Zr/Ti摩尔比对锶锆钛复合氧化物在可见光下光催化性能的影响

引用本文: 黄海凤, 贾建明, 卢晗锋, 张宏华, 潘烈群. Zr/Ti摩尔比对锶锆钛复合氧化物在可见光下光催化性能的影响[J]. 物理化学学报, 2013, 29(06): 1319-1326. doi: 10.3866/PKU.WHXB201304012 shu

Citation: HUANG Hai-Feng, JIA Jian-Ming, LU Han-Feng, ZHANG Hong-Hua, PAN Lie-Qun. Effect of Designed Zr/Ti Molar Ratio on the Photocatalytic Activity of Sr-Zr-Ti Mixed Oxide Catalysts under Visible Light[J]. Acta Physico-Chimica Sinica, 2013, 29(06): 1319-1326. doi: 10.3866/PKU.WHXB201304012 shu

Zr/Ti摩尔比对锶锆钛复合氧化物在可见光下光催化性能的影响

基金项目:
国家自然科学基金(21107096)资助项目 (21107096)

摘要:

通过分步沉积法制备了不同Zr/Ti 摩尔比的锶锆钛(SZT)复合氧化物催化剂, 以X射线衍射(XRD)、扫描电镜(SEM)、透射电镜(TEM)、紫外-可见(UV-Vis)漫反射光谱等表征手段考察不同Zr/Ti 摩尔比下SZT催化剂的结构形态, 以可见光下光催化降解亚甲基蓝为模型反应考察样品的光催化活性. 结果表明: Zr/Ti 摩尔比<1 时SZT催化剂发生Zr⁴⁺与Ti⁴⁺同质替换, 引起晶格缺陷, 光催化活性小幅提高; Zr/Ti 摩尔比≥1 时SZT催化剂产生SrZrO₃/Ti_nO_2n-1 (n=4, 9)的新晶相, Ti_nO_2n-1 (n=4, 9)的存在有利于光生电子-空穴的传导与分离, 可大幅提高催化剂光催化活性. 其中, SZT-5/5 表现出最高的光催化活性, 其一级反应速率常数达到0.2133 min^-1, 是同等光照条件下纯SrTiO₃样品(0.0158 min^-1)的13.5倍.

关键词:

English

Effect of Designed Zr/Ti Molar Ratio on the Photocatalytic Activity of Sr-Zr-Ti Mixed Oxide Catalysts under Visible Light

1.
1 College of Biological and Environmental Engineering, Zhejiang University of Technology, Hangzhou 310014, P. R. China;
2 Research Institute of Catalytic Reaction Engineering, College of Chemical Engineering and Materials Science, Zhejiang University of Technology, Hangzhou 310014, P. R. China;
3 Environmental Monitoring Station of Fuyang City, Fuyang 311400, Zhejiang Province, P. R. China
Received Date: 20 November 2012
Available Online: 17 May 2013
Fund Project:
国家自然科学基金(21107096)资助项目

Abstract:

A series of Sr-Zr-Ti (SZT) mixed oxide catalysts were prepared by a fractional-precipitation method. These photocatalysts were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), and ultraviolet visible (UV-Vis) diffuse reflectance absorption spectra. Photocatalytic degradation of methylene blue was investigated to determine the photoactivity of the catalyst. It was shown that with a Zr/Ti ratio<1, the SZT mixed oxide catalysts showed improved photocatalytic activity. This was attributed to lattice defects creating active photocatalytic sites because of Zr⁴⁺ doping. For Zr/Ti ratios ≥1, the catalysts showed markedly improved photocatalytic activity because of new crystalline phases of SrZrO₃ and Ti_nO_2n-1 (n=4, 9)that facilitated splitting and conduction for electron/hole. Typical SZT samples (Zr/Ti=4) showed the highest photocatalytic activity, with first-order reaction rate constant 13.5 times that of a SrTiO₃ sample.

Key words:

1. [1]
  
  (1) Yan, X. R.; Li, X. H.; Huo, M. L.; Guo,W.W.; ng, Y. J. Acta Phys. -Chim. Sin. 2001, 17, 23. [颜秀如, 李晓红, 霍明亮, 郭伟巍, 巩永进. 物理化学学报, 2001, 17, 23.] doi: 10.3866/PKU.WHXB20010105
  (1) Yan, X. R.; Li, X. H.; Huo, M. L.; Guo,W.W.; ng, Y. J. Acta Phys. -Chim. Sin. 2001, 17, 23. [颜秀如, 李晓红, 霍明亮, 郭伟巍, 巩永进. 物理化学学报, 2001, 17, 23.] doi: 10.3866/PKU.WHXB20010105
2. [2]
  (2) Kurokawa, H.; Yang, L. M.; Jacobson, C. P.; Jacobson, C. P.; DeJonghe, L. C.; Visco, S. J. Power Sources 2007, 164 (2), 510.doi: 10.1016/j.jpowsour.2006.11.048(2) Kurokawa, H.; Yang, L. M.; Jacobson, C. P.; Jacobson, C. P.; DeJonghe, L. C.; Visco, S. J. Power Sources 2007, 164 (2), 510.doi: 10.1016/j.jpowsour.2006.11.048
3. [3]
  (3) Huang, H. F.; Tang,W.; Chen, Y. F.; Chen, B. F. J. Mol. Catal.2005, 19 (5), 351. [黄海凤, 唐伟, 陈银飞, 陈碧芬. 分子催化, 2005, 19 (5), 351.](3) Huang, H. F.; Tang,W.; Chen, Y. F.; Chen, B. F. J. Mol. Catal.2005, 19 (5), 351. [黄海凤, 唐伟, 陈银飞, 陈碧芬. 分子催化, 2005, 19 (5), 351.]
4. [4]
  (4) Lee, M. S.; Meyer, J. U. Sensors and Actuators B, Chemical2000, 68 (1-3), 293. doi: 10.1016/S0925-4005(00)00447-0(4) Lee, M. S.; Meyer, J. U. Sensors and Actuators B, Chemical2000, 68 (1-3), 293. doi: 10.1016/S0925-4005(00)00447-0
5. [5]
  (5) Luo,W. J.; Li, Z. S.; Jiang, X. J.; Yu, T.; Liu, L. F.; Chen, X. Y.;Ye, J. H.; Zou, Z. G. Phys. Chem. Chem. Phys. 2008, 10, 6717.doi: 10.1039/b803996h(5) Luo,W. J.; Li, Z. S.; Jiang, X. J.; Yu, T.; Liu, L. F.; Chen, X. Y.;Ye, J. H.; Zou, Z. G. Phys. Chem. Chem. Phys. 2008, 10, 6717.doi: 10.1039/b803996h
6. [6]
  (6) Puangpetch, T.; Sreethawong, T.; Chavadej, S. Int. J. Hydrog. Energy 2010, 35, 6532.(6) Puangpetch, T.; Sreethawong, T.; Chavadej, S. Int. J. Hydrog. Energy 2010, 35, 6532.
7. [7]
  (7) Wang, D.; Kako, T.; Ye, J. J. Phys. Chem. C 2009, 113, 3785.doi: 10.1021/jp807393a(7) Wang, D.; Kako, T.; Ye, J. J. Phys. Chem. C 2009, 113, 3785.doi: 10.1021/jp807393a
8. [8]
  (8) Chen, L.; Zhang, S. C.;Wang, L. Q.; Xue, D. F.; Yin, S. J. Crystal Growth 2009, 311, 746.(8) Chen, L.; Zhang, S. C.;Wang, L. Q.; Xue, D. F.; Yin, S. J. Crystal Growth 2009, 311, 746.
9. [9]
  (9) Ryoko, K.; Tatsuya, I.; Hideki, K.; Akihiko, K. J. Phys. Chem. B2004, 108, 8992. doi: 10.1021/jp049556p(9) Ryoko, K.; Tatsuya, I.; Hideki, K.; Akihiko, K. J. Phys. Chem. B2004, 108, 8992. doi: 10.1021/jp049556p
10. [10]
  (10) Onishi, T. J. Top Catal. 2010, 53, 566. doi: 10.1007/s11244-010-9488-6(10) Onishi, T. J. Top Catal. 2010, 53, 566. doi: 10.1007/s11244-010-9488-6
11. [11]
  (11) Galinetto, P.; Casiraghi, A.; Mozzati, M. C.; Azzoni, C. B.;Norton, D.; Boatner, L. A. Ferroelectrics 2008, 368 (1), 120.doi: 10.1080/00150190802368248(11) Galinetto, P.; Casiraghi, A.; Mozzati, M. C.; Azzoni, C. B.;Norton, D.; Boatner, L. A. Ferroelectrics 2008, 368 (1), 120.doi: 10.1080/00150190802368248
12. [12]
  (12) Hua, N. P.;Wu, Z. Y.; Du, Y. K.; Zou, Z. G.; Yang, P. Acta Phys. -Chim. Sin. 2005, 21 (10), 1085. [华南平, 吴遵义, 杜玉扣, 邹志刚, 杨平. 物理化学学报, 2005, 21 (10), 1085.] doi: 10.3866/PKU.WHXB20051004(12) Hua, N. P.;Wu, Z. Y.; Du, Y. K.; Zou, Z. G.; Yang, P. Acta Phys. -Chim. Sin. 2005, 21 (10), 1085. [华南平, 吴遵义, 杜玉扣, 邹志刚, 杨平. 物理化学学报, 2005, 21 (10), 1085.] doi: 10.3866/PKU.WHXB20051004
13. [13]
  (13) Lu, H. F.; Zhou, Y.; Xu, B. Q.; Chen, Y. F.; Liu, H. Z. Acta Phys. -Chim. Sin. 2008, 24 (3), 459. [卢晗锋, 周瑛, 徐柏庆, 陈银飞, 刘化章. 物理化学学报, 2008, 24 (3), 459.] doi: 10.3866/PKU.WHXB20080319(13) Lu, H. F.; Zhou, Y.; Xu, B. Q.; Chen, Y. F.; Liu, H. Z. Acta Phys. -Chim. Sin. 2008, 24 (3), 459. [卢晗锋, 周瑛, 徐柏庆, 陈银飞, 刘化章. 物理化学学报, 2008, 24 (3), 459.] doi: 10.3866/PKU.WHXB20080319
14. [14]
  (14) Puangpetch, T.; Sreethawong, T.; Chavadej, S. Int. J. Hydrog. Energy 2010, 35, 6531. doi: 10.1016/j.ijhydene.2010.04.015(14) Puangpetch, T.; Sreethawong, T.; Chavadej, S. Int. J. Hydrog. Energy 2010, 35, 6531. doi: 10.1016/j.ijhydene.2010.04.015
15. [15]
  (15) Wei,W.; Dai, Y.; Guo, M.; Zhu, Y. Z.; Huang, B. B. J. Phys. Chem. C 2010, 114, 10917.(15) Wei,W.; Dai, Y.; Guo, M.; Zhu, Y. Z.; Huang, B. B. J. Phys. Chem. C 2010, 114, 10917.
16. [16]
  (16) Yang, J.; Li, D.;Wang, X. J. Solid State Chem. 2002, 165 (1),193. doi: 10.1006/jssc.2001.9526(16) Yang, J.; Li, D.;Wang, X. J. Solid State Chem. 2002, 165 (1),193. doi: 10.1006/jssc.2001.9526
17. [17]
  (17) Tanaka, T.; Teramura Kentaro, Y. T. J. Photochem. Photobiol. A-Chem. 2002, 148 (1-3), 277. doi: 10.1016/S1010-6030(02)00054-0(17) Tanaka, T.; Teramura Kentaro, Y. T. J. Photochem. Photobiol. A-Chem. 2002, 148 (1-3), 277. doi: 10.1016/S1010-6030(02)00054-0
18. [18]
  (18) Kataoka, S.; Tompkins, D. T.; Zeltner,W. A. J. Photochem. Photobiol. A-Chem. 2002, 148 (1-3), 323. doi: 10.1016/S1010-6030(02)00059-X(18) Kataoka, S.; Tompkins, D. T.; Zeltner,W. A. J. Photochem. Photobiol. A-Chem. 2002, 148 (1-3), 323. doi: 10.1016/S1010-6030(02)00059-X
19. [19]
  (19) Pan, L. Q.; Lu, H. F.; Huang, H. F. Rare Earths 2011, 3 (29),284. [潘烈群, 卢晗锋, 黄海凤. 中国稀土学报, 2011, 3 (29),284.](19) Pan, L. Q.; Lu, H. F.; Huang, H. F. Rare Earths 2011, 3 (29),284. [潘烈群, 卢晗锋, 黄海凤. 中国稀土学报, 2011, 3 (29),284.]
20. [20]
  (20) Yu, C. L.; Fan, C. F.; Yu, J. M. Mater. Res. Bull. 2011, 46 (1),145.(20) Yu, C. L.; Fan, C. F.; Yu, J. M. Mater. Res. Bull. 2011, 46 (1),145.
21. [21]
  (21) Tennakone, K.; Ileperuma, O. A.; Bandara, J. M. S.; Kiridena,W. C. B. Semicond. Sci. Technol. 1992, 7 (3), 424. doi: 10.1088/0268-1242/7/3B/109(21) Tennakone, K.; Ileperuma, O. A.; Bandara, J. M. S.; Kiridena,W. C. B. Semicond. Sci. Technol. 1992, 7 (3), 424. doi: 10.1088/0268-1242/7/3B/109
22. [22]
  (22) Wei, G. P.; Jiang, C. H.; Zhen,W.; Jin, D. R. Crystal Structure and Defects, 1st ed.; Code of Practice for Design andConstruction: Beijing, 2010; pp 5, 64-120. [魏光普, 姜传海,甄伟, 金灯仁. 晶体结构与缺陷, 第一版. 北京: 中国水利水电出版社; 2010: 5, 64-120.](22) Wei, G. P.; Jiang, C. H.; Zhen,W.; Jin, D. R. Crystal Structure and Defects, 1st ed.; Code of Practice for Design andConstruction: Beijing, 2010; pp 5, 64-120. [魏光普, 姜传海,甄伟, 金灯仁. 晶体结构与缺陷, 第一版. 北京: 中国水利水电出版社; 2010: 5, 64-120.]
23. [23]
  (23) Chen, J. Z. Modern Crystal Chemistry, 1st ed.; Science andTechnology Press: Beijin g, 2010; pp 140-160. [陈敬中. 现代晶体化学, 第一版. 北京: 科学技术出版社, 2010: 140-60.](23) Chen, J. Z. Modern Crystal Chemistry, 1st ed.; Science andTechnology Press: Beijin g, 2010; pp 140-160. [陈敬中. 现代晶体化学, 第一版. 北京: 科学技术出版社, 2010: 140-60.]
24. [24]
  (24) Xu, Y. L. Basic of Oxide and Compound Semiconductor, 1st ed.;Xidian University Press: Xi'an, 1991. [徐毓龙. 氧化物与化合物半导体基础, 第一版. 西安: 西安电子科技大学出版社,1991.](24) Xu, Y. L. Basic of Oxide and Compound Semiconductor, 1st ed.;Xidian University Press: Xi'an, 1991. [徐毓龙. 氧化物与化合物半导体基础, 第一版. 西安: 西安电子科技大学出版社,1991.]
25. [25]
  (25) Han,W. Q.;Wang, X. L. Appl. Phys. Lett. 2010, 2 (12), 3709.(25) Han,W. Q.;Wang, X. L. Appl. Phys. Lett. 2010, 2 (12), 3709.
26. [26]
  (26) Walsh, F. C.;Wills, R. G. A. Electrochimica Acta 2010, 55,6342. doi: 10.1016/j.electacta.2010.05.011(26) Walsh, F. C.;Wills, R. G. A. Electrochimica Acta 2010, 55,6342. doi: 10.1016/j.electacta.2010.05.011
27. [27]
  (27) Chen, G. Y.; Simon, R. B.; Thomas, E. M. The Electrochemical Society 2002, 149 (8), A1092.(27) Chen, G. Y.; Simon, R. B.; Thomas, E. M. The Electrochemical Society 2002, 149 (8), A1092.
28. [28]
  (28) Lakkis, S.; Schlenkcr, C.; Chakravcrty, B. K.; Buder, R.;Marezio, M. Physical Review B 1976, 14 (4), 1429.(28) Lakkis, S.; Schlenkcr, C.; Chakravcrty, B. K.; Buder, R.;Marezio, M. Physical Review B 1976, 14 (4), 1429.
29. [29]
  (29) Masayuki,W.;Wakana, U.; Tetsusuke, H. Luminescence 2007,122-123, 393.(29) Masayuki,W.;Wakana, U.; Tetsusuke, H. Luminescence 2007,122-123, 393.
30. [30]
  (30) Leandro, L.; Giuseppe, M. Physical Review B 2009, 79, 245133.doi: 10.1103/PhysRevB.79.245133(30) Leandro, L.; Giuseppe, M. Physical Review B 2009, 79, 245133.doi: 10.1103/PhysRevB.79.245133
31. [31]
  (31) Eyert, V.; Schwingenschl, U.; Eckern, U. Chemical Physics Letters 2004, 390, 151. doi: 10.1016/j.cplett.2004.04.015(31) Eyert, V.; Schwingenschl, U.; Eckern, U. Chemical Physics Letters 2004, 390, 151. doi: 10.1016/j.cplett.2004.04.015
32. [32]
  (32) Xu, Y.; Schoonen, M. A. A. American Mineralogist 2000, 85,543.(32) Xu, Y.; Schoonen, M. A. A. American Mineralogist 2000, 85,543.
33. [33]
  (33) Liu, S.W.; Lu, M. K.; Song, C. F.;Wang, S. F.; Gu, F.; Cheng,X. F.; Xu, D.; Yuan, D. R. J. Functional Materials 2004, 35 (2),233. [刘素文, 吕孟凯, 宋春风, 王淑芬, 顾锋, 程秀风,许东, 袁多荣. 功能材料, 2004, 35 (2), 233.]
  (33) Liu, S.W.; Lu, M. K.; Song, C. F.;Wang, S. F.; Gu, F.; Cheng,X. F.; Xu, D.; Yuan, D. R. J. Functional Materials 2004, 35 (2),233. [刘素文, 吕孟凯, 宋春风, 王淑芬, 顾锋, 程秀风,许东, 袁多荣. 功能材料, 2004, 35 (2), 233.]

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沈阳化工大学材料科学与工程学院沈阳 110142

Zr/Ti摩尔比对锶锆钛复合氧化物在可见光下光催化性能的影响

English

Effect of Designed Zr/Ti Molar Ratio on the Photocatalytic Activity of Sr-Zr-Ti Mixed Oxide Catalysts under Visible Light

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Zr/Ti摩尔比对锶锆钛复合氧化物在可见光下光催化性能的影响

English

Effect of Designed Zr/Ti Molar Ratio on the Photocatalytic Activity of Sr-Zr-Ti Mixed Oxide Catalysts under Visible Light

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？

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