载体结构对锡铁负载型催化剂脱硝性能的影响

doi:10.16085/j.issn.1000-6613.2016.12.027

化工进展 ›› 2016, Vol. 35 ›› Issue (12): 3919-3927.DOI: 10.16085/j.issn.1000-6613.2016.12.027

载体结构对锡铁负载型催化剂脱硝性能的影响

陈凯歌^1,2, 肖峰², 蒋晓萍², 许琦²

1 常州大学石油化工学院, 江苏常州 213000;
2 盐城工学院, 江苏盐城 224000

收稿日期:2016-03-16 修回日期:2016-08-08 出版日期:2016-12-05 发布日期:2016-12-05
通讯作者: 徐琦,教授,研究方向为大气污染治理技术(NO_x、CO₂、VOC等)。E-mail:xgsteve@ycit.cn。
作者简介:陈凯歌(1992-),男,硕士研究生,研究方向为氮氧化物的催化转化。E-mail:m13851068451_2@163.com。

Effect of pore structure on the performance of Sn-Fe supported catalyst in denitration

CHEN Kaige^1,2, XIAO Feng², JIANG Xiaoping², XU Qi²

1 School of Petrochemical Engineering, ChangZhou University, Changzhou 213000, Jiangsu, China;
2 Yancheng Institute of Technology, Yancheng 224000, Jiangsu, China

Received:2016-03-16 Revised:2016-08-08 Online:2016-12-05 Published:2016-12-05

摘要/Abstract

摘要： 利用凹凸棒土（ATP）、活性炭（AC）、介孔硅（MCM-41）、二氧化钛（TiO₂）这4种孔结构不同的载体，通过水热法制备了以Fe₂O₃为催化剂主活性组分、SnO₂为辅活性组分的锡铁负载型催化剂。催化剂的微观结构通过BET和SEM测试，并在催化剂评价装置中模拟烟气组成，考察锡铁负载型催化剂在反应温度为80～280℃、脱硝空速为32000～48000h^-1范围内的选择性催化还原（SCR）性能。同时考察了SO₂与H₂O对1/2SnFe/ATP催化剂的影响。实验表明，载体可能为催化剂提供大量Brønsted酸性位点，有利于反应气体吸附。1/2SnFe/ATP催化剂表现出最佳的SCR脱硝性能，在200℃时实现最高96.4%的NO转化率，而且由其抗硫性及其抗水性实验表明：SO₂单独作用于催化剂时，脱硝效率降低迟缓，切断二氧化硫后仍能恢复到85%以上。同时加入水和二氧化硫后，将会导致脱硝效率急剧下降。停止加入后，催化剂效率又开始慢慢恢复，效率可以恢复达到70%以上。

关键词: 载体结构, 脱硝, 负载型催化剂, 选择性催化还原

Abstract: Four catalyst supports of different pore structures,namely attapulgite(ATP),activated carbon(AC),mesoporous silica(MCM-41)and titanium dioxide(TiO₂),were used to prepare a series of Sn-Fe supported catalysts by the hydrothermal synthesis method with the Fe₂O₃ as active component,and SnO₂ as auxiliary active component. The materials before and after preparation were characterized by BET and SEM. The denitration performance of the prepared catalysts for artificial flue gas were tested in a catalyst evaluation device in a temperature range of(80-280℃)and space velocity range of(32000-48000h^-1). Meanwhile,the impact of SO₂ and H₂O on the catalyst(1/2SnFe/ATP)was investigated. The results showed that carriers might provide a large number of Brønsted acid sites,which was beneficial for the gas adsorption reaction. Among all the test catalysts,the 1/2SnFe/ATP had the best SCR denitration performance. At 200℃,the conversion of NO could reach by 96.4%. It was also found,when there was only SO₂,the NO removal efficiency decreased slowly,and would still be higher than 85% if SO₂ input was cut off. But when H₂O and SO₂ were simultaneously added,the NO removal efficiency fell sharply and would went back to above 70% if H₂O and SO₂ input was cut off.

Key words: support structure, denitration, supported catalysts, selective catalytic reduction(SCR)

中图分类号:

X511

陈凯歌, 肖峰, 蒋晓萍, 许琦. 载体结构对锡铁负载型催化剂脱硝性能的影响[J]. 化工进展, 2016, 35(12): 3919-3927.

CHEN Kaige, XIAO Feng, JIANG Xiaoping, XU Qi. Effect of pore structure on the performance of Sn-Fe supported catalyst in denitration[J]. Chemical Industry and Engineering Progree, 2016, 35(12): 3919-3927.

参考文献

[1] ZHANG Tao,LI Jian,WANG D,et al.Selective catalytic reduction of NO with NH₃ over HZSM-5-supported Fe-Cu nanocomposite catalysts:the Fe-Cu bimetallic effect[J].Applied Catalysis B:Environmental,2014,148-149(6):520-531.
[2] WU D W,ZHANG Q L,LIN T,et al.Effect of calcination temperature on performance of Mn-Fe/CeO₂-TiO₂ catalyst for selective catalytic reduction of NO by NH₃ at low temperature[J].Applied Surface Science, 2014,289:237-244.
[3] ZHANG Runduo,YANG Wei,LUO Na,et al.Low-temperature NH₃-SCR of NO by lanthanum manganite perovskites:effect of A-/B-site substitution and TiO₂/CeO₂ support[J].Applied Catalysis B:Environmental,2014,146(3):94-104.
[4] BONINGARI Thirupathi,PANAGIOTIS G Smirniotis.Nickel-doped Mn/TiO₂ as an efficient catalyst for the low-temperature SCR of NO with NH₃:catalytic evaluation and characterizations[J].Journal of Catalysis,2012,288(4):74-83.
[5] LEI Zhigang,HAN Bin,YANG Kun,et al.Influence of H₂O on the low-temperature NH₃-SCR of NO over V₂O₅/AC catalyst:an experimental and modeling study[J].Chemical Engineering Journal,2013,215/216:651-657.
[6] 李云涛,钟秦.低温NH₃-SCR反应机理及动力学研究进展[J].化学进展,2009(6):1094-1100.
[7] LIU F,HONG H,ZHANG C,et al.Mechanism of the selective catalytic reduction of NO_x with NH₃ over environmental-friendly iron titanate catalyst[J].Catalysis Today,2011,175(1):18-25.
[8] MARBAN Gregorio,ANTUNA Raquel,FUERTES Antonio B.Low-temperature SCR of NO_x with NH₃ over activated carbon fiber composite-supported metal oxides[J].Applied Catalysis B:Environmental,2003,41(3):323-338.
[9] FEDEYKO Joseph M,CHEN Bin,CHEN Hai-Ying.Mechanistic study of the low temperature activity of transition metal exchanged zeolite SCR catalysts[J].Catalysis Today,2010,151(3/4):231-236.
[10] YOUNG Jin Kim,HYUK Jae Kwon,ILEONG Heo,et al.Mn-Fe/ZSM5 as a low-temperature SCR catalyst to remove NO_x from diesel engine exhaust[J].Applied Catalysis B:Environmental,2012,126:9-21.
[11] LIU Z,HAO J,FU L,et al.Promoting effect of sol-gel method and pre-treatment on the activity of SnO₂/Al₂O₃ catalyst for NO reduction by propene[J].Reaction Kinetics&Catalysis Letters,2003,80(1):45-52.
[12] IWASAKI M,YAMAZAKI K,SHINJOH H.NO_x reduction performance of fresh and aged Fe-zeolites prepared by CVD:effects of zeolite structure and Si/Al₂ ratio[J].Applied Catalysis B:Environmental,2011,102(s1/2):302-309.
[13] 杨超,程华,黄碧纯.抗SO₂和H₂O中毒的低温NH₃-SCR脱硝催化剂研究进展[J].化工进展,2014,33(4):907-913.
[14] 刘福东,单文坡,石晓燕,等.用于NH₃选择性催化还原NO_x的钒基催化剂[J].化学进展,2012,24(4):445-455.
[15] KIJLSTRA W S,BRANDS D S,SMIT H I,et al.Mechanism of the selective catalytic reduction of NO with NH₃ over MnOx/Al₂O₃[J].Journal of Catalysis,1997,171(1):219-230.
[16] COLOMBO M,NOVA I,TRONCONI E.Detailed kinetic modeling of the NH₃-NO/NO₂ SCR reactions over a commercial Cu-zeolite catalyst for Diesel exhausts after treatment[J].Catalysis Today,2012,197(1):243-255.
[17] 蔡小峰,李晓芸.SNCR-SCR烟气脱硝技术及其应用[J].电力环境保护,2008,24(3):26-29.
[18] SHEN B,LIU T,ZHAO N,et al.Iron-doped Mn-Ce/TiO₂ catalyst for low temperature selective catalytic reduction of NO with NH₃[J].Journal of Environmental Sciences,2010,22(9):1447-1454.
[19] PANAHI P Nakhostin,SALARI D,NIAEI A,et al.NO reduction over nanostructure M-Cu/ZSM-5(M:Cr,Mn,Co and Fe) bimetallic catalysts and optimization of catalyst preparation by RSM[J].Journal of Industrial and Engineering Chemistry,2013,19(6):1793-1799.
[20] 刘亭,王廷春,吴瑞青,等.低温NH₃-SCR脱硝催化剂研究进展[J].安全与环境学报,2012(6):36-42.
[21] 戎雪佳.铁基氧化物催化剂用于NH₃选择性催化还原NO的研究[D].天津:天津大学,2014.

载体结构对锡铁负载型催化剂脱硝性能的影响

Effect of pore structure on the performance of Sn-Fe supported catalyst in denitration

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	邓丽萍, 时好雨, 刘霄龙, 陈瑶姬, 严晶颖. 非贵金属改性钒钛基催化剂NH₃-SCR脱硝协同控制VOCs[J]. 化工进展, 2023, 42(S1): 542-548.
[2]	王乐乐, 杨万荣, 姚燕, 刘涛, 何川, 刘逍, 苏胜, 孔凡海, 朱仓海, 向军. SCR脱硝催化剂掺废特性及性能影响[J]. 化工进展, 2023, 42(S1): 489-497.
[3]	王晋刚, 张剑波, 唐雪娇, 刘金鹏, 鞠美庭. 机动车尾气脱硝催化剂Cu-SSZ-13的改性研究进展[J]. 化工进展, 2023, 42(9): 4636-4648.
[4]	李东泽, 张祥, 田键, 胡攀, 姚杰, 朱林, 卜昌盛, 王昕晔. 基于水泥窑脱硝的碳基还原NO _x 研究进展[J]. 化工进展, 2023, 42(9): 4882-4893.
[5]	朱传强, 茹晋波, 孙亭亭, 谢兴旺, 李长明, 高士秋. 固体高分子脱硝剂选择性非催化还原NO _x 特性[J]. 化工进展, 2023, 42(9): 4939-4946.
[6]	白志华, 张军. 二乙烯三胺五亚甲基膦酸/Fenton体系氧化脱除NO[J]. 化工进展, 2023, 42(9): 4967-4973.
[7]	李佳, 樊星, 陈莉, 李坚. 硝酸生产尾气中NO _x 和N₂O联合脱除技术研究进展[J]. 化工进展, 2023, 42(7): 3770-3779.
[8]	张巍, 秦川, 谢康, 周运河, 董梦瑶, 李婕, 汤云灏, 马英, 宋健. H₂-SCR改性铂系催化剂低温脱硝的应用及性能强化挑战[J]. 化工进展, 2023, 42(6): 2954-2962.
[9]	周皞, 张恒, 温妮妮, 王旭瑞, 徐璐, 李玮, 苏亚欣. Cu-SAPO-44分子筛的制备及其C₃H₆-SCR脱硝性能[J]. 化工进展, 2023, 42(3): 1373-1382.
[10]	刘亮, 王朝曦, 李鑫龙, 张高山, 王守阳, 张林林, 陆畅, 卿梦霞. 钒钛系脱硝催化剂抗硫酸氢铵中毒改进措施研究进展[J]. 化工进展, 2023, 42(1): 215-225.
[11]	宋玉昆, 王国刚, 张新功, 刘大阔, 张金庆, 林瀚. SNAR：一种新型非氨基还原除酸脱硝工艺技术[J]. 化工进展, 2022, 41(S1): 606-612.
[12]	张新远, 张柏林, 张深根. 废钒钛系脱硝催化剂碱法回收研究进展[J]. 化工进展, 2022, 41(S1): 580-594.
[13]	马静, 马子然, 林德海, 马少丹, 王宝冬. 活化液助溶剂对再生脱硝催化剂性能的影响[J]. 化工进展, 2022, 41(8): 4173-4180.
[14]	杨希刚, 陈国庆, 黄林滨, 古世军, 李昌松, 张勇, 金保昇. 尿素法SNCR对大型电站煤粉锅炉运行影响的工业试验[J]. 化工进展, 2022, 41(7): 3573-3581.
[15]	杨广东, 苏林, 邹志雪, 姜涛. 微波诱导活性炭激发等离子体射流脱硝实验[J]. 化工进展, 2022, 41(2): 1054-1062.