具有多通道载流子分离功能的ZnO/P25异质结构光催化氧化甲苯

引用本文: 孔洁静, 赖晓冬, 芮泽宝, 纪红兵, 季生福. 具有多通道载流子分离功能的ZnO/P25异质结构光催化氧化甲苯[J]. 催化学报, 2016, 37(6): 869-877. doi: 10.1016/S1872-2067(15)61093-2 shu

Citation: Jiejing Kong, Xiaodong Lai, Zebao Rui, Hongbing Ji, Shengfu Ji. Multichannel charge separation promoted ZnO/P25 heterojunctions for the photocatalytic oxidation of toluene[J]. Chinese Journal of Catalysis, 2016, 37(6): 869-877. doi: 10.1016/S1872-2067(15)61093-2 shu

具有多通道载流子分离功能的ZnO/P25异质结构光催化氧化甲苯

a 中山大学化学与化学工程学院, 广东广州 510275;
b 中山大学化学工程与技术学院, 广东广州 510275;
c 中山大学惠州研究院废气净化与控制研发中心, 广东惠州 516081;
d 北京化工大学化工资源有效利用国家重点实验室, 北京 100029
基金项目:
化工资源有效利用国家重点实验室开放基金(CRE-2015-C-301).

广东省科技计划(2013B090500029)

广东省自然科学基金(2014A030313135, 2014A030308012)

国家自然科学基金(21576298, 21425627)

摘要: 甲苯是一种最常见的室内有毒挥发性有机物 (VOCs), 目前消除方法主要有吸附、催化燃烧和光催化氧化, 其中光催化是一种最高效和经济可行的方法, 能在较温和条件下将甲苯完全矿化为 CO₂. 作为研究最广泛的光催化剂, TiO₂在应用中通常有锐钛矿 (ATiO₂) 和金红石 (RTiO₂) 两种物相, 但单物相 TiO₂的低量子产率和光生电子-空穴对的快速复合严重限制了它的应用. 本文选择兼具锐钛矿和金红石两种物相的 P25 为催化剂载体, 通过负载少量 ZnO 和构建多组分并具备多通道载流子分离功能的异质结以提高 TiO₂ 基光催化剂的性能.
利用一步浸渍法制备了一系列 ZnO/P25 复合光催化剂, 考察了其光催化降解气相甲苯性能. X 射线粉末衍射结果表明, ZnO/P25 异质光催化剂是由 ATiO₂, RTiO₂和红锌矿三种物相结构组成. 高分辨透射电镜结果表明, ZnO/P25 具备三相异质结 ZnO(002)/ATiO₂(101)/RTiO₂(110). 紫外可见光谱、荧光光谱和光电流表征结果表明, ZnO/P25 所形成的三相异质结不但增强了光吸收能力, 还实现了多通道电子/空穴分离. 催化降解实验表明, ZnO/P25 异质光催化剂能在室温紫外光辐射下将甲苯完全矿化为 CO₂和 H₂O. 基于三相异质结和多通道光生电子-空穴对分离的形成及促进作用, ZnO/P25 光催化活性和速率均明显高于 P25. 本文报道的多通道载流子分离理念可为高效光催化剂设计和应用提供一种新思路.

关键词:

English

Multichannel charge separation promoted ZnO/P25 heterojunctions for the photocatalytic oxidation of toluene

a School of Chemistry and Chemical Engineering, Sun Yat-sen University, Guangzhou 510275, Guangdong, China;
b School of Chemical Engineering and Technology, Sun Yat-sen University, Guangzhou 510275, Guangdong, China;
c R&D Center of Waste-Gas Cleaning and Control, Huizhou Research Institute of Sun Yat-sen University, Huizhou 516081, Guangdong, China;
d State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Received Date: 22 January 2016
Revised Date: 29 March 2016
Fund Project:

This work was supported by the National Natural Science Foundation of China (21576298, 21425627), the Science and Technology Plan Project of Guangdong Province (2013B090500029), and Natural Science Foundation of Guangdong Province (2014A030313135, 2014A030308012), and the State Key Laboratory of Chemical Resource Engineering (CRE-2015-C-301), China.

Abstract: The fabrication of multicomponent heterojunctions is an effective strategy to improve the performance of TiO₂ based photocatalysts. We provide a new strategy for improving the charge separation and photocatalytic performance of ZnO/TiO₂ composites by the formation of multichannel charge separated heterojunctions. ZnO/P25 composites were prepared by an incipient wetness impregnation method, and applied for the photocatalytic destruction of gaseous toluene. The ZnO/P25 composites consist of anatase TiO₂ (ATiO₂), rutile TiO₂(RTiO₂) and hexagonal zincite structures. The parasitic phase of ZnO in P25 leads to the formation of ZnO(002)/ATiO₂(101)/RTiO₂(110) heterojunctions that exhibit enhanced light absorption and improved multichannel electron/hole separation. ZnO/P25 heterojunctions can completely oxidize toluene into CO₂ and H₂O under ultraviolet light irradiation at room temperature, and show enhanced photocatalytic activity in comparison with P25 owing to the efficient electron-hole separation. Such a multichannel charge separated design strategy may provide new insight into the design of highly effective photocatalysts and their potential technological applications.

Key words:

1. [1] D. A. Sarigiannis, S. P. Karakitsios, A. Gotti, I. L. Liakos, A. Katsoyiannis, Environ. Int., 2011, 37, 743-765.
2. [2] W. Z. Wang, H. L. Wang, T. L. Zhu, X. Fan, J. Hazard. Mater., 2015, 292, 70-78.
3. [3] Z. B. Rui, L. Y. Chen, H. Y. Chen, H. B. Ji, Ind. Eng. Chem. Res., 2014, 53, 15879-15888.
4. [4] Z. B. Rui, C. Y. Chen, Y. B. Lu, H. B. Ji, Chin. J. Chem. Eng., 2014, 22, 882-887.
5. [5] C. Y. Chen, F. Chen, L. Zhang, S. X. Pan, C. Q. Bian, X. M. Zheng, X. Q. Meng, F. S. Xiao, Chem. Commun., 2015, 51, 5936-5938.
6. [6] H. Einaga, S. Futamura, T. Ibusuki, Appl. Catal. B, 2002, 38, 215-225.
7. [7] M. J. Wang, F. Zhang, X. D. Zhu, Z. M. Qi, B. Hong, J. J. Ding, J. Bao, S. Sun, C. Gao, Langmuir, 2015, 31, 1730-1736.
8. [8] A. L. Linsebigler, G. Q. Lu, J. T. Yates, Chem. Rev., 1995, 95, 735-758.
9. [9] J. Zhang, Q. Xu, Z. C. Feng, M. J. Li, C. Li, Angew. Chem. Int. Ed., 2008, 47, 1766-1769.
10. [10] D. C. Hurum, A. G. Agrios, K. A. Gray, T. Rajh, M. C. Thurnauer, J. Phys. Chem. B, 2003, 107, 4545-4549.
11. [11] H. X. Li, Z. F. Bian, J. Zhu, Y. N. Huo, H. Li, Y. F. Lu, J. Am. Chem. Soc., 2007, 129, 4538-4539.
12. [12] W. J. Dai, J. Q. Yan, K. Dai, L. D. Li, N. J. Guan, Chin. J. Catal., 2015, 36, 1968-1975.
13. [13] C. L. Yu, W. Q. Zhou, J. C. Yu, H. Liu, L. F. Wei, Chin. J. Catal., 2014, 35, 1609-1618.
14. [14] R. Marschall, Adv. Funct. Mater., 2014, 24, 2421-2440.
15. [15] Y. H. Zhang, Z. R. Tang, X. Z. Fu, Y. J. Xu, ACS Nano, 2010, 4, 7303-7314.
16. [16] N. Qin, Y. H. Liu, W. M. Wu, L. J. Shen, X. Chen, Z. H. Li, L. Wu, Langmuir, 2015, 31, 1203-1209.
17. [17] N. Siedl, S. O. Baumann, M. J. Elser, O. Diwald, J. Phys. Chem. C, 2012, 116, 22967-22973.
18. [18] C. L. Yu, L. F. Wei, J. C. Chen, Y. Xie, W. Q. Zhou, Q. Z. Fan, Ind. Eng. Chem. Res., 2014, 53, 5759-5766.
19. [19] Y. Wang, Y. Z. Zheng, S. Q. Lu, X. Tao, Y. K. Che, J. F. Chen. ACS Appl. Mater. Interfaces, 2015, 7, 6093-6101.
20. [20] J. Wang, X. L. Liu, A. L. Yang, G. L. Zheng, S. Y. Yang, H. Y. Wei, Q. S. Zhu, Z. G. Wang, Appl. Phys. A, 2010, 103, 1099-1103.
21. [21] D. W. Kim, S. Lee, H. S. Jung, J. Y. Kim, H. Shin, K. S. Hong, Int. J. Hydrogen Energy, 2007, 32, 3137-3140.
22. [22] Y. Z. Lei, G. H. Zhao, M. C. Liu, Z. N. Zhang, X. L. Tong, T. C. Cao, J. Phys. Chem. C, 2009, 113, 19067-19076.
23. [23] D. Chen, H. Zhang, S. Hu, J. H. Li, J. Phys. Chem. C, 2008, 112, 117-122.
24. [24] F. X. Xiao, ACS Appl. Mater. Interfaces, 2012, 4, 7055-7063.
25. [25] L. Wu, J. Xing, Y. Hou, F. Y. Xiao, Z. Li, H. G. Yang, Chem.-Eur. J., 2013, 19, 8393-8396.
26. [26] T. Kawahara, Y. Konishi, H. Tada, N. Tohge, J. Nishii, S. Ito, Angew. Chem. Int. Ed., 2002, 41, 2811-2813.
27. [27] D. A. H. Hanaor, C. C. Sorrell, J. Mater. Sci., 2011, 46, 855-874.
28. [28] Z. B. Rui, Y. F. Huang, Y. Zheng, H. B. Ji, X. Yu, J. Mol. Catal. A, 2013, 372, 128-136.
29. [29] B. Ohtani, O. O. Prieto-Mahaney, D. Li, R. Abe, J. Photochem. Photobiol. A, 2010, 216, 179-182.
30. [30] J. M. Gallardo Amores, V. Sanchez Escribano, G. Buscab, J. Mater. Chem. 1995, 5, 1245-1249.
31. [31] F. Qin, H. P. Zhao, G. F. Li, H. Yang, J. Li, R. M. Wang, Y. L. Liu, J. C. Hu, H. Z. Sun, R. Chen, Nanoscale, 2014, 6, 5402-5409.
32. [32] H. F. Cheng, B. B. Huang, Y. Dai, X. Y. Qin, X. Y. Zhang, Langmuir, 2010, 26, 6618-6624.
33. [33] Z. F. Jiang, D. L. Jiang, Z. X. Yan, D. Liu, K. Qian, J. M. Xie, Appl. Catal. B, 2015, 170-171, 195-205.
34. [34] C. W. Kwon, A. Poquet, S. Mornet, G. Campet, M. H. Delville, M. Treguer, J. Portier, Mater. Lett., 2001, 51, 402-413.
35. [35] W. Y. Teoh, J. A. Scott, R. Amal, J. Phys. Chem. Lett., 2012, 3, 629-639.
36. [36] T. Tachikawa, M. Fujitsuka, T. Majima, J. Phys. Chem. C, 2007, 111, 5259-5275.
37. [37] L. Miao, P. Jin, K. Kaneko, A. Terai, N. Nabatova-Gabain, S. Tanemura, Appl. Surf. Sci., 2003, 212-213, 255-263.

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 835
HTML全文浏览量: 219

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

具有多通道载流子分离功能的ZnO/P25异质结构光催化氧化甲苯

English

Multichannel charge separation promoted ZnO/P25 heterojunctions for the photocatalytic oxidation of toluene

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

具有多通道载流子分离功能的ZnO/P25异质结构光催化氧化甲苯

English

Multichannel charge separation promoted ZnO/P25 heterojunctions for the photocatalytic oxidation of toluene

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

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs