La1-xSrxMnO3催化剂催化CH4选择性还原NO的实验研究

doi:10.7523/j.issn.2095-6134.2016.02.014

中国科学院大学学报 ›› 2016, Vol. 33 ›› Issue (2): 234-239.DOI: 10.7523/j.issn.2095-6134.2016.02.014

• 中国工程热物理学会2014年多相流年会专栏 • 上一篇下一篇

La_1-xSr_xMnO₃催化剂催化CH₄选择性还原NO的实验研究

张航¹, 黄思嘉², 李娜¹, 周屈兰¹

1. 西安交通大学动力工程多相流国家重点实验室, 西安 710049;
2. 福建省电力勘测设计院, 福州 350003

收稿日期:2015-03-13 修回日期:2015-07-07 发布日期:2016-03-15
通讯作者: 周屈兰
基金资助:
江苏省自然科学基金(BK20130459)资助

Selective catalytic reduction of NO with CH₄ on La_1-xSr_xMnO₃ catalysts

ZHANG Hang¹, HUANG Sijia², LI Na¹, ZHOU Qulan¹

1. State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an 710049, China;
2. Fujian Electric Power Survey & Design Institute, Fuzhou 350003, China

Received:2015-03-13 Revised:2015-07-07 Published:2016-03-15

摘要/Abstract

摘要：

采用溶胶-凝胶法和过量浸渍法制备粉末状及负载型La_(1-x)Sr_xMnO₃ (x=0.2、0.4)催化剂.SEM表征表明La_0.8Sr_0.2MnO₃催化剂具有连续多孔结构.在设计的固定床反应器中,实验测试表明La_0.8Sr_0.2MnO₃在900~1 000 ℃、停留时间大于2.2 s、含氧量小于6%时的NO脱除率达到90%以上,而La_0.6Sr_0.4MnO₃的高活性反应条件与La_0.8Sr_0.2MnO₃相似.在低温区,La_0.6Sr_0.4MnO₃的NO脱除率在600 ℃时达到40%,而La_0.8Sr_0.2MnO₃只有20%.根据实验结果计算了两种催化剂无氧反应条件下的活化能.La_0.6Sr_0.4MnO₃为催化剂的反应活化能比La_0.8Sr_0.2MnO₃为催化剂时低.

关键词: 钙钛矿, 甲烷, 一氧化氮, 选择性催化还原

Abstract:

The perovskite catalysts La_1-xSr_xMnO₃ (x=0.2, 0.4) powders and supported catalysts via sol-gel method were successfully synthesized. The images of SEM show that La_0.8Sr_0.2MnO₃ had a continuous and complete porous structure. The catalytic activity of supported La_1-xSr_xMnO₃ catalyst was tested in fixed bed reactor. The NO conversion ratio of La_0.8Sr_0.2MnO₃ was above 90% when the duration was longer than 2.2 s, the O₂ concentration was less than 6%, and the temperature was around 900-1 000 ℃, and La_0.6Sr_0.4MnO₃ acted similarly. At 600 ℃ the NO conversion ratio of La_0.6Sr_0.4MnO₃ was up to 40%, while the ratio of La_0.8Sr_0.2MnO₃ was only 20%. Besides, the activation energies for these two catalysts were calculated, and the activation energy for La_0.6Sr_0.4MnO₃ was lower than that for La_0.8Sr_0.2MnO₃.

Key words: perovskite, methane, NO, selective catalytic reduction

中图分类号:

TQ032
O643

张航, 黄思嘉, 李娜, 周屈兰. La_1-xSr_xMnO₃催化剂催化CH₄选择性还原NO的实验研究[J]. 中国科学院大学学报, 2016, 33(2): 234-239.

ZHANG Hang, HUANG Sijia, LI Na, ZHOU Qulan. Selective catalytic reduction of NO with CH₄ on La_1-xSr_xMnO₃ catalysts[J]. , 2016, 33(2): 234-239.

参考文献

[1] 张金桥.富氧条件下沸石分子筛负载Co, Mn选择催化CH₄还原NO_x的研究[D]. 太原: 太原理工大学, 2007.
[2] Iliopoulou E F, Evdou A P, Lemonidou A A, et al. Ag/alumina catalysts for the selective catalytic reduction of NO_x using various reductants[J]. Appl Catal A: Gen, 2004, 274(1/2): 179-189.
[3] Kotsifa A, Kondarides D I, Verykios XE. A comparative study of the selective catalytic reduction of NO by propylene over supported Pt and Rh catalysts[J]. Appl Catal B: Environ, 2008, 80(3/4): 260-270.
[4] Liu Z, Wang K, Zhang X, et al. Study on methane selective catalytic reduction of NO on Pt/Ce0.67 Zr0.33O2 and its application[J]. J Nat Gas Chem, 2009, 18(1): 66-70.
[5] Li Y, Battavio P B, Armor J N. Effect of water-vapor on the selective reduction of NO by methane over cobalt-exchanged ZSM-5[J]. J Catal, 1993, 142(2): 561-571.
[6] Choi B C, Foster D E. State-of-the-art of de-NOx technology using zeolite catalysts in automobile engines[J]. J Ind Eng Chem, 2005, 1(1): 1-9.
[7] 苏亚欣,苏阿龙,成豪.金属铁直接催化还原NO 的实验研究[J].煤炭学报, 2013, 38(s1) : 206-210.
[8] 苏亚欣,邓文义,苏阿龙.甲烷在氧化铁表面还原NO 的特性与反应机理研究[J].燃料化学学报,2013,41(9): 1 129-1 135.
[9] 梁珍成,秦永宁,乔冠东,等.La-Ce-Mn系钙钛矿型催化剂性能研究[J].化学物理学报,1997,10(1):60-67.
[10] Buciuman F-C, Joubert E, Menezo J-C, et al. Catalytic properties of La_0.8A_0.2MnO₃ (A=Sr, Ba, K, Cs) and LaMn_0.8B_0.2O₃ (B=Ni, Zn, Cu) perovskites: 2. Reduction of nitrogen oxides in the presence of oxygen[J]. Applied Catalysis B: Environmental, 2001, 35 (2): 149-156.
[11] Ishihara T, Ando M, Sada K, et al. Direct decomposition of NO into N₂ and O₂ over La(Ba)Mn(In)O₃ perovskite oxide[J]. Journal of Catalysis, 2003, 220 (1): 104-114.
[12] Oh S H, Mitchell P J,Siewert R M. Catalytic Contral of Air Pollution[P],ACS Symposium Series,1992,12: 495-509.
[13] Gutierrez LB, Ramallo-López JM, Irusta S, et al. Promotional effect of reduction treatments of ptIn(ferrierite) on its activity in the SCR of NO with methane. Kinetics and novel characterization studies[J]. The Journal of Physical Chemistry B, 2001, 105 (39): 9 514-9 523.
[14] 张航,黄思嘉,李娜等.La_1-xSr_xMnO₃选择性催化甲烷脱硝的实验研究[C]//中国动力工程学会锅炉专业委员会.中国动力工程学会锅炉专业委员会2013年学术研讨会论文集.四川. 2013: 168-176.
[15] Montanari T, Marie O, Daturi M, et al. Searching for the active sites of Co-H-MFI catalyst for the selective catalytic reduction of NO by methane: A FT-IR in situ and operando study[J]. Applied Catalysis B: Environmental, 2007, 71 (3/4): 216-222.
[16] 徐如人,庞文琴,霍启生.无机合成与制备化学[M].北京:高等教育出版社,2009.
[17] 潘智勇,张长斌,余长春,等.负载型镧锰钙钛矿催化剂上甲烷催化燃烧的研究[J].分子催化,2003,17(4): 274-278.

La_1-xSr_xMnO₃催化剂催化CH₄选择性还原NO的实验研究

Selective catalytic reduction of NO with CH₄ on La_1-xSr_xMnO₃ catalysts

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