La0.8Sr0.2Fe1-xScxO3-δ催化剂的制备、表征及甲烷催化燃烧性能

引用本文: 雷泽, 孙义, 韩敏芳, 王启宝. La_0.8Sr_0.2Fe_1-xSc_xO_3-δ催化剂的制备、表征及甲烷催化燃烧性能[J]. 物理化学学报, doi: 10.3866/PKU.WHXB201206153 shu

Citation: LEI Ze, SUN Yi, HAN Min-Fang, WANG Qi-Bao. Preparation, Characterization and Catalytic Activities of La_0.8Sr_0.2Fe_1-xSc_xO_3-δ Catalysts for Methane Combustion[J]. Acta Physico-Chimica Sinica, doi: 10.3866/PKU.WHXB201206153 shu

La_0.8Sr_0.2Fe_1-xSc_xO_3-δ催化剂的制备、表征及甲烷催化燃烧性能

基金项目:
国家自然科学基金(20806088)资助项目 (20806088)

摘要:

采用甘氨酸-硝酸盐溶液燃烧法制备了钙钛矿型氧化物催化剂La_0.8Sr_0.2Fe_1-xSc_xO_3-δ (LSFS, x=0, 0.3,0.4, 0.5, 0.6, 0.8, 1), 利用X射线衍射(XRD)、H₂程序升温还原(H₂-TPR)、扫描电子显微镜(SEM)和比表面积测试等手段对催化剂进行了系统表征, 并在常压微型固定床反应器上考察了催化剂对甲烷燃烧的催化性能. 结果表明, 经空气气氛下900 °C煅烧5 h制备的LSFS均具有单一的钙钛矿结构, 在La_0.8Sr_0.2FeO_3-δ (LSF)中掺杂Sc有助于改善催化剂的抗烧结性能, 提高催化剂的比表面积. 当LSF 中的Sc 掺杂量为0.4-0.6 时, 所形成的LSFS表现出良好的甲烷催化燃烧活性, 其中Sc 掺杂量为0.5 时, 其起燃温度(T₁₀)和完全转化温度(T₉₀)分别为406和563 °C, 与La_0.8Sr_0.2FeO_3-δ和La_0.8Sr_0.2ScO_3-δ相比, T₁₀分别降低了14和87 °C; T₉₀分别降低了59和95 °C.

关键词:

甲烷
/ 催化燃烧
/ 钙钛矿
/ 钪
/ 锶掺杂铁酸镧

English

Preparation, Characterization and Catalytic Activities of La_0.8Sr_0.2Fe_1-xSc_xO_3-δ Catalysts for Methane Combustion

1.
Research Center of Fuel Cell on Coal Gasification, School of Chemical and Environmental Engineering, China University of Mining & Technology, Beijing 100083, P. R. China
Received Date: 26 March 2012
Available Online: 02 August 2012
Fund Project:
国家自然科学基金(20806088)资助项目

Abstract:

Perovskite-type La_0.8Sr_0.2Fe_1-xSc_xO_3-δ (LSFS, x=0, 0.3, 0.4, 0.5, 0.6, 0.8, 1) catalysts were prepared by glycine-nitrate solution combustion. The catalysts were characterized by X-ray powder diffraction (XRD), H₂-temperature-programmed reduction (H₂-TPR), scanning electron microscopy (SEM), and specific surface area measurements. The catalytic performance of LSFS for methane combustion was investigated in a micro fixed-bed reactor. The results showed that all the LSFS catalysts have a single perovskite structure after calcining in air at 900 °C for 5 h. By doping Sc into La_0.8Sr_0.2FeO_3-δ, the sintering agglomeration between the LSFS particles is weakened, and therefore the specific surface area is increased. At Sc dopings of 0.4-0.6, the resultant LSFS gives od catalytic activity for methane combustion, with a light-off temperature (T₁₀) of 406 °C and a total conversion temperature (T₉₀) of 563 °C at a Sc doping of 0.5. Compared with La_0.8Sr_0.2FeO_3-δ and La_0.8Sr_0.2ScO_3-δ the T₁₀ is decreased by 14 and 87 °C, and T₉₀ is decreased by 59 and 95 °C, respectively.

Key words:

1. [1]
  
  (1) Sun, M. Y.; Liu, Y. J. Sino-global Energy 2008, 13 (3), 20. [孙茂远, 刘贻军. 中外能源, 2008, 13 (3), 20.]
  (1) Sun, M. Y.; Liu, Y. J. Sino-global Energy 2008, 13 (3), 20. [孙茂远, 刘贻军. 中外能源, 2008, 13 (3), 20.]
2. [2]
  (2) Yu, F. J.; Zhu, L.; Zhou, B.; Shao, L. N.; He, X.W. Clean Coal Technology 2009, 3, 5. [於俊杰, 朱玲, 周波, 邵立南, 何绪文. 洁净煤技术, 2009, 3, 5.](2) Yu, F. J.; Zhu, L.; Zhou, B.; Shao, L. N.; He, X.W. Clean Coal Technology 2009, 3, 5. [於俊杰, 朱玲, 周波, 邵立南, 何绪文. 洁净煤技术, 2009, 3, 5.]
3. [3]
  (3) Arai, H.; Machida, M. Catal. Today 1991, 10, 81. doi: 10.1016/0920-5861(91)80076-L(3) Arai, H.; Machida, M. Catal. Today 1991, 10, 81. doi: 10.1016/0920-5861(91)80076-L
4. [4]
  (4) Zhang, H. M.; Teraoka, Y.; Yamazoe, N. Catal . Today 1989, 6,155. doi: 10.1016/0920-5861(89)85018-7(4) Zhang, H. M.; Teraoka, Y.; Yamazoe, N. Catal . Today 1989, 6,155. doi: 10.1016/0920-5861(89)85018-7
5. [5]
  (5) Liu, Y.; Yang, X. G.;Wu, Y. Chin. J. Catal. 2000, 21, 59.[刘钰, 杨向光, 吴越. 催化学报, 2000, 21, 59.](5) Liu, Y.; Yang, X. G.;Wu, Y. Chin. J. Catal. 2000, 21, 59.[刘钰, 杨向光, 吴越. 催化学报, 2000, 21, 59.]
6. [6]
  (6) Yang, Q. H.; Fu, X. X.;Wang, J. Z. Chin. J. Catal. 1999, 20,521. [杨秋华, 傅希贤, 王俊珍. 催化学报, 1999, 20, 521.](6) Yang, Q. H.; Fu, X. X.;Wang, J. Z. Chin. J. Catal. 1999, 20,521. [杨秋华, 傅希贤, 王俊珍. 催化学报, 1999, 20, 521.]
7. [7]
  (7) Wang, P.; Yao, L. G.;Wang, M. X. Chin. J. Catal. 2000, 21, 23.[王鹏, 姚立广, 王明贤. 催化学报, 2000, 21, 23.](7) Wang, P.; Yao, L. G.;Wang, M. X. Chin. J. Catal. 2000, 21, 23.[王鹏, 姚立广, 王明贤. 催化学报, 2000, 21, 23.]
8. [8]
  (8) Bray, K. L. Chem. Eng. Sci. 1994, 49, 3337.(8) Bray, K. L. Chem. Eng. Sci. 1994, 49, 3337.
9. [9]
  (9) Ciambelli, P.; Cimino, S.; De Rossi, S.; Lisi, L.; Minelli, G.;Porta, P.; Russo, G. Applied Catalysis B: Environmental 2001,29, 239. doi: 10.1016/S0926-3373(00)00215-0(9) Ciambelli, P.; Cimino, S.; De Rossi, S.; Lisi, L.; Minelli, G.;Porta, P.; Russo, G. Applied Catalysis B: Environmental 2001,29, 239. doi: 10.1016/S0926-3373(00)00215-0
10. [10]
  (10) Leanza, R.; Rossetti, I.; Fabbrini, L.; Oliva, C.; Forni, L.Applied Catalysis B: Environmental 2000, 28, 55. doi: 10.1016/S0926-3373(00)00163-6(10) Leanza, R.; Rossetti, I.; Fabbrini, L.; Oliva, C.; Forni, L.Applied Catalysis B: Environmental 2000, 28, 55. doi: 10.1016/S0926-3373(00)00163-6
11. [11]
  (11) Lu, Y.; Kuang, D. T.; Liu, L. X. Journal of Daqing Petroleum Institute 2003, 27, 29. [卢艳, 匡洞庭, 刘立新. 大庆石油学院学报, 2003, 27, 29.](11) Lu, Y.; Kuang, D. T.; Liu, L. X. Journal of Daqing Petroleum Institute 2003, 27, 29. [卢艳, 匡洞庭, 刘立新. 大庆石油学院学报, 2003, 27, 29.]
12. [12]
  (12) Martinez-Ortega, F.; Batiot, C.; Barrault, J.; Ganne, M.;Tatibouët, J. M. Stud. Surf. Sci. Catal. 1998, 119, 45. doi: 10.1016/S0167-2991(98)80406-0(12) Martinez-Ortega, F.; Batiot, C.; Barrault, J.; Ganne, M.;Tatibouët, J. M. Stud. Surf. Sci. Catal. 1998, 119, 45. doi: 10.1016/S0167-2991(98)80406-0
13. [13]
  (13) Batiot-Dupeyrat, C.; Martinez-Ortega, F.; Ganne, M.; Tatibouët,J. M. Applied Catalysis A: General 2001, 206, 205. doi: 10.1016/S0926-860X(00)00596-2(13) Batiot-Dupeyrat, C.; Martinez-Ortega, F.; Ganne, M.; Tatibouët,J. M. Applied Catalysis A: General 2001, 206, 205. doi: 10.1016/S0926-860X(00)00596-2
14. [14]
  (14) Martinez-Ortega, F.; Batiot-Dupeyrat, C.; Valderrama, G.;Tatibouët, J. M. C. R. Acad. Sci. Paris, Se ´ rie IIc 2001, 4, 49.(14) Martinez-Ortega, F.; Batiot-Dupeyrat, C.; Valderrama, G.;Tatibouët, J. M. C. R. Acad. Sci. Paris, Se ´ rie IIc 2001, 4, 49.
15. [15]
  (15) Zhong, Z. Y.; Chen, K. D.; Ji, Y.; Yan, Q. J. Applied Catalysis A: General 1997, 156, 29. doi: 10.1016/S0926-860X(97)00003-3(15) Zhong, Z. Y.; Chen, K. D.; Ji, Y.; Yan, Q. J. Applied Catalysis A: General 1997, 156, 29. doi: 10.1016/S0926-860X(97)00003-3
16. [16]
  (16) Spinicci, R.; Tofanari, A.; Delmastro, A.; Mazza, D.; Ronchetti,S. Mater. Chem. Phys. 2002, 76, 20. doi: 10.1016/S0254-0584(01)00498-9(16) Spinicci, R.; Tofanari, A.; Delmastro, A.; Mazza, D.; Ronchetti,S. Mater. Chem. Phys. 2002, 76, 20. doi: 10.1016/S0254-0584(01)00498-9
17. [17]
  (17) Wang, C. H.; Chen, C. L;Weng, H. S. Chemosphere 2004, 57,1131. doi: 10.1016/j.chemosphere.2004.08.031(17) Wang, C. H.; Chen, C. L;Weng, H. S. Chemosphere 2004, 57,1131. doi: 10.1016/j.chemosphere.2004.08.031
18. [18]
  (18) Pecchi, G.; Reyes, P.; Zamora, R.; Campos, C.; Caduus, L. E.;Barbero, B. P. Catal. Today 2008, 133-135, 420.(18) Pecchi, G.; Reyes, P.; Zamora, R.; Campos, C.; Caduus, L. E.;Barbero, B. P. Catal. Today 2008, 133-135, 420.
19. [19]
  (19) Alifanti, M.; Kirchnerova, J.; Delmon, B.; Klvana, D. Applied Catalysis A: General 2004, 262, 167. doi: 10.1016/j.apcata.2003.11.024(19) Alifanti, M.; Kirchnerova, J.; Delmon, B.; Klvana, D. Applied Catalysis A: General 2004, 262, 167. doi: 10.1016/j.apcata.2003.11.024
20. [20]
  (20) Tian, T. F.; Zhan, M. C.;Wang,W. D.; Chen, C. S. Catal. Commun. 2009, 10, 513. doi: 10.1016/j.catcom.2008.10.028(20) Tian, T. F.; Zhan, M. C.;Wang,W. D.; Chen, C. S. Catal. Commun. 2009, 10, 513. doi: 10.1016/j.catcom.2008.10.028
21. [21]
  (21) Boekema, C.; Jonker, P. C.; Filoti, G.; Vander,W. F. Hyperfine Interactions 1979, 7, 45. doi: 10.1007/BF01021491(21) Boekema, C.; Jonker, P. C.; Filoti, G.; Vander,W. F. Hyperfine Interactions 1979, 7, 45. doi: 10.1007/BF01021491
22. [22]
  (22) Shannon, R. D. Acta Cryst. A 1976, 32, 751.(22) Shannon, R. D. Acta Cryst. A 1976, 32, 751.
23. [23]
  (23) Wei, Z. X.; Xu, Y, Q.; Liu, H. Y.; Hu, C.W. Journal of Hazardous Materials 2009, 165, 1056. doi: 10.1016/j.jhazmat.2008.10.086(23) Wei, Z. X.; Xu, Y, Q.; Liu, H. Y.; Hu, C.W. Journal of Hazardous Materials 2009, 165, 1056. doi: 10.1016/j.jhazmat.2008.10.086
24. [24]
  (24) Li, R. J.; Yu, C. C.; Dai, X. P.; Sheng, S. K. Chin. J. Catal.2002, 23, 549. [李然家, 余长春, 代小平, 沈师孔. 催化学报,2002, 23, 549.](24) Li, R. J.; Yu, C. C.; Dai, X. P.; Sheng, S. K. Chin. J. Catal.2002, 23, 549. [李然家, 余长春, 代小平, 沈师孔. 催化学报,2002, 23, 549.]
25. [25]
  (25) Liang, Z. C.; Qin, Y. N.; Qiao, G. D.; Qi, X. Z.; Liao, Q. L.Chinese Journal of Chemical Physics 1997, 10, 60. [梁珍成,秦永宁, 乔冠东, 齐晓周, 廖巧丽. 化学物理学报, 1997, 10,60.](25) Liang, Z. C.; Qin, Y. N.; Qiao, G. D.; Qi, X. Z.; Liao, Q. L.Chinese Journal of Chemical Physics 1997, 10, 60. [梁珍成,秦永宁, 乔冠东, 齐晓周, 廖巧丽. 化学物理学报, 1997, 10,60.]
26. [26]
  (26) Falcon, H.; Barbero, J. A.; Alonso, J. A.; Mart'nez-Lope, M. J.;Fierro, J. L. G. Chem. Mater. 2002, 14, 2325. doi: 10.1021/cm011292l(26) Falcon, H.; Barbero, J. A.; Alonso, J. A.; Mart'nez-Lope, M. J.;Fierro, J. L. G. Chem. Mater. 2002, 14, 2325. doi: 10.1021/cm011292l
27. [27]
  (27) Arai, H.; Machida, M. Applied Catalysis A: General 1996, 138,161. doi: 10.1016/0926-860X(95)00294-4(27) Arai, H.; Machida, M. Applied Catalysis A: General 1996, 138,161. doi: 10.1016/0926-860X(95)00294-4
28. [28]
  (28) Wu, Y. Chin. Sci. Bull. 1992, 2, 97. [吴越. 科学通报, 1992,2, 97.](28) Wu, Y. Chin. Sci. Bull. 1992, 2, 97. [吴越. 科学通报, 1992,2, 97.]
29. [29]
  (29) Yu, T.;Wu, Y. Chin. J. Catal. 1989, 10, 262. [于涛, 吴越.催化学报, 1989, 10, 262.](29) Yu, T.;Wu, Y. Chin. J. Catal. 1989, 10, 262. [于涛, 吴越.催化学报, 1989, 10, 262.]
30. [30]
  (30) Zhang, R. M.; Hu, R. S.; Hu, J. N.; Zhang, Y. L. Acta Phys. -Chim. Sin. 2011, 27, 1169. [张慧敏, 胡瑞生, 胡佳楠,张玉龙. 物理化学学报, 2011, 27, 1169.] doi: 10.3866/PKU.WHXB20110502(30) Zhang, R. M.; Hu, R. S.; Hu, J. N.; Zhang, Y. L. Acta Phys. -Chim. Sin. 2011, 27, 1169. [张慧敏, 胡瑞生, 胡佳楠,张玉龙. 物理化学学报, 2011, 27, 1169.] doi: 10.3866/PKU.WHXB20110502
31. [31]
  (31) Pan, Z. Y.; Zhang, C. B.; Yu, C. S.; Shen, S. K. J. Mol. Catal.2003, 17, 274. [潘智勇, 张长斌, 余长春, 沈师孔. 分子催化,2003, 17, 274.](31) Pan, Z. Y.; Zhang, C. B.; Yu, C. S.; Shen, S. K. J. Mol. Catal.2003, 17, 274. [潘智勇, 张长斌, 余长春, 沈师孔. 分子催化,2003, 17, 274.]
32. [32]
  (32) Yang, J. H.;Wang, Y. P.; Guo, C. L. J. Mol. Catal. 2006, 20,530. [杨继海, 王一平, 郭翠梨. 分子催化, 2006, 20, 530.]
  (32) Yang, J. H.;Wang, Y. P.; Guo, C. L. J. Mol. Catal. 2006, 20,530. [杨继海, 王一平, 郭翠梨. 分子催化, 2006, 20, 530.]

扫一扫看文章

计量

PDF下载量: 628
文章访问数: 2571
HTML全文浏览量: 102

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

La_0.8Sr_0.2Fe_1-xSc_xO_3-δ催化剂的制备、表征及甲烷催化燃烧性能

English

Preparation, Characterization and Catalytic Activities of La_0.8Sr_0.2Fe_1-xSc_xO_3-δ Catalysts for Methane Combustion

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

La0.8Sr0.2Fe1-xScxO3-δ催化剂的制备、表征及甲烷催化燃烧性能

English

Preparation, Characterization and Catalytic Activities of La0.8Sr0.2Fe1-xScxO3-δ Catalysts for Methane Combustion

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

La_0.8Sr_0.2Fe_1-xSc_xO_3-δ催化剂的制备、表征及甲烷催化燃烧性能

Preparation, Characterization and Catalytic Activities of La_0.8Sr_0.2Fe_1-xSc_xO_3-δ Catalysts for Methane Combustion

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs