微波辅助催化氧化苯高性能催化剂实验研究

卜龙利; 张钰彩; 王晓晖; 刘海楠; 张浩

微波辅助催化氧化苯高性能催化剂实验研究

西安建筑科技大学环境与市政工程学院, 陕西西安 710055

基金项目: 陕西省自然科学基金(2009JM7004); 陕西省教育厅省级重点实验室重点科研计划(2010JS027); 西安建筑科技大学基础研究基金(JC0809)。

详细信息

通讯作者:
卜龙利, Tel: 13630232698; E-mail: bolongli@xauat.edu.cn.

中图分类号: X703.1A
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出版历程
- 收稿日期: 2011-10-13
- 修回日期: 2011-12-26
- 刊出日期: 2012-07-31

Preparation and application of high-performance catalyst in microwave assisted catalytic oxidation of benzene

School of Environmental and Municipal Engineering, Xi’an University of Architecture and Technology, Xi’an 710055, China

摘要

摘要: 采用传统浸渍法制备分子筛负载过渡金属和稀土元素催化剂,通过微波辅助催化氧化苯性能实验考察其催化活性。研究表明,天津科密欧的5A分子筛为优良的催化剂载体,分子筛负载铜-锰-铈催化剂对苯的完全燃烧温度为230℃,铜(Cu)锰(Mn)双金属催化剂中晶相与非晶相Cu_1.5Mn_1.5O₄尖晶石提高了催化剂的催化活性,稀土铈(Ce)的助催化效果显著;30 h的连续性实验表明,Cu-Mn-Ce/分子筛催化剂具有良好的稳定性和高的催化活性。催化剂的比表面积和表面形貌表征表明,催化剂比表面积和孔径受高温煅烧和氧化反应而增大,从而有助于苯的吸附与氧化降解;X射线衍射表明,实验前后分子筛结构未发生明显变化,铜锰主要以二价和三价的氧化物形态分布于催化剂表面。
- 微波 /
- 催化氧化 /
- 分子筛负载金属催化剂 /
- 苯
Abstract: High-performance catalyst of molecular sieve supported transition metals and rare earth element was prepared by traditional impregnation method,and the catalytic activity was checked by microwave assisted catalytic oxidation of benzene in our study.It indicated that 5A type molecular sieve obtained from Tianjin kermel was an excellent carrier,and molecular sieve supported copper (Cu),manganese (Mn) and cerium (Ce) catalyst had a complete combustion temperature of 230℃ for benzene.The appearance of Cu_1.5Mn_1.5O₄ with crystalline spinel phase and amorphous phase improved the catalytic activity greatly,and the promoting effect of Ce was also significant.Molecular sieve loaded Cu-Mn-Ce catalyst showed good stability and high catalytic capacity after operating with 30 h.Based on the characteristics of the special surface area and surface morphology,it was found that the special surface area and pore size of the catalyst were enlarged during calcination and reaction,which are beneficial to the adsorption and oxidation of benzene.X-ray diffraction results showed that the crystalline structure of molecular sieve did not change significantly,and CuO and Mn₂O₃ were dispersed mainly onto the surface of the catalyst.
- microwave /
- catalytic oxidation /
- molecular sieve supported metal catalyst /
- benzene

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参考文献(22)

HIROTA K, SAKAI H, WASHIO M, KOJIMA T. Application of electron beams for the treatment of VOC streams[J]. Ind Eng Chem Res, 2004, 43(5): 1185-1191.

LU C-Y, WEY M-Y. Simultaneous removal of VOC and NO by activated carbon impregnated with transition metal catalysts in combustion flue gas[J]. Fuel Process Technol, 2007, 88(6): 557-567.

ANDREEVA D, PETROVA P, SOBCZAK J W, ILIEVA L, ABRASHEV M. Gold supported on ceria and ceria-alumina promoted by molybdena for complete benzene oxidation[J]. Appl Catal B, 2006, 67(3/4): 237-245.

NEDYALKOVA R, ILIEVA L, BERNARD M C, HUGOT-LE GOFF A, ANDREEVA D. Gold supported catalysts on titania and ceria, promoted by vanadia or molybdena for complete benzene oxidation[J]. Mater Chem Phys, 2009, 116(1): 214-218.

宋萃, 陈敏, 张婷, 郑小明. VOCs催化燃烧Pd-Y/不锈钢丝网催化剂的性能)[J]. 无机化学学报, 2009, 25(3): 397-401. (SONG Cui, CHEN Min, ZHANG Ting, ZHENG Xiao-ming. Pd-Y/stainless steel wire mesh catalyst for combustion of volatile organic compounds[J]. Chinese Journal of Inorganic Chemistry, 2009, 25(3): 397-401.)

TAI H S, JOU C H. Application of granular activated carbon packed-bed reactor in microwave radiation field to treat BT[J]. Chemosphere, 1998, 37(11): 2685-2698.

金钦汉, 戴树珊, 黄卡玛. 微波化学[M]. 北京: 科学出版社, 1999. (JIN Qin-han, DAI Shu-shan, HUANG Ka-ma. Microwave chemistry [M]. Beijing: Science Press, 1999.)

段明华, 牟真, 李进军, 解强. Co₃O₄/介孔分子筛催化剂对苯催化完全氧化的研究[J]. 环境工程学报, 2008, 2(8): 1087-1091. (DUAN Ming-hua, MU Zhen, LI Jin-jun, XIE Qiang. Complete catalytic oxidation of benzene on Co₃O₄ catalysts supported on mesoporous molecular sieves [J]. Chinese Journal of Environmental Engineering, 2008, 2(8): 1087-1091.)

张广宏, 季生福, 万会军, 赵福真, 朱吉钦, 李成岳. 铜锰基SBA-15催化剂的制备及其甲苯燃烧消除的催化性能 [J]. 北京化工大学学报, 2008, 35(1): 5-10. (ZHANG Guang-hong, JI Sheng-fu, WAN Hui-jun, ZHAO Fu-zhen, ZHU Ji-qing, LI Cheng-yue. Preparation of CuMn based SBA-15 catalysts and their performance in the catalytic combustion of toluene [J]. Journal of Beijing University of Chemical Technology, 2008, 35(1): 5-10.)

陈敏, 马莹, 宋萃, 张婷, 郑小明. Ce-Pt-Pd/不锈钢丝网催化剂的制备与催化性能[J]. 催化学报, 2009, 30(7): 649-653. (CHEN Min, MA Ying, SONG Cui, ZHANG Ting, ZHENG Xiao-ming. Preparation and performance of Ce-Pt-Pd/stainless steel wire meshes catalyst [J]. Chinese Journal of Catalysis, 2009, 30(7): 649-653.)

解丽丽. 微波加热沸石分子筛特性的研究. 山西: 太原理工大学, 2002: 25-27. (XIE Li-li. Study on the properties of microwave heating zeolites. Shanxi: Taiyuan University of Technology, 2002: 25-27.)

屠兢, 伏义路, 林培琰. Pd/γ-Al₂O₃三效催化剂中CeO₂助剂的作用[J]. 催化学报, 2001, 22(4): 390-396. (TU Jing, FU Yi-lu, LIN Pei-yan. Effect of ceria on Pd/γ-Al₂O₃ three-way catalysts [J]. Chinese Journal of Catalysis, 2001, 22(4): 390-396.)

郭建光, 李忠, 奚红霞, 何莼, 王伯光. CeO₂掺杂对CuO/沸石催化剂催化氧化VOCs 活性的影响[J]. 高校化学工程学报, 2005, 19(6): 776-780. (GUO Jian-guang, LI Zhong, XI Hong-xia, HE Chun, WANG Bo-guang. Effect of ceria doping on the VOCs oxidation activity of CuO/CeO₂/zeolite catalyst [J]. Journal of Chemical Engineering of Chinese Universities, 2005, 19(6): 776-780.)

于强强, 董园园, 廖卫平, 金明善, 何涛, 索掌怀. CeO₂-Al₂O₃负载金催化剂用于水煤气变换反应的催化活性[J]. 燃料化学学报, 2010, 38(2): 223-229. (YU Qiang-qiang, DONG Yuan-yuan, LIAO Wei-ping, JIN Ming-shan, HE Tao, SUO Zhang-huai. Preparation of ceria-alumina and catalytic activity of gold catalyst supported on ceria-alumina for water gas shift reaction[J]. Journal of Fuel Chemistry and Technology, 2010, 38(2): 223-229.)

曹利, 黄学敏, 冯燕. 掺杂CeO₂ 的CuMnOx 复合氧化物催化剂的制备及对甲苯催化燃烧性能研究 [J]. 西安建筑科技大学学报(自然科学版), 2010, 42(5): 729-733. (CAO Li, HUANG Xue-min, FENG Yan. Preparation of CuMnOx catalyst doped ceria and a study on the catalytic property of toluene [J]. Journal of Xi’an University of Architecture & Technology (Natural Science Edition), 2010, 42(5): 729-733.)

TANG X, XU Y, SHEN W. Promoting effect of copper on the catalytic activity of MnO_X-CeO₂ mixed oxide for complete oxidation of benzene[J]. Chem Eng J, 2008, 144(2): 175-180.

李吉花, 蒋毅, 王娟芸, 陈君和, 张志强, 王奂祎. 用于苯催化燃烧的Cu-Mn-O/Ce/γ-Al ₂O₃-Ti O₂催化剂 [J]. 应用化学, 2010, 27(2): 137-141. (LI Ji-hua, JIANG Yi, WANG Juan-yun, CHEN Jun-he, ZHANG Zhi-qiang, WANG Huan-yi. Catalytic combustion of benzene over the Cu-Mn-O/Ce/γ-Al₂O₃ catalysts [J]. Chinese Journal of Applied Chemistry, 2010, 27(2): 137-141.)

VU V H, BELKOUCH J, OULD-DRIS A, TAOUK B.Removal of hazardous chlorinated VOCs over Mn-Cu mixed oxide based catalyst[J]. J Hazard Mater, 2009, 169(1/3): 758-765.

赵福真, 曾鹏晖, 张广宏, 季生福, 李成岳. Cu-Co/SBA-15催化剂的结构特征及其催化甲苯燃烧性能 [J]. 催化学报, 2010, 31(3): 335-342. (ZHAO Fu-zhen, ZENG Peng-hui, ZHANG Guang-hong, JI Sheng-fu, LI Cheng-yue. Structure and catalytic performance of Cu-Co/SBA-15 catalyst for toluene combustion [J]. Chinese Journal of Catalysis, 2010, 31(3): 335-342.)

ZUO S, HUANG Q, LI J, ZHOU R. Promoting effect of Ce added to metal oxide supported on Al pillared clays for deep benzene oxidation[J]. Appl Catal B, 2009, 91(1/2): 204-209.

阳鹏飞, 周继承, 任文明. 微波固相法制备 Cu/ZSM-5催化剂及其催化性能[J]. 南华大学学报, 2010, 24(1): 64-69. (YANG Peng-fei, ZHOU Ji-cheng, REN Wen-ming. Preparati on of Cu/ZSM-5 catalysts by dry reaction under microwave irradiation and their catalytic performances [J]. Journal of University of South China ( Science and Technology), 2010, 24(1): 64-69.)

MORALES M R, BARBERO B P, CADUS L E. Total oxidation of ethanol and propane over Mn-Cu mixed oxide catalysts[J]. Appl Catal B, 2006, 67(3/4): 229-236.

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