过渡金属对分子筛担载Pd催化剂上CO氧化性能影响

化学学报 ›› 2004, Vol. 62 ›› Issue (20): 1981-1987. 上一篇下一篇

研究论文

过渡金属对分子筛担载Pd催化剂上CO氧化性能影响

毕玉水, 吕功煊

中国科学院兰州化学物理研究所, 羰基合成与选择氧化国家重点实验室, 兰州, 730000

投稿日期:2004-03-22 修回日期:2004-06-17 发布日期:2014-02-17
通讯作者: 吕功煊,E-mail:gxlu@ns.lzb.ac.cn;Tel:0931-4968178;Fax:0931-4968178. E-mail:gxlu@ns.lzb.ac.cn
基金资助:
国家重点基础研究发展规划(№.G20000264)资助项目.

Influences of Transition Metal Additives on CO Oxidation over NaZSM-5 Supported Pd

BI Yu-Shui, LÜ Gong-Xuan

State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000

Received:2004-03-22 Revised:2004-06-17 Published:2014-02-17

文章分享

摘要/Abstract

分别采用共浸和连续浸渍法制备了一系列添加过渡金属的Pd-M-O_x-NaZSM-5(M=Cr,Mn,Fe,Co,Ni,Cu,Zn,Mo,Zr等)负载型催化剂.以CO氧化为探针反应,考察了不同制备方法对CO氧化性能影响,结果表明共浸法制备的各催化剂其活性明显优于连续浸渍法.详细考察了反应温度、Fe含量、氢气预还原、空速以及水蒸气等对共浸Pd-Fe-O_x/NaZSM-5催化剂上CO氧化行为影响,并应用XRD和XPS等手段对催化剂体相结构和表面状态进行了表征.结果表明:加入Fe₂O₃可明显提高Pd/NaZSM-5催化剂活性,且催化CO氧化的转化率随反应温度及Fe含量增加而增加;空速增加以及H₂预还原作用导致Pd-Fe-O_x/NaZSM-5活性有所降低;催化剂对水蒸气较为敏感.XRD测试结果表明催化剂中Pd组分处于较高分散状态,以红铁矿形式存在的Fe₂O₃的引入,促进了Pd物种在NaZSM-5载体上的分散.表面XPS分析证实Fe₂O₃与Pd物种间存在较强的相互协同作用,且催化剂表面Pd物种处于较高氧化状态.Pd的高分散及其与Fe₂O₃的相互协同作用是共浸催化剂具有高活性的关键因素.

关键词: 过渡金属, Pd-Fe-O_x/NaZSM-5, 负载型催化剂, 低温, CO氧化

A series of transition metal-modified Pd-M-O_x-NaZSM-5 (M=Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Zr) catalysts were prepared by co-impregnation and sequential impregnation methods separately. Influences of different preparation methods on CO oxidation have been studied. It was found that catalysts prepared by co-impregnation method were superior to those of the sequential one. Effects of temperature, content of the promoter, H₂ pre-reduction, space velocity and moisture in the feed gas on Pd-Fe-O_x/NaZSM-5 catalyst prepared by co-impregnation method for CO oxidation have been investigated in detail. XRD and XPS techniques were used to verify the species in the catalyst. The addition of Fe₂O₃ obviously improved the activity and CO conversion increased with the increase of reaction temperature or Fe-loading amount. However, high space velocity as well as H₂ pre-reduction decreased the activity. The catalyst was sensitive to moisture and its activity was easily depressed by moisture in the feed gas. XRD showed that Pd species were highly dispersed on the surface of NaZSM-5, which was dependent upon the Fe-loading amount of hematite. XPS profiles revealed the presence of synergism between Fe₂O₃ and Pd species, and the Pd species kept a high oxidation state in the special structure of NaZSM-5. High dispersion of the Pd species as well as the synergism between Fe and the Pd species was responsible for the enhancement of catalytic activity.

Key words: transition metal, Pd₂Fe₂O_x/NaZSM-5, supported catalyst, low temperature, CO oxidation

引用此文

毕玉水, 吕功煊. 过渡金属对分子筛担载Pd催化剂上CO氧化性能影响[J]. 化学学报, 2004, 62(20): 1981-1987.

BI Yu-Shui, LÜ Gong-Xuan. Influences of Transition Metal Additives on CO Oxidation over NaZSM-5 Supported Pd[J]. Acta Chimica Sinica, 2004, 62(20): 1981-1987.

导出引用 EndNote|Reference Manager|ProCite|BibTeX|RefWorks

分享此文

参考文献

[1] Yuan, Y.; Kozlova, A. P.; Asakura, K.; Wan, H.; Tsai,K.; Iwasawa, Y. J. Catal. 1997, 170, 191.
[2] Wolf, A.; Schuth, F. Appl. Catal. A: General 2002, 226, 1.
[3] Manasilp, A.; Gulari, E. Appl. Catal. B: Enviromental 2002,37, 17.
[4] Hoffmann, J.; Meusel, I.; Hartmann, J.; Libuda, J.; Freund,H.-J. J. Catal. 2001, 204,378.
[5] Gadgil, M. M.; Sasikala, R.; Kulshreshtha, S. K. J. Mol.Catal. 1994, 87, 297.
[6] Kulshreshtha, S. K.; Gadgil, M. M. Appl. Catal. B: Environmental 1997, 11, 291.
[7] Venezia, A. M.; Liotta, L. F.; Deganello, G.; Schay, Z.;Horváth, D.; Guczi, L. Appl. Catal. A: General 2001, 211,167.
[8] Pavlova, S. N.; Sadykov, V. A.; Bulgakov, N. N.;Bredikhin, M. N. J. Catal. 1996, 161, 517.
[9] Thormahlen, P.; Skoglundh, M.; Fridell, E.; Andersson, B.J. Catal. 1999, 188, 300.
[10] Wu, H.-C.; Liu, L.-C.; Yang, S.-M. Appl. Catal. A: General 2001, 211, 159.
[11] Grunwaldt, J. D.; Kiener, C.; Wögerbauer, C.; Baiker, A.J. Catal. 1999, 181, 223.
[12] Hao, Z.; An, L.; Wang, H.; Hu, T. React. Kinet. Catal.Lett. 2000, 70(1), 153.
[13] Wang, G.; Zhang, W.; Lian, H.; Liu, Q.; Jiang, D.; Wu,T. React. Kinet. Catal. Lett. 2002, 75(2), 343.
[14] Guzman, J.; Gates, B. C. J. Phys. Chem. B 2002, 106,7659.
[15] Zanella, R.; Giorgio, S.; Henry, C. R.; Louis, C. J. Phys.Chem. B 2002, 106, 7634.
[16] Bourane, A.; Bianchi, D. J. Catal. 2002, 209, 114.
[17] Ertl, G. J. Mol. Catal. A: Chem. 2002, 182-183, 5.
[18] Engel, T.; Ertl, G. J. Chem. Phys. 1978, 69(3), 1267.
[19] Pavlova, S. N.; Sadykov, V. A.; Razdobariv, V. A.; Paukshtis, E. A. J. Catal. 1996, 161,507.
[20] Close, J. S.; White, J. M. J. Catal. 1975, 36, 185.
[21] Conrad, H.; Ertl, G.; Kuppers, J. Surf. Sci. 1978, 76,323.
[22] Rainer, D. R.; Koranne, M.; Vesecky, S. M.; Goodman, D.W. J. Phys. Chem. B 1997, 101(50), 10769.
[23] Luo, M.-F.; Zheng, X.-M. Appl. Catal. A: General 1999,189, 15.
[24] Jaeger, N. I.; Moller, K.; Plath, P. J. J. Chem. Soc.,Faraday Trans. 1 1986, 82, 3315.
[25] Femández-Garcia, M.; Martinez-Arias, A.; Salamanca, L. N.;Coronado, J. M.; Anderson, J. A.; Conesa, J. C.; Soria, J.J. Catal. 1999, 187(2), 474.
[26] Bi, Y.-S.; Lü, G-X. Appl. Catal. B: Enviromental 2003, 41,279.
[27] Goursot, A.; Coq, B.; Fajula, F. J. Catal. 2003, 216,324.
[28] Dyakonov, A. J. Appl. Catal. B: Enviromental 2003, 45,241.
[29] Wolf, M. M.; Zhu, H.; Green, W. H.; Jackson, G. S. Appl.Catal. A: General 2003, 244, 323.
[30] Aylor, A. W.; Lobree, L. J.; Reimer, J. A.; Bell, A. T. J.Catal. 1997, 172, 453.
[31] Petró, J.; Schay, Z.; László, K.; Kiss, J. React. Kinet.Catal. Lett. 2002, 76(2), 383.
[32] Kim, K. S.; Gossmann, A. F.; Winograd, N. Anal. Chem.1974, 46(2), 197.
[33] Jing, L.-Q.; Cai, W.-M.; Sun, X.-J.; Hou, H.-G.; Xu,Z.-L.; Du, Y.-Q. Chin. J. Catal. 2002, 23(4), 336 (in Chinese).(井立强,蔡伟民,孙晓君,侯海鸽,徐自力,杜尧国,催化学报,2002,23(4),336.)
[34] Usami, Y.; Kagawa, K.; Kawazoe, M.; Matsumura, Y.; Sakurai, H.; Haruta, M. Appl. Catal. A: General 1998, 171,123.
[35] Jing, L.-Q.; Xu, Z.-L.; Sun, X.-J.; Shang, J.; Cai, W.-M.Appl. Surf. Sci. 2001, 180, 308.
[36] Moulder, J. F.; Stickle, W. F.; Soble, P. E.; Bomben, K.D. Handbook of X-Ray Photoelectron Spectrocopy, Physical Electronics Inc., U.S.A., 1995.
[37] Crabb, E.; Marshall, R. Appl. Catal. A: General 2001, 217,41.
[38] Wen, B.; Jia, J.; Wlofgang, M. H.; Sachtler, M. H. J.Phys. Chem. B 2002, 106, 7520.
[39] Watanale, M.; Uchida, H.; Ohkubom, K.; Igarashi, H. Appl.Catal. B: Enviromental 2003, 46, 595.
[40] Tripathi, A. K.; Kamble, V. S.; Gupta, N. M. J. Catal.1999, 187(2), 332.
[41] Gupta, N. M.; Tripathi, A. K. J. Catal. 1999, 187(2), 343.
[42] Panov, G. I.; Uriarte, A. K.; Rodkin, M. A.; Sobolev, V. I.Catal. Taday 1998, 41, 365.
[43] Aparicio, L. M.; Dumesic, J. A. J. Mol. Catal. 1989, 49,205.
[44] Kurkina, E. S.; Tolstunova, E. D. Appl. Surf. Sci. 2001,182, 77.

过渡金属对分子筛担载Pd催化剂上CO氧化性能影响

Influences of Transition Metal Additives on CO Oxidation over NaZSM-5 Supported Pd

PDF

可视化

被引次数

摘要/Abstract

引用此文

分享此文

参考文献

相关文章 15

编辑推荐

相关统计

本文评价

[1]	黄家翩, 刘飞, 吴劼. 二氟环丙烯参与的有机反应研究进展^★[J]. 化学学报, 2023, 81(5): 520-532.
[2]	韩明亮, 徐丽华. 过渡金属催化的硫酯的交叉偶联反应研究进展[J]. 化学学报, 2023, 81(4): 381-392.
[3]	马雪璐, 李蒙, 雷鸣. 三核过渡金属配合物在催化反应中的研究进展[J]. 化学学报, 2023, 81(1): 84-99.
[4]	贾亚辉, 李春生, 徐忠震, 刘伟, 高道伟, 陈国柱. 载体相变下Pt-TiO₂ SMSI研究及其对CO催化性能的影响[J]. 化学学报, 2022, 80(9): 1289-1298.
[5]	刘霞, 匡春香, 苏长会. 过渡金属催化的1,2,3-三氮唑导向的C—H键官能团化反应研究进展[J]. 化学学报, 2022, 80(8): 1135-1151.
[6]	熊昆, 陈伽瑶, 杨娜, 蒋尚坤, 李莉, 魏子栋. 理论探究水溶液条件对TMN_xC_y催化氮还原性能的增强机制[J]. 化学学报, 2021, 79(9): 1138-1145.
[7]	麻旺坪, 贺彦彦, 刘洪来. 烯烃连接的三嗪共轭多孔聚合物的合成及其可见光催化产氢性能[J]. 化学学报, 2021, 79(7): 914-919.
[8]	张洪浩, 俞寿云. 过渡金属与光氧化还原协同催化的烯丙基取代反应的研究进展[J]. 化学学报, 2019, 77(9): 832-840.
[9]	杨启亮, 王向阳, 翁信军, 杨祥, 徐学涛, 童晓峰, 方萍, 伍新燕, 梅天胜. 电氧化促进的钯催化的芳烃C(sp ²)—H键氯代反应[J]. 化学学报, 2019, 77(9): 866-873.
[10]	路福东, 姜烜, 陆良秋, 肖文精. 炔丙基自由基在有机合成化学中的应用[J]. 化学学报, 2019, 77(9): 803-813.
[11]	王强, 顾庆, 游书力. 过渡金属催化不对称C—H键官能团化反应构建轴手性联芳基化合物研究进展[J]. 化学学报, 2019, 77(8): 690-704.
[12]	余俊, 杨宇森, 卫敏. 水滑石基负载型催化剂的制备及其在催化反应中的应用[J]. 化学学报, 2019, 77(11): 1129-1139.
[13]	吴庆远, 秦瑞轩, 臧丹丹, 张无用, 吴炳辉, 郑南峰. 表面具丰富羟基的介孔TiO₂稳定Pt-OH-Fe(III)催化界面[J]. 化学学报, 2018, 76(8): 617-621.
[14]	李翠, 张琪, 傅尧. 过渡金属催化的醇类脱氧脱水反应[J]. 化学学报, 2018, 76(7): 501-514.
[15]	楚婉怡, 唐笑, 李振, 林景诚, 钱觉时. 液相合成超薄TiO₂纳米片微结构影响因素研究[J]. 化学学报, 2018, 76(7): 549-555.