Fe掺杂TiO2和Fe2O3量子点共负载催化剂:吸附与光催化协同作用高效降解有机染料

doi:10.1016/S1872-2067(17)62976-0

催化学报 ›› 2018, Vol. 39 ›› Issue (5): 920-928.DOI: 10.1016/S1872-2067(17)62976-0

Fe掺杂TiO₂和Fe₂O₃量子点共负载催化剂:吸附与光催化协同作用高效降解有机染料

沈国强^a,b, 潘伦^a,b, 吕哲^a,b, 王重庆^a,b, Fazal-e-Aleem^c, 张香文^a,b, 邹吉军^a,b

a 天津大学化工学院, 绿色合成与转化教育部重点实验室, 天津 300072, 中国;
b 天津化学化工协同创新中心, 天津 300072, 中国;
c 拉哈尔大学物理系, 巴基斯坦

收稿日期:2017-12-20 修回日期:2018-01-19 出版日期:2018-05-18 发布日期:2018-04-19
通讯作者: 张香文, 邹吉军
基金资助:
国家自然科学基金（21506156，51661145026，21676193）；天津市自然科学基金（15JCZDJC37300，16JCQNJC05200）；巴基斯坦自然科学基金（PSF/257NSFC-Eng/P-UoL（02））.

Fe-TiO₂ and Fe₂O₃ quantum dots co-loaded on MCM-41 for removing aqueous rose bengal by combined adsorption/photocatalysis

Guoqiang Shen^a,b, Lun Pan^a,b, Zhe Lü^a,b, Chongqing Wang^a,b, Fazal-e-Aleem^c, Xiangwen Zhang^a,b, Ji-Jun Zou^a,b

a Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Tianjin Unviersity, Tianjin 300072, China;
b Collaborative Innovation Center of Chemical Science and Engineering(Tianjin), Tianjin 300072, China;
c Department of Physics, The University of Lahore, Lahore 54600, Pakistan

Received:2017-12-20 Revised:2018-01-19 Online:2018-05-18 Published:2018-04-19
Contact: 10.1016/S1872-2067(17)62976-0
Supported by:
This work was supported by the National Natural Science Foundation of China (21506156, 51661145026, 21676193), the Tianjin Municipal Natural Science Foundation (15JCZDJC37300, 16JCQNJC05200), and the Pakistan Science Foundation (PSF/257NSFC-Eng/P-UoL (02)).

摘要/Abstract

摘要：

光催化作为节能、清洁的环境处理技术，被广泛应用于污染物处理领域，如室内气体净化、尾气VOCs处理和水体有机污染降解等.在众多光催化剂中，TiO₂以其良好的化学稳定性、无二次污染、无刺激性和安全无毒等优势得到广泛研究.然而TiO₂是宽禁带材料，仅能吸收太阳光谱的紫外光部分，通常需要用紫外光源来激发，光生电子-空穴易复合，这限制了其应用.过渡金属离子掺杂能在TiO₂价带之上形成新的掺杂能级，从而提高其光谱响应范围，提高全光谱反应活性；与体相TiO₂相比，纳米尺寸的TiO₂具有更高的光催化活性，尤其小于10nm的量子点尺寸TiO₂有着高活性面积、较短的光生电子-空穴迁移路径和独特的量子尺寸效应；Fe₂O₃作为吸附材料与TiO₂构建复合材料能够发挥吸附与光催化协同作用，从而提高污染物处理效率.
我们以构建Fe掺杂TiO₂和Fe₂O₃量子点共负载催化剂为目标，以钛酸四丁酯（TBT）和硫酸亚铁为前驱体，采用常温水解方法将Fe掺杂的TiO₂量子点生长在MCM-41分子筛表面，并通过调节硫酸亚铁加入量合成了MCM-41负载的Fe掺杂TiO₂和Fe₂O₃量子点催化剂.采用透射电子显微镜和X射线衍射研究了复合晶体结构，采用X射线光电子能谱、紫外-可见光谱和傅里叶变换红外光谱等表征手段研究了复合量子点材料生长机理和能带结构.结合吸附过程和光降解过程建立了吸附与光催化协同作用与污染物处理效率之间的关联关系.
表征结果表明，硫酸亚铁水溶液加速TBT水解成功地在MCM-41表面生长了Fe掺杂TiO₂量子点，并且量子点粒径随Fe前驱体量的增加而变大；前驱体比例Ti/Fe ≤ 3.0时，过量的硫酸亚铁会析出并在焙烧过程中在MCM-41上分解为Fe₂O₃量子点，Fe₂O₃量随着硫酸亚铁加入量提高而增多.通过调节Fe前驱体的量，一方面Fe掺杂在二氧化钛价带之上形成了掺杂能级，减小了带隙，拓宽了光响应范围，另一方面引入适量Fe₂O₃量子点，实现了Fe掺杂TiO₂和Fe₂O₃量子点共负载催化剂的构建.复合材料实现了吸附过程与光催化降解过程的协同作用，Fe₂O₃将污染物富集于催化剂表面，Fe掺杂TiO₂将其有效降解，大大提高了污染物处理能力，其中FT/M-3.0处理效率最高，并在10次循环处理后依然维持较高的吸附能力和光催化降解能力.该工作为高效光催化水处理催化剂的设计和构建提供了新思路和策略.

关键词: 量子点, 二氧化钛, 氧化铁, 光催化, 吸附

Abstract:

Adsorption and photodegradation are promising approaches for removing organic pollutions. In this study, we combined these two processes by co-loading Fe-TiO₂ and Fe₂O₃ quantum dots (QDs) on porous MCM-41, using a simple hydrolysis method. X-ray diffraction, high-resolution transmission electron microscopy, and X-ray photoelectron spectroscopy results indicated that Fe-TiO₂ QDs are formed at low Fe precursor concentrations, while additional Fe₂O₃ QDs are formed at higher Fe precursor concentrations. The Fe₂O₃ and Fe-TiO₂ QDs impart high adsorption capacity and high photoactivity to the porous MCM-41, respectively. Thus, their combination results in a synergic effect of the adsorption and photodegradation. The highest-performing sample exhibits excellent performance in removing rose bengal from aqueous solution.

Key words: Quantum dot, Titania, Ferric oxide, Photocatalysis, Adsorption

沈国强, 潘伦, 吕哲, 王重庆, Fazal-e-Aleem, 张香文, 邹吉军. Fe掺杂TiO₂和Fe₂O₃量子点共负载催化剂:吸附与光催化协同作用高效降解有机染料[J]. 催化学报, 2018, 39(5): 920-928.

Guoqiang Shen, Lun Pan, Zhe Lü, Chongqing Wang, Fazal-e-Aleem, Xiangwen Zhang, Ji-Jun Zou. Fe-TiO₂ and Fe₂O₃ quantum dots co-loaded on MCM-41 for removing aqueous rose bengal by combined adsorption/photocatalysis[J]. Chinese Journal of Catalysis, 2018, 39(5): 920-928.

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参考文献

[1] J. T. Liu, X. Ge, X. X. Ye, G. Z. Wang, H. M. Zhang, H. Zhou, Y. X. Zhang, H. Zhao, J. Mater. Chem. A, 2016, 4, 1970-1979.
[2] Z. F. Huang, J. J. Song, L. Pan, F. L. Lv, Q. Wang, J. J. Zou, X. W. Zhang, L. Wang, Chem. Commun., 2014, 50, 10959-10962.
[3] L. Pan, G. Q. Shen, J. W. Zhang, X. C. Wei, L. Wang, J. J. Zou, X. W. Zhang, Ind. Eng. Chem. Res., 2015, 54, 7226-7232.
[4] C. S. Cheng, J. Deng, B. Lei, A. He, X. Zhang, L. Ma, S. Li, C. S. Zhao, J. Hazard. Mater., 2013, 263, 467-478.
[5] B. Wang, H. B. Wu, L. Yu, R. Xu, T. T. Lim, X. W. Lou, Adv. Mater., 2012, 24, 1111-1116.
[6] J. Li, Q. H. Fan, Y. J. Wu, X. X. Wang, C. L. Chen, Z. Y. Tang, X. K. Wang, J. Mater. Chem. A, 2016, 4, 1737-1746.
[7] S. B. Wang, X. W. Zhang, L. Pan, F. M. Zhao, J. J. Zou, T. R. Zhang, L. Wang, Appl. Catal. B, 2015, 164, 234-240.
[8] L. Pan, S. B. Wang, W. B. Mi, J. J. Song, J. J. Zou, L. Wang, X. W. Zhang, Nano Energy, 2014, 9, 71-79.
[9] X. Jia, M. Tahir, L. Pan, Z. F. Huang, X. W. Zhang, L. Wang, J. J. Zou, Appl. Catal. B, 2016, 198, 154-161.
[10] L. Pan, S. B. Wang, J. Xie, L. Wang, X. Zhang, J. J. Zou, Nano Energy, 2016, 28, 296-303.
[11] L. Pan, J. Zhang, X. Jia, Y. H. Ma, X. W. Zhang, L. Wang, J. J. Zou, Chinese J. Catal., 2017, 38, 253-259.
[12] L. Pan, S. B. Wang, J. J. Zou, Z. F. Huang, L. Wang, X. W. Zhang, Chem. Commun., 2014, 50, 988-990.
[13] R. Daghrir, P. Drogui, D. Robert, Ind. Eng. Chem. Res., 2013, 52, 3581-3599.
[14] B. Liu, H. M. Chen, C. Liu, S. C. Andrews, C. Hahn, P. D. Yang, J. Am. Chem. Soc., 2013, 135, 9995-9998.
[15] S. George, S. Pokhrel, Z. X. Ji, B. L. Henderson, T. Xia, L. J. Li, J. I. Zink, A. E. Nel, L. Madler, J. Am. Chem. Soc., 2011, 133, 11270-11278.
[16] W. L. Wang, Z. F. Wang, J. J. Liu, Z. G. Zhang, L. Y. Sun, Sci. Rep., 2017, 7, 43755.
[17] P. S. Niphadkar, S. K. Chitale, S. K. Sonar, S. S. Deshpande, P. N. Joshi, S. V. Awate, J. Mater. Sci., 2014, 49, 6383-6391.
[18] V. Etacheri, G. Michlits, M. K. Seery, S. J. Hinder, S. C. Pillai, ACS Appl. Mater. Interfaces, 2013, 5, 1663-1672.
[19] J. G. Yu, J. X. Low, W. Xiao, P. Zhou, M. Jaroniec, J. Am. Chem. Soc., 2014, 136, 8839-8842.
[20] H. J. Jouybari, S. Saedodin, A. Zamzamian, M. E. Nimvari, S. Wongwises, Renew. Energy, 2017, 114, 1407-1418.
[21] A. Fabre, S. Salameh, L. C. Ciacchi, M. T. Kreutzer, J. R. van Om-men, J. Nanopart. Res., 2016, 18, 200.
[22] H. Y. Zhu, R. Jiang, L. Xiao, W. Li, J. Hazard. Mater., 2010, 179, 251-257.
[23] J. Y. Liu, L. M. Wong, G. Gurudayal, L. H. Wong, S. Y. Chiam, S. F. Yau Li, Y. Ren, J. Mater. Chem. A, 2016, 4, 13280-13288.
[24] L. Lu, J. Li, J. Yu, P. Song, D. H. L. Ng, Chem. Eng. J., 2016, 283, 524-534.
[25] T. Wen, J. Wang, S. J. Yu, Z. S. Chen, T. Hayat, X. K. Wang, ACS Sus-tain. Chem. Eng., 2017, 5, 4371-4380.
[26] J. F. Berry, E. Bill, E. Bothe, S. DeBeer. George, B. Mienert, F. Neese, K. Wieghardt, Science, 2006, 312, 1937-1941.
[27] C. T. Yavuz, J. T. Mayo, W. W. Yu, A. Prakash, J. C. Falkner, S. Yean, L. L. Cong, H. J. Shipley, A. Kan, M. Tomson, D. Natelson, V. L. Colvin, Science, 2006, 314, 964-967.
[28] J. Engel, S. R. Bishop, L. Vayssieres, H. L. Tuller, Adv. Funct. Mater., 2014, 24, 4952-4958.
[29] M. S. Nahar, K. Hasegawa, S. Kagaya, Chemosphere, 2006, 65, 1976-1982.
[30] W. Choi, A. Termin, M. R. Hoffmann, J. Phys. Chem., 1994, 98, 13669-13679.
[31] L. Pan, G. Q. Shen, J. W. Zhang, X. C. Wei, L. Wang, J. J. Zou, X. W. Zhang, Ind. Eng. Chem. Res., 2015, 54, 7226-7232.
[32] Z. Zhang, M. F. Hossain, T. Takahashi, Appl. Catal. B, 2010, 95, 423-429.
[33] G. Salvinelli, G. Drera, C. Baratto, A. Braga, L. Sangaletti, ACS Appl. Mater. Interfaces, 2015, 7, 765-773.
[34] T. G. Kim, H. Choi, S. Jeong, J. W. Kim, J. Phys. Chem. C, 2014, 118, 27884-27889.
[35] A. K. Dutta, S. K. Maji, B. Adhikary, Mater. Res. Bull., 2014, 49, 28-34.
[36] M. A. Salam, R. M. El-Shishtawy, A. Y. Obaid, J. Ind. Eng. Chem., 2014, 20, 3559-3567.
[37] J. J. Shen, R. Steinbach, J. M. Tobin, M. Mouro Nakata, M. Bower, M. R. S. McCoustra, H. Bridle, V. Arrighi, F. Vilela, Appl. Catal. B, 2016, 193, 226-233.
[38] R. J. Li, L. F. Liu, F. L. Yang, J. Hazard. Mater., 2014, 280, 20-30.
[39] J. Z. Zhang, J. Phys. Chem. B, 2000, 104, 7239-7253.
[40] C. J Sartoretti, B. D. Alexander, R. Solarska, I. A. Rutkowska, J. Augustynski, R. Cerny, J. Phys. Chem. B, 2005, 109, 13685-13692.
[41] M. Zhang, Y. J. Lin, T. J. Mullen, W. F. Lin, L. D. Sun, C. H. Yan, T. E. Patten, D. Wang, G. Y. Liu, J. Phys. Chem. Lett., 2012, 3, 3188-3192.
[42] C. H. Miao, T. F. Shi, G. P. Xu, S. L. Ji, C. H. Ye, ACS Appl. Mater. Interfaces, 2013, 5, 1310-1316.
[43] D. K. Zhong, J. W. Sun, H. Inumaru, D. R. Gamelin, J. Am. Chem. Soc., 2009, 131, 6086-6087.
[44] A. T. Nguyen, R. S. Juang, J. Environ. Manage., 2015, 147, 271-277.
[45] T. P. Yoon, M. A. Ischay, J. Du, Nat. Chem., 2010, 2, 527-532.
[46] S. Ghosh, N. A. Kouame, L. Ramos, S. Remita, A. Dazzi, A. Den-iset-Besseau, P. Beaunier, F. Goubard, P. H. Aubert, H. Remita, Nat. Mater., 2015, 14, 505-511.
[47] A. Zada, Y. Qu, S. Ali, N. Sun, H. W. Lu, R. Yan, X. L. Zhang, L. Q. Jing, J. Hazard. Mater., 2018, 342, 715-723.

Fe掺杂TiO₂和Fe₂O₃量子点共负载催化剂:吸附与光催化协同作用高效降解有机染料

Fe-TiO₂ and Fe₂O₃ quantum dots co-loaded on MCM-41 for removing aqueous rose bengal by combined adsorption/photocatalysis

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