Cu的负载方法对CuSAPO-34脱除柴油车尾气中NOx的影响

doi:10.1016/S1872-2067(11)60517-2

催化学报 ›› 2013, Vol. 34 ›› Issue (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NO_x的影响

左永权^a, 韩丽娜^a,b, 鲍卫仁^a, 常丽萍^a, 王建成^a

a 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;
b 太原理工大学材料科学与工程学院,山西太原030024

收稿日期:2012-11-30 修回日期:2012-12-26 出版日期:2013-06-07 发布日期:2013-06-09
通讯作者: 韩丽娜,王建成
基金资助:
国家自然科学基金(20906067);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).

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

ZUO Yongquan^a, HAN Lina^a,b, BAO Weiren^a, CHANG Liping^a, WANG Jiancheng^a

a Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province,Taiyuan University of Technology, Taiyuan 030024, Shanxi, China;
b School of materials science and engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China

Received:2012-11-30 Revised:2012-12-26 Online:2013-06-07 Published:2013-06-09
Supported by:
This work was supported by the National Natural Science Foundation of China (20906067), the Program for the Top Young Academic Leaders of Higher Learning Institutions of Shanxi, and China Postdoctoral Science Foundation (2011M500543).

摘要/Abstract

摘要：

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NO_x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.

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

Abstract:

CuSAPO-34 samples prepared by hydrothermal synthesis (HS), pore-volume impregnation (PVI), and ion-exchange (IE) methods were characterized using X-ray diffraction, scanning electronic microscopy, atomic absorption spectroscopy, temperature-programmed reduction with hydrogen, X-ray absorption near-edge structure spectroscopy, X-ray photoelectron spectroscopy, and N₂ adsorption. The selective catalytic reduction (SCR) ability over CuSAPO-34 for NO_x from a simulated diesel exhaust was investigated through C₃H₆-SCR and NH₃-SCR, before and after aging of the CuSAPO-34 catalyst. The results indicated that the sample prepared by IE had significantly better activity compared with those prepared using HS and PVI, especially in C₃H₆-SCR at temperatures below 300℃. The activity of CuSAPO-34 in NO SCR was affected by the preparation method as a result of changes in the specific area (A_BET), pore-size distribution, and the valence state of the active component. The active component of the catalyst prepared by HS was mainly Cu²⁺, whereas those of samples prepared by IE and PVI were mainly Cu⁺. Aging treatment can destroy the structure of the catalyst, decrease its surface area, and reduce the number of active Cu components on the catalyst surface, leading to a visible decrease in catalytic activity. The CuSAPO-34 prepared using the PVI method had the smallest decrease in NO SCR activity after aging, showing that it had better anti-aging properties.

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

左永权, 韩丽娜, 鲍卫仁, 常丽萍, 王建成. Cu的负载方法对CuSAPO-34脱除柴油车尾气中NO_x的影响[J]. 催化学报, 2013, 34(6): 1112-1122.

ZUO Yongquan, HAN Lina, BAO Weiren, CHANG Liping, WANG Jiancheng. Effect of CuSAPO-34 catalyst preparation method on NO_x removal from diesel vehicle exhausts[J]. Chinese Journal of Catalysis, 2013, 34(6): 1112-1122.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(11)60517-2

https://www.cjcatal.com/CN/Y2013/V34/I6/1112

参考文献

[1] Kaspar J, Fornasiero P, Hickey N. Catal Today, 2003, 77: 419

[2] Farrauto R J, Heck R M. Catal Today, 1999, 51: 351

[3] Mihaylov M, Hadjiivanov K, Panayotov D. Appl Catal B, 2004, 51: 33

[4] Pieterse J A Z, van den Brink R W, Booneveld S, de Bruijn F A. Appl Catal B, 2003, 46: 239

[5] Subbiah A, Cho B K, Blint R J, Gujar A, Price G L, Yie J E. Appl Catal B, 2003, 42: 155

[6] Mosqueda-jimenez B I, Jentys A, Seshan K, Lercher J A. J Catal, 2003, 218: 348

[7] Mosqueda-jimenez B I, Jentys A, Seshan K, Lercher J A. J Catal, 2003, 218: 375

[8] Resini C, Montanari T, Nappi L, Bagnasco G, Turco M, Busca G, Bregani F, Notaro M, Rocchini G. J Catal, 2003, 214: 179

[9] Liu F D, Shan W P, Shi X Y, Zhang C B, He H. Chin J Catal (刘福东,单文坡,石晓燕,张长斌,贺泓), 2011, 32: 1113

[10] Park J H, Park H J, Baik J H, Nam I S, Shin C H, Lee J H, Cho B K, Oh S H. J Catal, 2006, 240: 47

[11] Iwamoto M, Yahiro H, Shundo S, Yu-u Y, Mizuno N. Appl Catal, 1991, 69: L15

[12] Liu H X, Xie Z K, Zhang C F, Chen Q L. Ind Catal (刘红星,谢在库,张成芳,陈庆龄. 工业催化), 2001, 10: 49

[13] Liu Z M, Huang X Y, He C Q, Yang Y, Yang L X, Cai G Y. Chin J Catal (刘中民,黄兴云,何长青,杨越,杨立新,蔡光宇. 催化学报), 1996, 17: 540

[14] Goepper M, Goth F, Delmotte L, Guth J L, Kessler H. Stud Surf Sci Catal, 1989, 49, 857

[15] Ishihara T, Kagawa M, Hadama F, Takita Y. J Catal, 1997, 169: 93

[16] Seker E, Cavataio J, Gulari E, Lorpongpaiboon P, Osuwan S. Appl Catal A, 1999, 183: 121

[17] Haneda M, Kintaichi Y, Hamada H. Appl Catal B, 2001, 31: 251

[18] Chen L, Horiuchi T, Osaki T, Mori T. Appl Catal B, 1999, 23: 259

[19] Haneda M, Kintaichi Y, Shimada H, Hamada H. J Catal, 2000, 192: 137

[20] Liu Z Q, Tang L, Chang L P, Wang J C, Bao W R. Chin J Catal (刘致强,唐磊,常丽萍,王建成,鲍卫仁. 催化学报), 2011, 32: 546

[21] Huang L, Peng F, Wang H J, Yu H, Li Z. Catal Commu, 2009, 10: 1839

[22] Shimokawabe M, Takezawa N, Kobayashi H. Appl Catal B, 1982, 2: 379

[23] Chang F W, Yang H C, Roselin L S, Kuo W Y. Appl Catal A, 2006, 304: 30

[24] Palomares A E, Marquez F, Valencia S, Corma A. J Mol Catal A, 2000, 162: 175

[25] Li X L, Zhang R F. Spectrosc Spect Anal (李兴林,张瑞峰. 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. Appl Surf Sci, 2007, 253: 5062

[27] Alonso F, Melkonian T, Moglie Y, Yus M. Eur J Org Chem, 2011: 2524

[28] Wang B X, Fu Y L. J Mol Catal (China) (王必勋,伏义路. 分子催化), 1996, 10: 81

[29] Wilken N, Wijayanti K, Kamasamudram K, Currier N W, Vedaiyan R, Yezerets A, Olsson L. Appl Catal B, 2011, 111-112: 58

Cu的负载方法对CuSAPO-34脱除柴油车尾气中NO_x的影响

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

PDF

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

[1]	李义磊, 王晓静, 郝影娟, 赵君, 刘英, 穆惠英, 李发堂. 合理设计具有空间分离催化位点的中空立方体顺序材料作为高效的全解水光催化剂[J]. 催化学报, 2021, 42(6): 1040-1050.
[2]	刘晓玲, 陈磊, 许红中, 蒋师, 周瑜, 王军. 直接合成Beta沸石封装Pt纳米粒子用于5-羟甲基糠醛合成2,5-呋喃二甲酸[J]. 催化学报, 2021, 42(6): 994-1003.
[3]	孙传智, 陈葳, 贾轩轩, 刘安鼐, 高飞, 冯帅, 董林. Sm掺杂对Fe₂O₃催化剂NH₃-SCR反应活性及抗水抗硫性作用[J]. 催化学报, 2021, 42(3): 417-430.
[4]	孙丽婧, 杨淼, 曹毅, 田鹏, 吴鹏飞, 曹磊, 徐舒涛, 曾姝, 刘中民. 重构法合成Cu-SAPO-34及其NH₃-SCR催化性能[J]. 催化学报, 2020, 41(9): 1410-1420.
[5]	俞齐军, 李金哲, 危长城, 曾姝, 徐舒涛, 刘中民. 球磨在制备Cs/X型催化剂中的作用以及对甲苯甲醇侧链烷基化反应的影响[J]. 催化学报, 2020, 41(8): 1268-1278.
[6]	刘晓娜, 曹毅, 闫娜娜, 马超, 曹磊, 郭鹏, 田鹏, 刘中民. Cu-SAPO-17:一种新颖的NO_x选择性催化还原催化剂[J]. 催化学报, 2020, 41(11): 1715-1722.
[7]	潘会严, 陈小伟, Oihane Sanz, Miguel A. Cauqui, Jose M. Rodríguez-Izquierdo, Juan J. Delgado. 一步水热法有效调变锰钾矿中钾含量及其对锰钾矿催化剂氧化还原性和催化性能的影响[J]. 催化学报, 2019, 40(6): 940-952.
[8]	张祎旸, 曾慧, 贾斌, 王智华, 刘志明. Pd/TiO₂催化剂上氢气选择性催化还原NO_x的研究[J]. 催化学报, 2019, 40(6): 849-855.
[9]	姚小江, 曹俊, 陈丽, 亢科科, 陈阳, 田密, 杨复沫. MnO_x/CeO₂纳米棒催化剂在低温NH₃-SCR反应中的阳离子(Zr⁴⁺,Al³⁺,Si⁴⁺)掺杂效应[J]. 催化学报, 2019, 40(5): 733-743.
[10]	明淑君, 庞磊, 范驰, 郭文, 董亚浩, 刘鹏, 陈真, 李涛. 柴油机尾气中的碱性无机污染物引起Cu-SAPO-18脱硝催化剂的化学失活[J]. 催化学报, 2019, 40(4): 590-599.
[11]	曹俊, 姚小江, 杨复沫, 陈丽, 傅敏, 汤常金, 董林. Ce⁴⁺,Zr⁴⁺共掺杂提高V₂O₅-WO₃/TiO₂催化剂脱硝性能及抗K中毒能力[J]. 催化学报, 2019, 40(1): 95-104.
[12]	陈传敏, 曹悦, 刘松涛, 陈建猛, 贾文波. 改性钒钛基SCR催化剂的研究进展[J]. 催化学报, 2018, 39(8): 1347-1365.
[13]	赵孟莉, 王婉妮, 黄辰曦, 董旺, 汪洋, 程盛, 王慧庆, 钱海生. 近红外光驱动的UCNPs/Zn_xCd_1-xS纳米复合结构的化学合成并用于光化学还原六价铬[J]. 催化学报, 2018, 39(7): 1240-1248.
[14]	文叶轩, 曹爽, 费晓琦, 王海强, 吴忠标. 一步水热法合成具有(001)高能晶面的SO₄^2--TiO₂及其NH₃-SCR脱硝性能[J]. 催化学报, 2018, 39(4): 771-778.
[15]	盛重义, 麻丁仁, 俞丹青, 肖香, 黄冰洁, 杨柳, 王圣. 低温NH₃-SCR新型MnO_x@TiO₂纳米棒核壳结构催化剂的合成及抗SO₂性能研究[J]. 催化学报, 2018, 39(4): 821-830.

Cu的负载方法对CuSAPO-34脱除柴油车尾气中NOx的影响

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

PDF

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

Cu的负载方法对CuSAPO-34脱除柴油车尾气中NO_x的影响

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