预处理条件对Ag/SBA-15催化剂上甲苯催化氧化反应性能的影响

doi:10.1016/S1872-2067(17)62842-0

催化学报 ›› 2017, Vol. 38 ›› Issue (9): 1603-1612.DOI: 10.1016/S1872-2067(17)62842-0

预处理条件对Ag/SBA-15催化剂上甲苯催化氧化反应性能的影响

秦媛, 曲振平, 董翠, 黄娜

大连理工大学环境学院, 工业生态与环境工程教育部重点实验室, 辽宁大连 116024

收稿日期:2016-12-13 修回日期:2017-04-19 出版日期:2017-09-18 发布日期:2017-09-06
通讯作者: 曲振平
基金资助:
国家自然科学基金（21377016，21577014）；长江学者与创新团队发展计划（IRT_13R05）.

Effect of pretreatment conditions on catalytic activity of Ag/SBA-15 catalyst for toluene oxidation

Yuan Qin, Zhenping Qu, Cui Dong, Na Huang

Key Laboratory of Industrial Ecology and Environmental Engineering(MOE), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, Liaoning, China

Received:2016-12-13 Revised:2017-04-19 Online:2017-09-18 Published:2017-09-06
Contact: 10.1016/S1872-2067(17)62842-0
Supported by:
This work was supported by the National Natural Science Foundation of China (21377016, 21577014) and Program for Changjiang Scholars and Innovative Research Team in University (IRT_13R05).

摘要/Abstract

摘要：

甲苯是一种典型的挥发性有机污染物.近年来，催化氧化法是一种广泛使用并具有开发潜力的有效去除挥发性有机污染物的方法，而贵金属催化剂一直是首选.介孔二氧化硅材料SBA-15具有规则孔道和较高的比表面积因而在催化领域中具有较大的应用潜力.本课题组已对一系列的SBA-15负载的纳米银催化剂的制备和低温催化氧化性能进行了研究，本文则通过研究不同预处理处理气氛对Ag/SBA-15催化剂结构以及甲苯催化氧化性能的系统研究，获得纳米银催化剂结构与甲苯催化氧化性能间的构效关系，对新催化剂的结构优化以及甲苯催化净化的低温催化剂开发具有重要的科学意义.
研究表明，处理气氛明显影响了银物种和氧物种的状态，进而影响了催化剂的催化活性，先氧气（500℃）后氢气（300℃）处理的O500-H300催化剂对甲苯的反应活性明显优于在500℃氧气处理样品O500及氢气处理样品H500.由X-射线衍射和O₂-程序升温脱附（TPD）可知，氧气500℃处理使催化剂上形成大颗粒银粒子和氧化银粒子，以及大量次表层氧物种.氢气处理使催化剂形成较大的银粒子，由于未经过氧气处理，该催化剂上并没有次表层氧的生成.先氧气处理再氢气处理后催化剂上形成高分散的小粒径银粒子以及次表层氧物种，这表明低温氢气处理可以降低银粒子的尺寸并使催化剂上的银粒子得到再分散，同时不会影响次表层氧物种的形成.从催化剂的甲苯吸附和TPD实验中看出，大尺寸银粒子对甲苯具有较强的吸附性能，从而有利于甲苯在低温的催化氧化，但是在高温反应中没有优势；小尺寸银粒子虽然对甲苯的吸附能力不强，但是对分子氧有较好的吸附作用，进而增强自身与甲苯的相互作用，而且也促进了分子氧的活化，预处理中形成的次表层氧有效增强了甲苯和银粒子的相互作用，因此，先氧气后氢气处理的O500-H300样品在反应中显示出最好的甲苯催化活性.

关键词: SBA-15, 负载型银催化剂, 预处理条件, 竞争吸附, 甲苯氧化

Abstract:

The catalytic oxidation of toluene over Ag/SBA-15 synthesized under different pretreatment condi-tions, including O₂ at 500℃ (denoted O500), H₂ at 500℃ (H500), and O₂ at 500℃ followed by H₂ at 300℃ (O500-H300) was studied. The pretreated samples were investigated by N₂ physisorption, X-ray diffraction, and ultraviolet-visible diffuse reflectance. The pretreatment atmosphere greatly influences the status of the Ag and O species, which in turn significantly impacts the adsorption and catalytic removal of toluene. Ag₂O and amorphous Ag particles, as well as a large amount of subsur-face oxygen species, are formed on O500, and the subsurface oxygen enhances the interaction be-tween Ag species and toluene, so O500 shows good activity at higher temperature. However, its activity at lower temperature is not as high as expected, with a reduced presence of Ag₂O and lower adsorption capacity for toluene. H₂ pretreatment at 500℃ is conducive to the formation of large Ag particles and yields the largest adsorption capacity for toluene, so H500 exhibits the best activity at lower temperatures; however, because of poor interaction between Ag and toluene, its activity at higher temperature is modest. The O500-H300 sample exhibits excellent catalytic activity during the whole reaction process, which can be attributed to the small and highly dispersed Ag nanoparti-cles as well as the existence of subsurface oxygen.

Key words: SBA-15, Supported silver catalyst, Pretreatment condition, Competitive adsorption, Toluene oxidation

秦媛, 曲振平, 董翠, 黄娜. 预处理条件对Ag/SBA-15催化剂上甲苯催化氧化反应性能的影响[J]. 催化学报, 2017, 38(9): 1603-1612.

Yuan Qin, Zhenping Qu, Cui Dong, Na Huang. Effect of pretreatment conditions on catalytic activity of Ag/SBA-15 catalyst for toluene oxidation[J]. Chinese Journal of Catalysis, 2017, 38(9): 1603-1612.

×
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(17)62842-0

https://www.cjcatal.com/CN/Y2017/V38/I9/1603

参考文献

[1] S. W. Baek, J. R. Kim, S. K. Ihm, Catal. Today, 2004, 93-95, 575-581.
[2] T. Masui, H. Imadzu, N. Matsuyama, N. Imanaka, J. Hazard. Mater., 2010, 176, 1106-1109.
[3] J. Bedia, J. M. Rosas, J. Rodriguez-Mirasol, T. Cordero, Appl. Catal. B, 2010, 94, 8-18.
[4] X. R. Fu, Y. Liu, W. Y. Yao, Z. B. Wu, Catal. Commun., 2016, 83, 22-26.
[5] H. G. Yang, J. G. Deng, Y. X. Liu, S. H. Xie, P. Xu, H. X. Dai, Chin. J. Catal., 2016, 37, 934-946.
[6] D. Chlala, J. M. Giraudon, N. Nuns, C. Lancelot, R. N. Vannier, M. Labaki, J. F. Lamonier, Appl. Catal. B, 2016, 184, 87-95.
[7] F. Wang, H. X. Dai, J. G. Deng, S. H. Xie, H. G. Yang, W. Han, Chin. J. Catal., 2014, 35, 1475-1481.
[8] B. Z. Gao, J. G. Deng, Y. X. Liu, Z. X. Zhao, X. W. Li, Y. Wang, H. X. Dai, Chin. J. Catal., 2013, 34, 2223-2229.
[9] X. D. Zhang, Y. X. Wang, F. L. Hou, H. X. Li, Y. Yang, Y. Q. Yang, Y. Wang, Appl. Surf. Sci., 2017, 476-483.
[10] X. D. Zhang, H. Dong, Y. Wang, N. Liu, Y. H. Zuo, L. F. Cui, Chem. Eng. J., 2016, 283, 1097-1107.
[11] H. L. Jiang, T. Akita, T. Ishida, M. Haruta, Q. Xu, J. Am. Chem. Soc., 2011, 133, 1304-1306.
[12] L. Zhang, F. D. Liu, Y. B. Yu, Y. C. Liu, Zhang, C. B. He Hong, Chin. J. Catal., 2011, 32, 727-735.
[13] L. Zhang, C. B. Zhang, H. He, J. Catal., 2009, 261, 101-109.
[14] Q. Wu, H. W. Gao, H. He, Chin. J. Catal., 2006, 27, 403-408.
[15] L. Ma, L. H. Jia, X. F. Guo, L. J. Xiang, Chin J. Catal., 2014, 35, 108-119.
[16] V. Zielasek, B. Jürgens, C. Schulz, J. Biener, M. M. Biener, A. V. Ham-za, M. Bäumer, Angew. Chem. Int. Ed., 2006, 45, 8241-8244.
[17] A. Wittstock, B. Neumann, A. Schaefer, K. Dumbuya, C. Kübel, M. M. Biener, V. Zielasek, H. P. Steinrück, J. M. Gottfried, J. Biener, A. Hamza, M. Bäumer, J. Phys. Chem. C, 2009, 113, 5593-5600.
[18] C. X. Xu, J. X. Su, X. H. Xu, P. P. Liu, H. J. Zhao, F. Tian, Y. Ding, J. Am. Chem. Soc., 2007, 129, 42-43.
[19] Y. X. Yang, C. Ochoa-Hernández, P. Pizarro, V. A. de la Peña O'shea, J. M. Coronado, D. P. Serrano., Appl. Catal. B, 2016, 197, 206-213.
[20] Y. H. Cheng, L. B. Zhou, J. X. Xu, C. X. Miao, W. M. Hua, Y. H. Yue, Z. Gao, Microporous Mesoporous Mater., 2016, 234, 370-376.
[21] X. D. Zhang, Z. P. Qu, F. L. Yu, Y. Wang, J. Catal., 2013, 297, 264-271.
[22] D. Chen, Z. P. Qu, Y. H. Sun, K. Gao, Y. Wang, Appl. Catal. B, 2013, 142-143, 838-848.
[23] E. Van Steen, G. S. Swell, R. A. Makhothe, C. Miklethwaite, H. Man-stein, M. de Lange, C. T. O'Connor, J. Catal., 1996, 162, 220-229.
[24] L. M. Chen, D. Ma, X. H. Bao, J. Phys. Chem. C, 2007, 111, 2229-2242.
[25] W. B. Li, M. Zhang, J. X. Wang, Catal. Today, 2008, 137, 340-344.
[26] H. Li, H. Li, W. L. Dai, J. F. Deng, Appl. Catal. A, 2001, 207, 151-157.
[27] K. J. Kim, H. G. Ahn, Appl. Catal. B, 2009, 91, 308-318.
[28] L. Savio, A. Gerbi, L. Vattuone, R. Pushpa, N. Bonini, S. de Gironcoli, M. Rocca, J. Phys. Chem. C, 2007, 111, 10923-10930.
[29] X. D. Zhang, Z. P. Qu, F. L. Yu, Y. Wang, X. Zhang, J. Mol. Catal. A, 2013, 370, 160-166.
[30] Z. P. Qu, M. J. Cheng, W. X. Huang, X. H. Bao, J. Catal., 2005, 229, 446-458.
[31] Z. P. Qu, W. X. Huang, M. J. Cheng, X. H. Bao, J. Phys. Chem. B, 2005, 109, 15842-15848.
[32] B. Wang, D. Weng, X. D. Wu, J. Fan, Catal. Today, 2010, 153, 111-117.
[33] K. S. W. Sing, D. H. Everett, R. A. W. Haul, L. Moscou, R. A. Pierotti, J. Rouquérol, T. Siemieniewska, Pure Appl. Chem., 1985, 57, 603-619.
[34] S. C. Kim, J. H. Moon, J. Nanosci. Nanotechnol., 2011, 11, 1660-1663.
[35] A. Aboukaïs, M. Skaf, S. Hany, R. Cousin, S. Aouad, M. Labaki, E. Abi-Aad, Mater. Chem. Phys., 2016, 177, 570-576.
[36] H. G. Yang, J. G. Deng, Y. X. Liu, S. H. Xie, Z. X. Wu, H. X. Dai, J. Mol. Catal. A, 2016, 414, 9-18.
[37] X. Y. Liu, A. Q. Wang, T. Zhang, D. S. Su, C. Y. Mou, Catal. Today, 2010, 160, 103-108.
[38] X. She, M. Flytzani-Stephanopoulos, J. Catal., 2006, 237, 79-93.
[39] A. Keshavaraja, X. She, M. Flytzani-Stephanopoulos, Appl. Catal. B, 2000, 27, L1-L9.
[40] G. Mie, Ann. Phys. 1908, 25, 377-445.
[41] K. Shimizu, J. Shibata, H. Yoshida, A. Satsuma, T. Hattori, Appl. Catal. B, 2001, 30, 151-162.
[42] R. T. Yang, A. J. Herna'ndez-Maldonado, F. H. Yang, Science, 2003, 301, 79-81.
[43] A. J. Herna'ndez-Maldonado, R. T. Yang, AIChE J., 2004, 50, 791-801.
[44] K. Kosuge, S. Kubo, N. Kikukawa, M. Takemori, Langmuir, 2007, 23, 3095-3102.
[45] W. G. Shim, S. C. Kim, H. C. Kang, S. W. Nahm, J. W. Lee, H. Moon, Appl. Surf. Sci., 2007, 253, 5868-5875.
[46] W. G. Shim, J. W. Lee, S. C. Kim, Appl. Catal. B, 2008, 84, 133-141.
[47] W. G. Shim, S. C. Kim, Appl. Surf. Sci., 2010, 256, 5566-5571.
[48] M. Skotak, D. Lomot, Z. Karpinski, Appl. Catal. A, 2002, 229, 103-115.
[49] S. A. Tan, R. B. Grant, R. M. Lambert, J. Catal., 1987, 104, 156-163.
[50] A. Kokalj, A. D. Corso, S. de Gironcoli, S. Baroni, Surf. Sci., 2003, 532-535, 191-197.
[51] V. V. Dutova, G. V. Mamontova, V. I. Zaikovskii, O. V. Vodyankina., Catal. Today, 2016, 278, 150-156.

预处理条件对Ag/SBA-15催化剂上甲苯催化氧化反应性能的影响

Effect of pretreatment conditions on catalytic activity of Ag/SBA-15 catalyst for toluene oxidation

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]	邓长顺, 许孟霞, 董珍, 李磊, 杨金月, 郭学峰, 彭路明, 薛念华, 祝艳, 丁维平. 十六烷基膦酸配合的复合氧化物纳米催化剂稳定的O/W乳液中甲苯单一氧化为苯甲醛[J]. 催化学报, 2020, 41(2): 341-349.
[2]	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.
[3]	楚庆岩, 陈静, 侯文华, 余昊轩, 王平, 刘睿, 宋广亮, 朱红军, 赵萍萍. 超声吸附制备均匀分散在SBA-15的S₂O₈^2--Fe₂O₃纳米粒子:增强S₂O₈^2--Fe₂O₃本体催化活性[J]. 催化学报, 2018, 39(5): 955-963.
[4]	沈行加, 吴先元, 江大好, 李小年, 倪珺. 利用原位红外光谱确证Ru/SBA-15的加氢活性位点[J]. 催化学报, 2017, 38(9): 1597-1602.
[5]	李冰, 徐振新, 储伟, 罗仕忠, 敬方梨. 有序介孔Sn-SBA-15负载铂催化剂上丙烷脱氢性能的提高[J]. 催化学报, 2017, 38(4): 726-735.
[6]	袁博, 张宝, 王志亮, 卢胜梅, 李军, 刘龑, 李灿. 钨酸铋担载钯纳米粒子光催化甲苯及其衍生物到醛的氧化反应[J]. 催化学报, 2017, 38(3): 440-446.
[7]	Sang Wook Han, Myung-Geun Jeong, Il Hee Kim, Hyun Ook Seo, Young Dok Kim. 更低温度下和重复再生时NiO/SiO₂催化剂上甲苯完全氧化反应[J]. 催化学报, 2016, 37(11): 1931-1940.
[8]	邹成龙, 沙观宇, 顾海芳, 黄曜, 牛国兴. 改善SBA-15介孔材料水热稳定性的简单溶剂热后处理方法[J]. 催化学报, 2015, 36(8): 1350-1357.
[9]	Marzieh Mohammadi, Ghasem Rezanejade Bardajee, Nader Noroozi Pesyan. Efficient solvent-free synthesis of pyridopyrazine and quinoxaline derivatives using copper-DiAmSar complex anchored on SBA-15 as a reusable catalyst[J]. 催化学报, 2015, 36(8): 1379-1386.
[10]	Sanjay Srivastava, Pravakar Mohanty, Jigisha K. Parikh, Ajay K. Dalai, S. S. Amritphale, Anup K. Khare. Cr-free Co-Cu/SBA-15 catalysts for hydrogenation of biomass-derived α-, β-unsaturated aldehyde to alcohol[J]. 催化学报, 2015, 36(7): 933-942.
[11]	邹成龙, 沙观宇, 黄曜, 牛国兴, 赵东元. Al³⁺离子介入提升(NH₄)₂SiF₆对SBA-15介孔材料的水热稳定化作用[J]. 催化学报, 2015, 36(7): 1001-1008.
[12]	王润琴, 林荣和, 丁云杰, 刘佳, 罗文婷, 杜虹, 吕元 . 水热合成一锅法制备FePO₄-SBA-15及其水热稳定性能[J]. 催化学报, 2015, 36(3): 446-453.
[13]	胡龙兴, 杨帆, 邹联沛, 袁航, 胡星. Co-Fe/SBA-15与过一硫酸盐联用非均相催化降解水中染料罗丹明B[J]. 催化学报, 2015, 36(10): 1785-1797.
[14]	刘会敏, 李宇明, 吴昊, 杨维维, 贺德华. Nd, Ce和La改性对Ni/SBA-15催化剂在CH₄/CO₂重整反应中性能的影响[J]. 催化学报, 2014, 35(9): 1520-1528.
[15]	朱学成, 沈如伟, 张利雄. SBA-15负载的 Cu(Ⅱ) 席夫碱配合物催化的苯乙烯氧化反应制备苯甲醛[J]. 催化学报, 2014, 35(10): 1716-1726.