AgMn/HZSM-5催化剂上室温O3氧化脱除空气中的苯：Mn含量和水含量的影响

doi:10.1016/S1872-2067(14)60070-X

催化学报 ›› 2014, Vol. 35 ›› Issue (9): 1465-1474.DOI: 10.1016/S1872-2067(14)60070-X

AgMn/HZSM-5催化剂上室温O₃氧化脱除空气中的苯：Mn含量和水含量的影响

刘阳, 李小松, 刘景林, 石川, 朱爱民

大连理工大学等离子体物理化学实验室, 辽宁大连116024

收稿日期:2014-01-22 修回日期:2014-03-03 出版日期:2014-08-19 发布日期:2014-08-22
通讯作者: 朱爱民
基金资助:
国家自然科学基金（U1201231，11175036）.

Ozone catalytic oxidation of benzene over AgMn/HZSM-5 catalysts at room temperature：Effects of Mn loading and water content

Yang Liu, Xiaosong Li, Jinglin Liu, Chuan Shi, Aimin Zhu

Laboratory of Plasma Physical Chemistry, Dalian University of Technology, Dalian 116024, Liaoning, China

Received:2014-01-22 Revised:2014-03-03 Online:2014-08-19 Published:2014-08-22
Supported by:
This work was supported by the National Natural Science Foundation of China (U1201231, 11175036).

摘要/Abstract

摘要：

考察了Mn含量和水含量对AgMn/HZSM-5（AgMn/HZ）催化剂上室温O₃氧化（OZCO）脱除空气中苯的影响. 研究发现，Mn含量为2.4 wt%的AgMn/HZ催化剂（AgMn/HZ（2.4））具有大的比表面积和高的MnO_x分散度，OZCO活性和稳定性最高. 反应后的程序升温脱附结果表明，2.4 wt%的Mn含量能有效抑制苯和甲酸在催化剂上的残留. 当Mn含量≤ 2.4 wt%时，催化剂分解O₃的活性在苯氧化过程中占主导；当Mn含量 > 2.4 wt%时，苯的活化起主要作用. 基于AgMn/HZ（2.4）催化剂优越的反应活性和稳定性，进一步研究了湿气流中该催化剂上苯的氧化. 与干气流相比，水汽的加入能显著提高催化剂的反应活性和稳定性，且以0.1-0.2 vol%水含量时最优.

关键词: 催化氧化苯, 臭氧, AgMn/HZSM-5催化剂, Mn含量, 水含量

Abstract:

The effects of Mn loading and water content on AgMn/HZSM-5 (AgMn/HZ) catalysts were investigated in the ozone catalytic oxidation (OZCO) of benzene in a continuous air flow at room temperature. The catalytic activity is closely related to the Mn loading, and the AgMn/HZ catalyst with 2.4 wt% Mn (AgMn/HZ(2.4)) had the highest activity and stability in benzene oxidation as a result of its large surface area and high MnO_x dispersion. Temperature-programmed desorption of the used catalysts demonstrated that 2.4 wt% was also the optimal Mn loading for suppressing the accumulation of benzene and HCOOH over the catalyst surface after benzene oxidation. For AgMn/HZ catalysts with Mn loadings ≤ 2.4 wt%, O₃ decomposition to active oxygen species (O*) plays the most important role in benzene oxidation; however, benzene activation is the crucial step for benzene oxidation by O₃ over AgMn/HZ catalysts with Mn loadings > 2.4 wt%. The AgMn/HZ(2.4) catalyst was then used to perform OZCO of benzene in a humid stream. Compared with dry gas, water vapor greatly enhanced the activity and stability of the AgMn/HZ(2.4) catalyst, and 0.1-0.2 vol% was the optimal water content for benzene oxidation.

Key words: Catalytic oxidation of benzene, Ozone, AgMn/HZSM-5 catalyst, Mn loading, Water vapor

刘阳, 李小松, 刘景林, 石川, 朱爱民. AgMn/HZSM-5催化剂上室温O₃氧化脱除空气中的苯：Mn含量和水含量的影响[J]. 催化学报, 2014, 35(9): 1465-1474.

Yang Liu, Xiaosong Li, Jinglin Liu, Chuan Shi, Aimin Zhu. Ozone catalytic oxidation of benzene over AgMn/HZSM-5 catalysts at room temperature：Effects of Mn loading and water content[J]. Chinese Journal of Catalysis, 2014, 35(9): 1465-1474.

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参考文献

[1] Whysner J, Reddy M V, Ross P M, Mohan M, Lax E A. Mutat Res, 2004, 566: 99
[2] Zhao D Z, Ding T Y, Li X S, Liu J L, Shi C, Zhu A M. Chin J Catal (赵德志, 丁天英, 李小松, 刘景林, 石川, 朱爱民. 催化学报), 2012, 33: 396
[3] Kasprzyk-Hordern B, Zió?ek M, Nawrocki J. Appl Catal B, 2003, 46: 639
[4] Xiao H, Liu R P, Zhao X, Qu J H. Chemosphere, 2008, 72: 1006
[5] Long L P, Zhao J G, Yang L X, Fu M L, Wu J L, Huang B C, Ye D Q. Chin J Catal (龙丽萍, 赵建国, 杨利娴, 付名利, 吴军良, 黄碧纯, 叶代启. 催化学报), 2011, 32: 904
[6] Konova P, Stoyanova M, Naydenov A, Christoskova St, Mehandjiev D. Appl Catal A, 2006, 298: 109
[7] Naydenov A, Mehandjiev D. Appl Catal A, 1993, 97: 17
[8] Mehandjiev D, Cheshkova K, Naydenov A, Georgesku V. React Kinet Catal Lett, 2002, 76: 287
[9] Dimitrova S, Ivanov G, Mehandjiev D. Appl Catal A, 2004, 266: 81
[10] Stoyanova M, Konova P, Nikolov P, Naydenov A, Christoskova St, Mehandjiev D. Chem Eng J, 2006, 122: 41
[11] Einaga H, Futamura S. J Catal, 2004, 227: 304
[12] Einaga H, Ogata A. J Hazard Mater, 2009, 164: 1236
[13] Einaga H, Futamura S. React Kinet Catal Lett, 2004, 81: 121
[14] Einaga H, Harada M, Ogata A. Catal Lett, 2009, 129: 422
[15] Mehandjiev D, Zhecheva E, Ivanov G, Ioncheva R. Appl Catal A, 1998, 167: 277
[16] Mehandjiev D, Naydenov A, Ivanov G. Appl Catal A, 2001, 206: 13
[17] Naydenov A, Stoyanova R, Mehandjiev D. J Mol Catal A, 1995, 98: 9
[18] Einaga H, Ogata A. Environ Sci Technol, 2010, 44: 2612
[19] Rezaei E, Soltan J. Chem Eng J, 2012, 198-199: 482
[20] Rezaei E, Soltan J, Chen N. Appl Catal B, 2013, 136-137: 239
[21] Rezaei E, Soltan J, Chen N, Lin J R. Chem Eng J, 2013, 214: 219
[22] Einaga H, Futamura S. J Catal, 2006, 243: 446
[23] Einaga H, Teraoka Y, Ogat A. Catal Today, 2011, 164: 571
[24] Zhao D Z, Shi C, Li X S, Zhu A M, Jang B W L. J Hazard Mater, 2012, 239-240: 362
[25] Wang M X, Zhang P Y, Li J G, Jiang C J. Chin J Catal (王鸣晓, 张彭义, 李金格, 姜传佳. 催化学报), 2014, 35: 335
[26] Wang M Y, Zhu T L, Fan X. Chin Environ Sci (王美艳, 朱天乐, 樊星. 中国环境科学), 2009, 29: 806
[27] Einaga H, Teraoka Y, Ogat A. J Catal, 2013, 305: 227
[28] Fan H Y, Shi C, Li X S, Zhao D Z, Xu Y, Zhu A M. J Phys D, 2009, 42: 225105
[29] Fan H Y, Li X S, Shi C, Zhao D Z, Liu J L, Liu Y X, Zhu A M. Plasma Chem Plasma Process, 2011, 31: 799
[30] Zhao D Z, Li X S, Shi C, Fan H Y, Zhu A M. Chem Eng Sci, 2011, 66: 3922
[31] Qu Z P, Bu Y B, Qin Y, Wang Y, Fu Q. Appl Catal B, 2013, 132-133: 353
[32] Bogdanchikova N, Meunier F C, Avalos-Borja M, Breen J P, Pestryakov A. Appl Catal B, 2002, 36: 287
[33] Shi C, Chen B B, Li X S, Crocker M, Wang Y, Zhu A M. Chem Eng J, 2012, 200-202: 729
[34] Ma F T, Lou H. Chin J Catal (马福泰, 楼辉. 催化学报), 1984, 5: 82
[35] Boot L A, Kerkhoffs M H J V, van der Linden B T, Jos van Dillen A, Geus J W, van Buren F R. Appl Catal A, 1996, 137: 69
[36] Dhandapani B, Oyama S T. Appl Catal B, 1997, 11: 129
[37] Oyama S T. Catal Rev-Sci Eng, 2000, 42: 279
[38] Wang H C, Chang S H, Hung P C, Hwang J F, Chang M B. J Hazard Mater, 2009, 164: 1452
[39] Radhakrishnan R, Oyama S T, Chen J G, Asakura K. J Phys Chem B, 2001, 105: 4245
[40] Wang H C, Chang S H, Hung P C, Hwang J F, Chang M B. Chemosphere, 2008, 71: 388

AgMn/HZSM-5催化剂上室温O₃氧化脱除空气中的苯：Mn含量和水含量的影响

Ozone catalytic oxidation of benzene over AgMn/HZSM-5 catalysts at room temperature：Effects of Mn loading and water content

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