleva, Kinet. Catal., 1988, 29, 596-603.
[67] I. V. Desyatov, E. A. Paukshtis, A. V. Mashkina, React. Kinet. Catal. Lett., 1990, 41, 161-165.
[68] O. Saur, T. Chevreau, J. Lamotte, J. Travert, J. C. Lavalley, J. Chem. Soc., Faraday Trans. 1, 1981, 77, 427-437.
[69] C. L. Liu, T. T. Chuang, I. G. Dalla Lana, J. Catal., 1972, 26, 474-482.
[70] E. Laperdrix, A. Sahibed-dine, G. Costentin, O. Saur, M. Bensitel, C. Nedez, A. B. Mohamed Saad, J.C. Lavalley, Appl. Catal. B, 2000, 26, 71-80.
[71] A. V. Deo, I. G. Dalla Lana, H. W. Habgood, J. Catal., 1971, 21, 270-281.
[72] G. Herzberg, Infrared and Raman spectra of polyatomic molecules, D. Nostrand Co. Inc., Princeton, New Jersey, 1959, 283.
[73] T. L. Slager, C. H. Amberg, Can. J. Chem., 1972, 50, 3416-3423.
[74] C. L. Garcia, J. A. Lercher, J. Phys. Chem., 1992, 96, 2230-2235.
[75] M. Ziolek, I. Sobczak, I. Nowak, M. Daturi, J. C. Lavalley, Appl. Catal. B, 2000, 28, 197-207.
[76] J. C. Lavalley, J. Travert, T. Chevreau, J. Lamotte, O. Saur, J. Chem. Soc. Chem. Commun., 1979, 147-148.
[77] T. Yamaguchi, T. Jin, K. Tanabe, J. Phys. Chem., 1986, 90, 3148-3152.
[78] M. Bensitel, O. Saur, J. C. Lavalley, B. A. Morrow, Mater. Chem. Phys., 1988, 19, 147-156.
[79] Z. M. George, M. Bensitel, M. Lion, O. Saur, J. C. Lavalley, Appl. Catal., 1988, 43, 167-176.
[80] M. Prettre, R. Sion, Z. Elektrochem., 1959, 63, 100-105.
[81] M. Steijns, F. Derks, A. Verloop, P. Mars, J. Catal., 1976, 42, 87-95.
[82] C. Morterra, G. Cerrato, V. Bolis, Catal. Today, 1993, 17, 505-515.

χ-氧化铝的添加对纯的和修饰的γ-氧化铝上H₂S氧化反应性能的影响

Effect of χ-alumina addition on H₂S oxidation properties of pure and modified γ-alumina

PDF

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

[1]	凌云健, 冉义华, 邵伟鹏, 李娜, 焦峰, 潘秀莲, 傅强, 刘志, 杨帆, 包信和. ZnCr₂O₄表面CO加氢反应活性位点的探测[J]. 催化学报, 2022, 43(8): 2017-2025.
[2]	翁雪霏, 杨双莉, 丁丁, 陈明树, 万惠霖. 宽波段原位红外吸收光谱在Pd/SiO₂和Cu/SiO₂催化剂上CO氧化中的应用[J]. 催化学报, 2022, 43(8): 2001-2009.
[3]	曹凯鹏, 樊栋, 曾姝, 樊本汉, 陈南, 高铭斌, 朱大丽, 王林英, 田鹏, 刘中民. 无机体系合成纳米丝光沸石组装体及其优异的二甲醚羰基化催化性能[J]. 催化学报, 2021, 42(9): 1468-1477.
[4]	武慧中, 王佳栋, 陈瑞敏, 袁潮苇, 张锦, 张育新, 盛剑平, 董帆. 具有独特电子结构的锌掺杂SnO₂介导形成氧空位实现高效稳定的光催化降解甲苯[J]. 催化学报, 2021, 42(7): 1195-1204.
[5]	丁倩, 陈涛, 政, 冯兆池, 王秀丽. Cr₂O₃-Rh/Ga₂O₃光催化分解水的时间分辨红外光谱研究[J]. 催化学报, 2021, 42(5): 808-816.
[6]	Steffen Cychy, Sebastian Lechler, Zijian Huang, Michael Braun, Ann Cathrin Brix, Peter Blümler, Corina Andronescu, Friederike Schmid, Wolfgang Schuhmann, Martin Muhler. 甘油氧化的光谱电化学傅里叶变换衰减全反射谱红外光谱薄膜流动池中硼酸镍层厚度的优化[J]. 催化学报, 2021, 42(12): 2206-2215.
[7]	刘怡, 张光辉, 王建洋, 朱杰, 张新宝, Jeffrey T. Miller, 宋春山, 郭新闻. CO₂消除镓氢物种提升Ga₂O₃/SiO₂丙烷脱氢反应性能[J]. 催化学报, 2021, 42(12): 2225-2233.
[8]	朱文军, 陈霄, 金建辉, 邸鑫, 梁长海, 刘中民. Co₃O₄-CeO₂氧化物对丙烷完全氧化的催化性能[J]. 催化学报, 2020, 41(4): 679-690.
[9]	赵梓俨, Dmitry E. Doronkin, 叶英浩, Jan-Dierk Grunwaldt, 黄泽皑, 周莹. 光照对Pt/Al₂O₃光热CO₂加氢反应的增强作用[J]. 催化学报, 2020, 41(2): 286-293.
[10]	路饶, 贺雷, 王阳, 高新芊, 李文翠. 镍掺杂对氧化铝纳米片负载金催化剂在CO氧化反应中的促进作用[J]. 催化学报, 2020, 41(2): 350-356.
[11]	任泉明, 莫胜鹏, 樊洁, 冯振涛, 张明远, 陈培榕, 高加俭, 付名利, 陈礼敏, 吴军良, 叶代启. 构筑耦合界面提高MnO₂@Co₃O₄催化氧化甲苯性能[J]. 催化学报, 2020, 41(12): 1873-1883.
[12]	张祎旸, 曾慧, 贾斌, 王智华, 刘志明. Pd/TiO₂催化剂上氢气选择性催化还原NO_x的研究[J]. 催化学报, 2019, 40(6): 849-855.
[13]	孙艳娟, 王红, 邢倩, 崔雯, 李解元, 吴素娟, 孙立东. 氧空位对Bi₂MoO₆的关键作用:促进可见光光催化活性和反应机理[J]. 催化学报, 2019, 40(5): 647-655.
[14]	高新芊, 陆文多, 户守昭, 李文翠, 陆安慧. 棒状多孔氧化铝负载氧化铬催化丙烷脱氢反应性能[J]. 催化学报, 2019, 40(2): 184-191.
[15]	戴晓霞, 蒋威宇, 王望龙, 翁小乐, 尚媛, 薛烨辉, 吴忠标. 超临界水热合成过渡金属改性铈基催化剂应用于CO-SCR脱硝研究[J]. 催化学报, 2018, 39(4): 728-735.