不同类型含铁分子筛上N2O催化分解反应

催化学报 , 2013, 34(5): 876-888. doi: 10.1016/S1872-2067(12)60555-5

不同类型含铁分子筛上N2O催化分解反应

王俊英 ^1, , 夏海岸 ^2, , 鞠晓花 ^3, , 范峰滔 ^4, , 冯兆池 ^5, , 李灿 ^6,

1.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023;中国科学院大学,北京100049

2.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

3.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

4.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

5.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

6.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

基金项目: the National Natural Science Foundation of China(21173213) 国家重点基础研究发展计划(973计划,2009CB623507) 国家自然科学基金(21173213) the National Basic Research Program of China(973Program,2009CB623507)

关键词：铁 , 分子筛 , 氧化亚氮分解 , 拉曼光谱

Catalytic performance of different types of iron zeolites in N2O decomposition

WANG Junying ^1, , XIA Haian ^2, , JU Xiaohua ^3, , FAN Fengtao ^4, , FENG Zhaochi ^5, , LI Can ^6,

1.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023;中国科学院大学,北京100049

2.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

3.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

4.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

5.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

6.中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

Keywords： Iron , Zeolite , Nitrous oxide decomposition , Raman spectroscopy

采用固态离子交换法制备了一系列Fe/Al摩尔比为0.33的Fe/分子筛(ZSM-35,ZSM-5,beta和mordenite(丝光沸石))样品,并利用紫外-可见漫反射光谱、原位红外光谱和可见拉曼光谱以及瞬态应答实验考察了分子筛种类对N2O分解反应性能的影响.研究表明,经高温处理(HT)后分子筛的催化活性顺序为Fe/ZSM-35＞ Fe/beta＞ Fe/ZSM-5＞ Fe/mordenite,与骨架外铝稳定的双核铁物种含量一致.这说明双核铁物种是高温处理后Fe/分子筛样品中N2O分解的活性位,而它的形成与分子筛种类密切相关.Fe/ZSM-35分子筛十元环孔道中相邻两个α位和八元环孔道中相邻两个β位都能稳定两个Fe(Ⅱ)离子而形成能高效分解N2O的双核铁活性中心.Fe/beta和Fe/ZSM-5分子筛中只有落在相邻两个β位上的两个Fe(Ⅱ)离子才能形成参与N2O分解的高活性的双铁活性中心.Fe/mordenite-HT分子筛上的铁物种绝大部分以孤立Fe离子的形式存在,因此其催化N2O分解反应活性很低.

参考文献

[1]	Pérez-Ramírez J;Kapteijn F;Sch(o)ffel K;Moulijn J A .[J].Applied Catalysis B:Environmental,2003,44:117.
[2]	Pérez-Ramírez J;Kapteijn F;Mul G;Xu X Moulijn J A .[J].Catalysis Today,2002,76:55.
[3]	Parmon V N;Panov G I;Uriarte A;Noskov A S .[J].Catalysis Today,2005,100:115.
[4]	Hansen N;Heyden A;Bell A T;Keil F J .[J].Journal of Catalysis,2007,248:213.
[5]	Pirngruber GD;Roy PK;Prins R .The role of autoreduction and of oxygen mobility in N2O decomposition over Fe-ZSM-5[J].Journal of Catalysis,2007(1):147-157.
[6]	Roy P K;Prins R;Pirngruber G D .[J].Applied Catalysis B:Environmental,2008,80:226.
[7]	(Φ)ygarden A H;Pérez-Ramírez J .[J].Applied Catalysis B:Environmental,2006,65:163.
[8]	Kaucky D;Sobalik Z;Schwarze M;Vondrova A;Wichterlova B .Effect of FeH-zeolite structure and Al-Lewis sites on N2O decomposition and NO/NO2-assisted reaction[J].Journal of Catalysis,2006(2):293-300.
[9]	Jí(s)a K;Nováková J;Schwarze M;Vondrová A Sklenák S Sobalik Z .[J].Journal of Catalysis,2009,262:27.
[10]	Sklenák S;Andrikopoulos P C;Boekfa B;Jansang B Nováková J Benco L Bucko T Hafner J Děde(c)ek J Sobalík Z .[J].Journal of Catalysis,2010,272:262.
[11]	Pantu P;Boekfa B;Sunpetch B;Limtrakul J .[J].Chemical Engineering Communications,2008,195:1477.
[12]	Pérez-Ramírez J;Groen J C;Brückner A;Kumar M S Bentrup U Debbagh M N Villaescusa L A .[J].Journal of Catalysis,2005,232:318.
[13]	Melián-Cabrera I;Mentruit C;Pieterse J A Z;van den Brink R W Mul G Kapteijn F Moulijn J A .[J].CATALYSIS COMMUNICATIONS,2005,6:301.
[14]	Xia HA;Sun KQ;Fan FT;Sun KJ;Su WG;Feng ZC;Ying PL;Li C .Effect of extra-framework gallium on the structure of iron species in Fe/ZSM-5[J].Journal of Catalysis,2008(2):269-275.
[15]	Děde(c)ek J;Kauck(y) D;Wichterlová B .[J].Microporous and Mesoporous Materials,2000,35-36:483.
[16]	Sobalík Z;Děde(c)ek J;Kauck(y) D;Wichterlová B Drozdová L Prins R .[J].Journal of Catalysis,2000,194:330.
[17]	Děde(c)ek J;(C)apek L;Kauck(y) D;Sobalíl Z Wichterlová B .[J].Journal of Catalysis,2002,211:198.
[18]	Drozdová L;Prins R;Děde(c)ek J;Sobalík Z Wichterlová B .[J].Journal of Physical Chemistry B,2002,106:2240.
[19]	Děde(c)ek J;Wichterlová B .[J].Journal of Physical Chemistry B,1999,103:1462.
[20]	Atffield M P;Weigel S J;Cheetham A K .[J].Journal of Catalysis,1997,170:227.
[21]	Dalconi M C;Cruciani G;Alberti A;Ciambelli P Rapacciuolo M T .[J].Microporous and Mesoporous Materials,2000,39:423.
[22]	Sun K Q;Xia H A;Feng Zh Ch;van Santen R Hensen E J M Li C .[J].Journal of Catalysis,2008,254:383.
[23]	Wang J Y;Li G N;Ju X H;Xia H A Fan F T Wang J H Feng Zh Ch Li C .[J].Journal of Catalysis,2013,301:77.
[24]	Kumar MS;Schwidder M;Grunert W;Bruckner A .On the nature of different iron sites and their catalytic role in Fe-ZSM-5 DeNO(x) catalysts: new insights by a combined EPR and UV/VIS spectroscopic approach[J].Journal of Catalysis,2004(2):384-397.
[25]	Pérez-Ramírez J .[J].Journal of Catalysis,2004,227:512.
[26]	Pérez-Ramírez J;Kumar M S;BrücknerA .[J].Journal of Catalysis,2004,223:13.
[27]	Pérez-Ramírez J;Mul G;Kapteijn F;Moulijn J A Overweg A R Doménech A Ribera A Arends I W C E .[J].Journal of Catalysis,2002,207:113.
[28]	Bordiga S.;Geobaldo F.;Lamberti C.;Giamello E.;Zecchina A. Leofanti G.;Petrini G.;Tozzola G.;Vlaic G.;Buzzoni R. .STRUCTURE AND REACTIVITY OF FRAMEWORK AND EXTRAFRAMEWORK IRON IN FE-SILICALITE AS INVESTIGATED BY SPECTROSCOPIC AND PHYSICOCHEMICAL METHODS[J].Journal of Catalysis,1996(2):486-501.
[29]	Hadjiivanov K;Ivanova E;Kefirov R;Janas J Plesniar A Dzwigaj S Che M .[J].Microporous and Mesoporous Materials,2010,131:1.
[30]	Hensen E J M;Zhu Q;van Santen R A .[J].Journal of Catalysis,2003,220:260.
[31]	Long J L;Zhang Z Zh;Ding Zh X;Ruan R Sh Li Zh H Wang X X .[J].J Phys Chem C,2010,114:15713.
[32]	Lobree LJ.;Reimer JA.;Bell AT.;Hwang IC. .An in situ infrared study of NO reduction by C3H8 over Fe-ZSM-5[J].Catalysis Letters,1999(3/4):233-240.
[33]	Yuranov I;Bulushev DA;Renken A;Kiwi-Minsker L .Benzene to phenol hydroxylation with N2O over Fe-Beta and Fe-ZSM-5: Comparison of activity per Fe-site[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2007(0):128-136.
[34]	Xia H A;Sun K Q;Sun K J;Feng Zh Ch Li W X Li C .[J].J Phys Chem C,2008,112:9001.
[35]	Li C;Xiong G;Xin Q;Liu J K,Ying P L,Feng Zh Ch,Li J,Yang W B,Wang Y Zh,Wang G R,Liu X Y,Lin M,Wang X Q,Min E Z .[J].AngewChem Int Ed,1999,38:2220.
[36]	范峰滔,徐倩,夏海岸,孙科举,冯兆池,李灿.催化材料的紫外拉曼光谱研究[J].催化学报,2009(08):717-739.
[37]	Nosheen S;Galasso F;Suib S L .[J].SciAdv Mater,2009,1:31.
[38]	Twu J;Dutta P K;Kresge C T .[J].Journal of Physical Chemistry,1991,95:5267.
[39]	Dutta P K;Rao K M;Park J Y .[J].Journal of Physical Chemistry,1991,95:6654.
[40]	Fan F T;Feng Zh Ch;Li C .[J].Accounts of Chemical Research,2010,43:378.
[41]	Yu Y;Xiong G;Li C;Xiao F-Sh .[J].Microporous and Mesoporous Materials,2001,46:23.
[42]	de Faria D L A;Venaüncio Silva S;de Oliveira M T .[J].Journal of Raman Spectroscopy,1997,28:873.
[43]	Tosheva L;Mihailova 8;Valtchev V;Sterte J .[J].Microporous and Mesoporous Materials,2001,48:31.
[44]	Lewandowska A E;Banares M A;Tielens F;Che M Dzwigaj S .[J].J Phys Chem C,2010,114:19771.
[45]	Dutta P K;Rao K M;Park J Y .[J].LANGMUIR,1992,8:722.
[46]	Suzuki Y;Wakihara T;Itabashi K;Ogura M Okubo T .[J].Topics in Catalysis,2009,52:67.
[47]	Mihailova B;Valtchev V;Mintova S;Faust A-C Petkov N Bein T .[J].Physical Chemistry Chemical Physics,2005,7:2756.
[48]	Majano G;Mintova S;Ovsitser O;Mihailova B Bein T .[J].Microporous and Mesoporous Materials,2005,80:227.
[49]	Fan F T;Sun K J;Feng Zh Ch;Xia H A Han B Lian Y X Ying P L Li C .[J].Chemistry-A European Journal,2009,15:3268.
[50]	Dědecěk J;Kauck(y) D;Wichterlová B .[J].Topics in Catalysis,2002,18:283.
[51]	Kaucky D.;Dedecek J.;Wichterlova B.;Vondrova A. .Activity of Co ion sites in ZSM-5, ferrierite, and mordenite in selective catalytic reduction of NO with methane[J].Journal of Catalysis,2000(2):318-329.
[52]	Kapteijn F;Rodriguez-Mirasol J;Moulijn J A .[J].Applied Catalysis B:Environmental,1996,9:25.
[53]	Dědecěk J;Kauck(y) D;Wichterlová B;Gonsiorová O .[J].Physical Chemistry Chemical Physics,2002,4:5406.

上一张下一张

计量

下载量()
访问量()

作者相关

文章评分

您的评分：
1

0%
2

0%
3

0%
4

0%
5

0%

材料期刊网