N 掺杂TiO2 纳米粒子表面光生电荷特性与光催化活性

doi:10.3866/PKU.WHXB20101007

物理化学学报 >> 2010, Vol. 26 >> Issue (10): 2733-2738.doi: 10.3866/PKU.WHXB20101007

N 掺杂TiO₂ 纳米粒子表面光生电荷特性与光催化活性

张晓茹, 林艳红, 张健夫, 何冬青, 王德军

吉林大学化学学院, 长春130012

收稿日期:2010-05-21 修回日期:2010-07-16 发布日期:2010-09-27
通讯作者: 林艳红 E-mail:linyh@jlu.edu.cn
基金资助:
国家重点基础研究发展规划项目(973) (2007CB613303),国家自然科学基金(20703020, 20873053)和吉林大学科学前沿与交叉学科创新项目(421031401412)资助

Photoinduced Charge Carrier Properties and Photocatalytic Activity of N-Doped TiO₂ Nanocatalysts

ZHANG Xiao-Ru, LIN Yan-Hong, ZHANG Jian-Fu, HE Dong-Qing, WANG De-Jun

College of Chemistry, Jilin University, Changchun 130012, P. R. China

Received:2010-05-21 Revised:2010-07-16 Published:2010-09-27
Contact: LIN Yan-Hong E-mail:linyh@jlu.edu.cn
Supported by:
The project was supported by the National Key Basic Research Programof China (973) (2007CB613303), National Natural Science Foundation of China (20703020, 20873053), and Scientific Forefront and Interdisciplinary Innovation Project, Jilin University, China (421031401412).

摘要/Abstract

摘要：

以尿素为氮源, 采用水热法制备了不同N 掺杂量的TiO₂ (N-TiO₂)光催化剂. 利用X 射线衍射(XRD), 紫外-可见漫反射光谱(UV-Vis DRS),X 射线光电子能谱(XPS) 及荧光(PL) 光谱等技术对其进行了系统的表征. 以罗丹明B (RhB) 和甲基橙(MO) 溶液的脱色降解为模型反应, 分别考察了N-TiO₂ 光催化剂在紫外和可见光区的光催化活性. 利用表面光伏(SPV) 和瞬态光伏(TPV) 技术研究了N-TiO₂ 纳米粒子表面光生电荷的产生和传输机制, 并探讨了光生电荷与光催化活性之间的关系. 结果显示, 随着N 含量的增大, TiO₂ 表面光伏响应阈值红移, 可见光部分光电压响应强度逐渐增强, 瞬态光伏响应达到最大值的时间亦有着不同程度的延迟. 这表明适量的N 掺杂能够提高TiO₂ 纳米粒子中光生载流子的分离效率, 相应地延长载流子的传输时间, 增加光生电荷的寿命, 从而促进其光催化活性; 而过量的N 掺杂则增加了TiO₂ 纳米粒子中光生载流子的复合中心, 抑制其光催化活性.

关键词: N 掺杂TiO₂, 表面光伏, 瞬态光伏, 光生电荷, 光催化活性

Abstract:

Nitrogen-doped TiO₂ (N-TiO₂) photocatalysts with different amounts of N doping were successfully synthesized by the hydrothermal method using urea as the nitrogen source. The samples were characterized by X-ray diffraction (XRD), UV-Vis diffuse reflectance spectroscopy (UV -Vis DRS),X -ray photoelectron spectroscopy (XPS), and photoluminescence (PL) spectroscopy. The photodegradation of rhodamineB (RhB) and methyl orange (MO) solutions was used to evaluate the photocatalytic activity of the catalysts under UV and visible light irradiation. Surface photovoltage (SPV) and transient photovoltage (TPV) techniques were used to investigate the separation and transport mechanism of the photogenerated charge carriers of the N-doped TiO₂ nanoparticles. The relationship between the photogenerated charge carriers and photocatalytic activity was also discussed. The results showed that the SPV threshold values shifted to the visible region and a stronger photovoltaic response in the visible region was observed with an increase in N doping. We also found that the maximum TPV response time was different for N-TiO₂. These results indicate that with an appropriate amount of N doping, the photoinduced charge carriers separate efficiently, the transmission time increases, and the lifetime of the photoinduced charge carriers increases. Therefore, the photocatalytic activity is enhanced. However, excessive N acts as recombination centers for photoinduced electrons and holes, which reduces their photocatalytic activity.

Key words: N-doped TiO₂, Surface photovoltage, Transient photovoltage, Photo-induced charge carrier, Photocatalytic activity

MSC2000:

O643

张晓茹, 林艳红, 张健夫, 何冬青, 王德军. N 掺杂TiO₂ 纳米粒子表面光生电荷特性与光催化活性[J]. 物理化学学报, 2010, 26(10): 2733-2738.

ZHANG Xiao-Ru, LIN Yan-Hong, ZHANG Jian-Fu, HE Dong-Qing, WANG De-Jun. Photoinduced Charge Carrier Properties and Photocatalytic Activity of N-Doped TiO₂ Nanocatalysts[J]. Acta Phys. -Chim. Sin., 2010, 26(10): 2733-2738.

参考文献

1. Mor, G. K.; Shankar, K.; Paulose, M.; Varghese, O. K.; Grimes, C. A. Nano Lett., 2006, 6: 215
2. Konstantinau, I. K.; Albanis, T. A. Appl. Catal. B, 2003, 42: 319
3. Sakthivel, S.; Kisch, H. Angew. Chem. Int. Edit., 2003, 42: 4908
4. Hua, N. P.;Wu, Z. Y.; Du, Y. K.; Zou, Z. G.; Yang, P. Acta Phys. - Chim. Sin., 2005, 21: 1081 [华南平, 吴尊义,杜玉扣, 邹志刚, 杨平. 物理化学学报, 2005, 21: 1081]
5. Asahi, R.; Morikawa, T.; Ohwaki, T.; Aoki, K.; Taga, Y. Science, 2001, 293: 269
6. Lin, Z. S.; Orlov, A.; Lambert, R. M.; Payne, M. J. Phys. Chem. B, 2005, 109: 20948
7. Kuroda, Y.; Mori, T.; Yagi, K.; Makihata, N.; Kawahara, Y.; Nagao, M.; Kittaka, S. Langmuir, 2005, 21: 8026
8. Kisch, H.; Sakthivel, S.; Janczarek, M.; Mitoraj, D. J. Phys. Chem. C, 2007, 111: 11445
9. Yang, K. S.; Dai, Y.; Huang, B. B. J. Phys. Chem. C, 2007, 111: 12086
10. Tian, F. H.; Liu, C. B. J. Phys. Chem. B, 2006, 110: 17866
11. Zhou, Y. K.; Holme, T.; Berry, J.; Ohno, T. R.; Ginley, D.; Hayre, R. O. J. Phys. Chem. C, 2010, 114: 506
12. Li, J. Y.; Lu, N.; Quan, X.; Chen, S.; Zhao, H. M. Ind. Eng. Chem. Res., 2008, 47: 3804
13. Linsebigler, A. L.; Lu, G. Q.; Yates, J. T. Chem. Rev., 1995, 95: 735
14. Monllor-Satoca, D.; Gómez, R. J. Phys. Chem. C, 2008, 112: 139
15. Gross, D.; Mora-Seró, I.; Dittrich, T.; Belaidi, A.; Mauser, C.; Houtepen, A. J.; Como, E. D.; Rogach, A. L.; Feldmann, J. J. Am. Chem. Soc., 2010, 132: 5981
16. Duzhko, V.; Timoshenko, V. Y.; Koch, F.; Dittrich, T. Phys. Rev. B, 2001, 64: 075204
17. Alexander, D. Q.; Li, L. S. J. Phys. Chem. B, 2004, 108: 12842
18. Huang, D. G.; Liao, S. J.; Zhou,W. B.; Quan, S. Q.; Liu, L.; He, Z. J.;Wan, J. B. J. Phys. Chem. Sol., 2009, 70: 853
19. Sathishi, M.; Viswanathan, B.; Viswanath, R. P.; Gopinath, C. S. Chem. Mater., 2005, 17: 6349
20. Li, H.; Li, J.; Huo, Y. J. Phys. Chem. B, 2006, 110: 1559
21. Burda, C.; Lou, Y.; Chen, X.; Samia, A. C. S.; Stout, J.; Gole, J. M. Nano Lett., 2003, 3: 1049
22. Valentin, C. D.; Pacchioni, G.; Selloni, A.; Livraghi, S.; Giamello, E. J. Phys. Chem. B, 2005, 109: 11414
23. Kronik, L.; Shapira, Y. Surf. Sci. Rep., 1999, 371: 206
24. Liu, E. K.; Zhu, B. S.; Luo, J. S. Semiconductor physics. Beijing: Electronics Industry Press, 2003: 98-100 [刘恩科,朱秉升, 罗晋生.半导体物理学.北京: 电子工业出版社, 2003: 98-100]
25. Wei, X.; Xie, T. F.; Xu, D.; Zhao, Q. D.; Pang, S.; Wang, D. J. Nanotechnology, 2008, 19: 275707

[1]	陈锐杰,李娣,方振远,黄元勇,罗必富,施伟东. In₂O₃三维纳米结构的控制合成及高效光解水产氢活性研究[J]. 物理化学学报, 2020, 36(3): 1903047 - .
[2]	赵菲,时林其,崔佳宝,林艳红. Au纳米粒子负载的ZnO空心球复合材料的光生电荷转移行为及光催化活性[J]. 物理化学学报, 2016, 32(8): 2069 -2076 .
[3]	齐齐,王育乔,王莎莎,祁昊楠,卫涛,孙岳明. 还原氧化石墨烯/TiO₂纳米复合物制备及其光催化性能[J]. 物理化学学报, 2015, 31(12): 2332 -2340 .
[4]	余长林,魏龙福,李家德,何洪波,方稳,周晚琴. GO/Ag₃PO₄复合光催化剂的制备、表征及光催化性能[J]. 物理化学学报, 2015, 31(10): 1932 -1938 .
[5]	姚利珍,孔德生,杜玖瑶,王泽,张经纬,王娜,李文娟,冯媛媛. 表面钒修饰对α-Fe₂O₃材料光电化学性能的增强作用[J]. 物理化学学报, 2015, 31(10): 1895 -1904 .
[6]	林彩芳, 陈小平, 陈澍, 上官文峰. 水热法制备NiS/Cd_1-xZn_xS及其高效光催化产氢性能[J]. 物理化学学报, 2015, 31(1): 153 -158 .
[7]	赵伟荣, 施巧梦, 刘莹. SnO₂/TiO₂纳米管复合光催化剂的性能及失活再生[J]. 物理化学学报, 2014, 30(7): 1318 -1324 .
[8]	傅平丰, 张彭义. 低温静电自组装法制备贵金属修饰TiO₂纳米结构薄膜及其增强的光催化性能[J]. 物理化学学报, 2014, 30(5): 965 -972 .
[9]	王景声, 王恩君, 于彦龙, 郭丽梅, 曹亚安. 三维有序结构In 掺杂TiO₂薄膜的可见光催化活性[J]. 物理化学学报, 2014, 30(3): 513 -519 .
[10]	林雪, 郭晓宇, 王庆伟, 常利民, 翟宏菊. Bi₂MoO₆/BiVO₄异质结的水热合成和可见光催化活性[J]. 物理化学学报, 2014, 30(11): 2113 -2120 .
[11]	崔海琴, 井立强, 谢明政, 李志君. 金红石相TiO₂纳米棒的氢化处理及其光催化活性[J]. 物理化学学报, 2014, 30(10): 1903 -1908 .
[12]	张宇, 林申, 张钰, 宋溪明. ZnO/BiVO₄-V₂O₅异质结构光生电荷性质及可见光下表面光电流行为[J]. 物理化学学报, 2013, 29(11): 2399 -2404 .
[13]	郭丽梅, 匡元江, 杨晓丹, 于彦龙, 姚江宏, 曹亚安. 偏硼酸锶/碳酸锶复合催化剂光催化还原CO₂生成CH₄的研究[J]. 物理化学学报, 2013, 29(07): 1558 -1565 .
[14]	郭丽梅, 匡元江, 杨晓丹, 于彦龙, 姚江宏, 曹亚安. 偏硼酸锶催化剂光催化还原CO₂合成CH₄[J]. 物理化学学报, 2013, 29(02): 397 -402 .
[15]	陈金毅, 李念, 李晶, 朱亮, 彭昌军. 交联累托石/Cu₂O纳米复合材料的制备及可见光催化性能[J]. 物理化学学报, 2011, 27(04): 932 -938 .

N 掺杂TiO₂ 纳米粒子表面光生电荷特性与光催化活性

Photoinduced Charge Carrier Properties and Photocatalytic Activity of N-Doped TiO₂ Nanocatalysts

PDF

赞

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

Metrics

推荐阅读 0