Cu的负载方法对CuSAPO-34脱除柴油车尾气中NOx的影响

催化学报 , 2013, 34(6): 1112-1122. doi: 10.1016/S1872-2067(11)60517-2

Cu的负载方法对CuSAPO-34脱除柴油车尾气中NOx的影响

左永权 ^1, , 韩丽娜 ^2, , 鲍卫仁 ^3, , 常丽萍 ^4, , 王建成 ^5,

1.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024

2.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024;太原理工大学材料科学与工程学院,山西太原030024

3.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024

4.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024

5.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024

基金项目: 山西省高等学校优秀青年学术带头人和中国博士后面上基金(2011M500543).This work was supported by the National Natural Science Foundation of China(20906067) 国家自然科学基金(20906067) the Program for the Top Young Academic Leaders of Higher Learning Institutions of Shanxi,and China Postdoctoral Science Foundation(2011M500543)

关键词： CuSAPO-34 , 水热合成 , 离子交换 , 等体积浸渍 , 选择性催化还原 , 老化

Effect of CuSAPO-34 catalyst preparation method on NOx removal from diesel vehicle exhausts

ZUO Yongquan ^1, , HAN Lina ^2, , BAO Weiren ^3, , CHANG Liping ^4, , WANG Jiancheng ^5,

1.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024

2.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024;太原理工大学材料科学与工程学院,山西太原030024

3.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024

4.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024

5.太原理工大学煤科学与技术山西省和教育部重点实验室,山西太原030024

Keywords： CuSAPO-34 , Hydrothermal synthesis , Ion-exchange , Pore volume impregnation , Selective catalytic reduction , Aging

采用X射线衍射、扫描电镜、原子吸收、程序升温还原、X射线吸收近边吸收谱、X射线光电子能谱、氮吸附等手段对水热合成(HS)、等体积浸渍(PVI)与离子交换(IE)法制备的CuSAPO-34样品进行了表征,并评价了老化前后催化剂上C3H6-SCR与NH3-SCR脱除模拟柴油车尾气中NOx的反应活性.结果表明,IE法制得的催化剂活性最高,尤其在C3H6-SCR低温阶段；PVI法制得的催化剂活性最差.制备方法影响CuSAPO-34催化剂的比表面积、孔径分布和活性组分价态从而改变其催化活性.各催化剂均存在Cu+和Cu2+,但比例明显不同.HS样品以Cu2+为主,另两种样品则含较多的Cu+.老化不仅部分破坏了分子筛的形貌、降低了分子筛的比表面积,尤其是表面Cu含量,而且有部分Cu生成了CuSO4,使得老化后催化剂的脱硝活性降低.PVI法制得的催化剂老化后活性下降幅度最小,表明该分子筛抗老化能力较强.

参考文献

[1]	Kaspar J;Fornasiero P;Hickey N .[J].Catalysis Today,2003,77:419.
[2]	Farrauto R J;Heck R M .[J].Catalysis Today,1999,51:351.
[3]	Mihaylov M;Hadjiivanov K;Panayotov D .[J].Applied Catalysis B:Environmental,2004,51:33.
[4]	Pieterse J A Z;van den Brink R W;Booneveld S;de Bruijn F A .[J].Applied Catalysis B:Environmental,2003,46:239.
[5]	Subbiah A;Cho B K;Blint R J;Gujar A Price G L Yie J E .[J].Applied Catalysis B:Environmental,2003,42:155.
[6]	Mosqueda-Jimenez BI.;Jentys A.;Seshan K.;Lercher JA. .Structure-activity relations for Ni-containing zeolites during NO reduction - I. Influence of acid sites[J].Journal of Catalysis,2003(2):348-353.
[7]	Mosqueda-Jimenez BI.;Jentys A.;Seshan K.;Lercher JA. .Structure-activity relations for Ni-containing zeolites during NO reduction - II. Role of the chemical state of Ni[J].Journal of Catalysis,2003(2):375-385.
[8]	Resini C;Montanari T;Nappi L;Bagnasco G Turco M Busca G Bregani F Notaro M Rocchini G .[J].Journal of Catalysis,2003,214:179.
[9]	刘福东;单文坡;石晓燕;张长斌,贺泓 .[J].,2011,32:1113.
[10]	Park JH;Park HJ;Baik JH;Nam IS;Shin CH;Lee JH;Cho BK;Oh SH .Hydrothermal stability of CuZSM5 catalyst in reducing NO by NH3 for the urea selective catalytic reduction process[J].Journal of Catalysis,2006(1):47-57.
[11]	Iwamoto M;Yahiro H;Shundo S;Yu-u Y Mizuno N .[J].Applied Catalysis,1991,69:L15.
[12]	刘红星;谢在库;张成芳;陈庆龄 .[J].工业催化,2001,10:49.
[13]	刘中民;黄兴云;何长青;杨越杨立新蔡光宇 .[J].催化学报,1996,17:540.
[14]	Goepper M;Goth F;Delmotte L;Guth J L Kessler H .[J].Studies in surface science and catalysis,1989,49:857.
[15]	Ishihara T.;Hadama F.;Takita Y.;Kagawa M. .COPPER ION-EXCHANGED SAPO-34 AS A THERMOSTABLE CATALYST FOR SELECTIVE REDUCTION OF NO WITH C3H6[J].Journal of Catalysis,1997(1):93-102.
[16]	Seker E;Cavataio J;Gulari E;Lorpongpaiboon P Osuwan S .[J].Applied Catalysis A:General,1999,183:121.
[17]	Haneda M.;Hamada H.;Kintaichi Y. .Effect of SO2 on the catalytic activity of Ga2O3-Al2O3 for the selective reduction of NO with propene in the presence of oxygen[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2001(4):251-261.
[18]	Chen L;Horiuchi T;Osaki T;Mori T .[J].Applied Catalysis B:Environmental,1999,23:259.
[19]	Haneda M.;Shimada H.;Hamada H.;Kintaichi Y. .Selective reduction of NO with propene over Ga2O3-Al2O3: Effect of sol-gel method on the catalytic performance[J].Journal of Catalysis,2000(1):137-148.
[20]	刘致强,唐磊,常丽萍,王建成,鲍卫仁.Cu-SAPO-34/堇青石的原位制备及其催化丙烷还原柴油机车尾气中NOx[J].催化学报,2011(04):546-554.
[21]	Huang L;Peng F;Wang H J;Yu H Li Z .[J].Catal Commu,2009,10:1839.
[22]	Shimokawabe M;Takezawa N;Kobayashi H .[J].Applied Catalysis B:Environmental,1982,2:379.
[23]	Chang FW;Yang HC;Roselin LS;Kuo WY .Ethanol dehydrogenation over copper catalysts on rice husk ash prepared by ion exchange[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(1):30-39.
[24]	Palomares A E;Marquez F;Valencia S;Corma A .[J].Journal of Molecular Catalysis A:Chemical,2000,162:175.
[25]	李兴林;张瑞峰 .[J].光谱学与光谱分析,1996,16:119.
[26]	Lopez M C;Galiana B;Algora C;Rey-Stolle I Gabas M Ramos-Barrado J R .[J].ApplSurfSci,2007,253:5062.
[27]	Alonso, F.;Melkonian, T.;Moglie, Y.;Yus, M. .Homocoupling of terminal alkynes catalysed by ultrafine copper nanoparticles on titania[J].European journal of organic chemistry,2011(13):2524-2530.
[28]	王必勋;伏义路 .[J].分子催化,1996,10:81.
[29]	Wilken N;Wijayanti K;Kamasamudram K;Currier N W Vedaiyan R Yezerets A Olsson L .[J].Applied Catalysis B:Environmental,2011,111-112:58.

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