Cu/Dy/S2O82-/Al-PILR催化剂制备及其选择催化还原 NO

郭锡坤; 李式伟; 郭伟斌

Cu/Dy/S₂O₈^2-/Al-PILR催化剂制备及其选择催化还原 NO

1.
汕头大学理学院, 广东汕头 515063;
2.
汕头大学医学院第一附属医院, 广东汕头 515041

基金项目: 广东省科技计划项目(2006B36702003)。

详细信息

通讯作者:
郭伟斌(1974-),男,高级工程师,参加计算机技术在化学工程的应用研究,Ted:0754-88282806,E-mail:gwbok@163.com。

中图分类号: O634.3
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出版历程
- 收稿日期: 2011-11-03
- 修回日期: 2012-01-28
- 刊出日期: 2012-09-29

Preparation of Cu/Dy/S₂O₈^2-/Al-PILR catalyst and its catalytic performance for selective reduction of NO

1.
College of Science, Shantou University, Shantou 515063, China;
2.
The First Affiliated Hospital of Shantou University Medical Collage, Shantou 515041, China

摘要

摘要: 采用累托土为原料,合成铝交联累托土 (Al-PILR),然后分步浸渍负载 (NH₄)₂S₂O₈、Dy(NO₃)₃和 Cu(NO₃)₂,制成 Cu/Dy/S₂O₈^2-/Al-PILR催化剂。考察该催化剂对 C₃H₆选择性还原 NO的催化性能,并且利用低角 XRD、BET、Py-IR、IR、TG和SEM等方法,研究催化剂结构与性能的关系。实验结果表明,铝交联剂能很好地撑开累托土的土层,显著增大催化剂的比表面积; S₂O₈^2-能明显增加铝交联累托土B(Brönsted)酸的酸量; Dy能进一步增加B酸的酸量,有效提高催化活性和热稳定性。因此, Cu/Dy/S₂O₈^2-/Al-PILR催化剂具有良好的催化性能, 最佳催化活性温度为300℃,NO转化率高达80.3%,在有10%水蒸气存在的情况下仍可达77.6%。
- S₂O₈^2-改性 /
- 镝 /
- 铝交联累托土 /
- NO /
- 选择性还原
Abstract: By using rectorite as raw materials, the Al-pillared rectorite(Al-PILR) was synthetized, then the Cu/Dy/S₂O₈^2-/Al-PILR catalyst was prepared by loading of (NH₄)₂S₂O₈, Dy(NO₃)₃ and Cu(NO₃)₂ onto the Al-pillared rectorite step by step. The catalytic performance of the Cu/Dy/S₂O₈^2-/Al-PILR catalyst on the selective catalytic reduction of NO with propylene was investigated. The relationship between the structure and the performance of the Cu/Dy/S₂O₈^2-/Al-PILR catalyst was also explored by means of Low-angle X-ray diffraction (LAXRD), Surface area measurements (BET), Pyridine absorption infared spectrum (Py-IR), Infrared spectroscopy (IR), Thermal gravimetric analysis (TG) and Scanning electron microscope (SEM). The experimental results indicated that the Al pillaring agent could effectively insert into the layer of rectorite and remarkably enlarge the specific surface area, and S₂O₈^2- could obviously increase the Brönsted acid amount of the Al-pillared rectorite, Dy could further increase the Brönsted acid amount to improve the catalytic activity and thermal stability effectively. Therefore, the Cu/Dy/S₂O₈^2-/Al-PILR catalyst exhibited excellent catalytic performance. The NO conversion was up to 80.3% at 300℃ and 77. 6% even at the presence of 10% volume fraction of water vapor.
- S₂O₈^2-modification /
- Dy /
- Al-pillared rectorite /
- NO /
- selective reduction

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参考文献(24)

陈树伟, 闫晓亮, 陈佳琪, 马静红, 李瑞丰. 富氧条件下Mn/ZSM-5选择催化 CH₄还原 NO[J]. 催化学报, 2010, 31(9): 1107-1114. (CHEN Shu-wei, YAN Xiao-liang, CHEN Jia-qi, MA Jing-hong, LI Rui-feng. Selective catalytic reduction of NO in excess oxygen by methane over Mn/ZSM-5 catalysts[J]. Chinese Journal of Catalysis, 2010, 31(9): 1107-1114.)

吴大旺, 张秋林, 林涛, 龚茂初, 陈耀强. Ce_xTi_1-xO₂ 负载锰基催化剂的制备及其低温 NH₃选择催化还原 NO[J]. 无机化学学报, 2011, 27(1): 53-60. (WU Da-wang, ZHANG Qiu-lin, LIN Tao, GONG Mao-chu, CHEN Yao-qiang. Ce_xTi_1-xO₂ Supported manganese-based catalyst: Preparation and catalytic performance for selective reduction of NO with NH₃ at lower temperature[J]. Chinese Journal of Inorganic Chemistry, 2011, 27(1): 53-60.)

陆光. 柱层粘土催化剂上丙烯选择还原 NO反应的研究. 大连: 大连理工大学,2011. (LU Guang. Selective reduction of NO with C₃H₆ over Cu-Ti-PILC Catalysts.Dalian:Dalian Uiversity of Technology, 2011.)

IWAMOTO M, HAMADA H. Removal of nitrogen monoxide from exhaust gases through novel catalylic processes[J]. Catal Today, 1991,10(1): 57-71.

王琪莹, 文炎柄, 董新法, 林维明. 交联粘土合成及其在 C₃H₆选择性催化还原 NOx中的应用研究 [J]. 高校化学工程学报, 2006, 20(4): 598-603. (WANG Qi-ying, WEN Yan-bing, DONG Xin-fa, LIN Wei-ming. Application of pillaerd clays inselective catalytic reduction of NOx by C₃H₆[J]. Journal of Chemical Engineering of Chinese Universities, 2006, 20(4): 598-603.)

朱永青, 李俊华, 康守方, 李临生, 王建昕. 稀燃汽油机 Ag/Al₂O₃催化剂上选择性还 NOx[J]. 清华大学学报(自然科学版), 2007, 47(3): 361-364. (ZHU Yong-qing, LI Jun-hua, KANG Shou-fang, LI Lin-sheng,WANG Jian-xin. Selective catalytic reduction of NOx on Ag/Al₂O₃ catalyst in lean-burn gasoline engines[J]. Journal of Tsinghua University(Science and Technology), 2007, 47(3): 361-364.)

GANEMI B, BJORNBOM E, DEMIVEL B. Zeolite Cu-ZSM-5: Material characteristics and NO decomposition[J]. Microporous Mesoporous Mater, 2000, 38(2/3): 287-300.

DORADO F, LUCAS A D, GARCFA P B, ROMERO A,VALVERDE J L. Copper ion-exchanged and impregnated Fe-pillared clays: Study of the influence of the synthesis conditions on the activity for the selective catalytic reduction of NO with C₃H₆[J]. App Catal A, 2006, 305 (2): 189-196.

LIN Q, HAO J, LI J, MA Z, LIN W.Copper-impregnated Al-Ce-pillared clay for selective catalytic reduction of NO by C₃H₆[J].Catal Today, 2007, 126 (3/4): 351-358.

文焱炳, 董新法, 林维明. Cu/Ce-Ti-PILC上丙烯选择催化还原 NO的研究 [J]. 广州大学学报(自然科学版), 2008, 7(1): 53-57. (WEN Yan-bing, DONG Xin-fa, LIN Wei-ming. Study on Cu/Ce-Ti-PILC for selective catalytic reduction of NO by propylene[J].Journal of Guangzhou University(Natural Science Edition), 2008, 7(1): 53-57.)

DORADO F, GARCFA P B, LUCAS A D, RAMOS M J, ROMERO A. Hydrocarbon selective catalytic reduction of NO over Cu/Fe-pillared clays: Diffuse reöectance infrared spectroscopy studies[J]. J Mol Catal A, 2010, 332(1/2): 45-52.

叶青, 闫立娜, 霍飞飞, 王海平, 程水源, 康天放. Cu 负载 Fe 柱撑钠化海泡石: 结构特点及其丙烯选择性催化还原NO性质研究[J]. 化学学报, 2011, 69(13): 1524-1532. (YE Qing, YAN Li-na, HUO Fei-fei, WANG Hai-ping, CHENG Shui-yuan, KANG Tian-fang. Copper impregnated Fe-pillared sodium-treated sepiolite(Fe-NaPILCS) for selective catalytic reduction of NO with C₃H₆[J]. Acta Chimica Sinica, 2011, 69(13): 1524-1532.)

CIAMBELLI P, CORBO P, MIGLIARDINI F. Potentiatities and limitations of lean de-NO_x catalysts in reducing automotive exhaust emissions[J]. Catal Today, 2000, 59(3/4): 279-286.

DATKA J, TUREK A M, JEHNG J M, WACHS I E. Acidic properties of supported niobium oxide catalysts: An infrared spectroscopy investigation[J]. J Catal, 1992,135(1):186-199.

尹元根. 多相催化剂的研究方法 [M]. 北京: 化学工业出版社, 1988: 582-584. (YIN Yuan-Gen. Research methods of heterogeneous catalysts[M]. Beijing: Chemical Industry Press, 1988: 582-584.)

谭宇新. 贫燃条件下汽车尾气净化催化剂的研究.广州: 华南理工大学, 2000. (TAN Yu-xin. Study on automobile exhaust catalyst under lean-burn conditions. Guangzhou: South China University of Technology, 2000.)

JUNG S M, GRANGE P. Characterization and reactivity of pure TiO₂-SO₄^2-SCR catalyst: Influence of SO₄^2-content[J]. Catal Today, 2000, 59(3/4): 305-312.

YANG R T, THARAPPIWATTANANON N, LONG R Q. Lon-exchanged pillared clays for selective catalytic reduction of NO by ethylene in the presence of oxygen[J]. Appl Catal B, 1998, 19(3/4): 289-304.

赵东源, 杨亚书, 辛勤, 张慧, 郭燮贤. 柱撑粘土分子筛的红外光谱研究 [J]. 光谱学与光谱分析, 1994, 14(4): 27-30. (ZHAO Dong-yu, YANG Ya-shu,XIN Qin,ZHANG Hui,GUO Xie-xian. Studies on the IR spectra of the pillared clay molecular sieve[J]. Speetroseopy and Spectral Analysis, 1994, 14(4): 27-30.)

高根之, 于世涛, 杨锦京. SO₄^2-/TiO₂-Al₂O₃-SnO₂ 催化剂的研制及其催化合成己二酸二辛酯[J]. 催化学报, 1996, 17(1): 83-86. (GAO Gen-zhi, YU Shi-tao, YANG Jin-zong. Preparation of SO₄^2-/TiO₂-Al₂O₃-SnO₂and its catalytic properties for the synthesis of dioctyl adipate[J]. Chinese Journal of Catalysis, 1996, 17(1): 83-86.)

张斌, 周永元. 淀粉接枝共聚反应中引发剂的研究状况与进展 [J]. 高分子材料科学与工程, 2007, 23(2): 36-40. (ZHANG Bin, ZHOU Yong-yuan. Development of initiators in graft copolymerization of acrylic monomers onto starch[J].Polymer Materials Science and Engineering, 2007, 23(2): 36-40.)

YADAV D, NAIR J. Sulfated zirconia and its modified versions as promising catalysts for industrial processes[J]. Microporous Mesoporous Mater, 1999, 33(1/3): 1-48.

李来生, 吴少林, 刘至力. SO₄^2-/Fe₂O₃-Dy₂O₃催化α-萘乙酸与甲醇酯化反应的色谱法研究[J]. 化学研究与应用, 1996, 8(4): 531-534. (LI Lai-sheng, WU Shao-lin, LIU Zhi-li. The study on SO₄^2-/Fe₂O₃-Dy₂O₃ for catalytic esterification of α-naphthyl-acetic acid and methanol by high performanc eliquid chromatography[J]. Chemical Research and Application, 1996, 8(4): 531-534.)

SRINIVASAN R, KEOGH R A, MIBURN D R, DAVIS B H. Sulfated zirconia catalysts: Characterization by TGA/DTA mass spectrometry [J]. J Catal, 1995, 153(1): 123~130.

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Cu/Dy/S₂O₈^2-/Al-PILR催化剂制备及其选择催化还原 NO

通讯作者:
郭伟斌(1974-),男,高级工程师,参加计算机技术在化学工程的应用研究,Ted:0754-88282806,E-mail:gwbok@163.com。

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Preparation of Cu/Dy/S₂O₈^2-/Al-PILR catalyst and its catalytic performance for selective reduction of NO

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