可见光辐射下富勒烯[60]-氧化铁复合催化剂的制备及光芬顿法降解有机污染物研究

doi:10.1016/S1872-2067(18)63067-0

催化学报 ›› 2018, Vol. 39 ›› Issue (6): 1051-1059.DOI: 10.1016/S1872-2067(18)63067-0

可见光辐射下富勒烯[60]-氧化铁复合催化剂的制备及光芬顿法降解有机污染物研究

邹丛阳^a,b, 孟则达^b, 纪文超^a, 刘守清^b, 申哲民^a, 张园^b, 蒋妮姗^b

a 上海交通大学环境科学与工程学院, 上海 200240;
b 苏州科技大学环境科学与工程学院石湖校区, 江苏苏州 215009

收稿日期:2018-01-08 修回日期:2018-03-21 出版日期:2018-06-18 发布日期:2018-05-16
通讯作者: 申哲民
基金资助:
国家自然科学基金（21347006，21576175，51478285，51403148）；苏州科技大学江苏省环境科学与工程重点实验室开放课题（zd131205）；水处理技术与材料协同创新中心，苏州分离净化材料和技术重点实验室（SZS201512）.

Preparation of a fullerene[60]-iron oxide complex for the photo-fenton degradation of organic contaminants under visible-light irradiation

Cong-yang Zou^a,b, Ze-da Meng^b, Wen-chao Ji^a, Shou-qing Liu^b, Zhemin Shen^a, Yuan Zhang^b, Ni-shan Jiang^b

a School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;
b School of Environmental Science and Engineering, Suzhou University of Science and Technology Shihu Campus, Suzhou 215009, Jiangsu, China

Received:2018-01-08 Revised:2018-03-21 Online:2018-06-18 Published:2018-05-16
Contact: 10.1016/S1872-2067(18)63067-0
Supported by:
The work was supported by the National Natural Science Foundation of China (21347006, 21576175, 51478285, 51403148), the Opening Project of Key Laboratory of Jiangsu Province environmental science and engineering of Suzhou University of Science and Technology (zd131205), Collaborative Innovation Center of Technology and Material of Water Treatment and Suzhou Key Lab of Separation and Purification Materials & Technologies (SZS201512).

摘要/Abstract

摘要：

采用简单的可升级的化学浸渍法，将Fe₂O₃掺杂到富勒烯[60]（C₆₀）上，制得C₆₀-Fe₂O₃纳米复合材料.采用了粉末X射线衍射、X射线光电子能谱（XPS）、扫描电镜、高分辨透射电镜、紫外-可见吸收光谱、拉曼光谱和傅里叶变换红外光谱，对其进行了表征.结果发现，XPS数据中，Fe2p_3/2和Fe2p_1/2的XPS特征峰分别位于结合能710.9和724.1eV处，对应Fe₂O₃的Fe³⁺.富勒烯颗粒均匀分散在Fe₂O₃纳米颗粒表面，Fe₂O₃纳米颗粒的平均尺寸大约为20-30nm；Fe₂O₃对于可见光只有微弱的吸收，而制备出的C₆₀-Fe₂O₃纳米复合材料对于可见光有较强的吸收响应.
本文将C₆₀-Fe₂O₃纳米复合光催化材料用于光催化降解50mL，20mg/lMB和50mL，10mg/L苯酚实验.结果发现，在双氧水存在下和可见光（>420nm）辐射条件下，C₆₀-Fe₂O₃对上述有机污染物均有较好的降解效果.通过测定上述有机物的削减程度，评估了C₆₀-Fe₂O₃催化剂的光催化活性，通过改变实验条件，得到可见光/C₆₀-Fe₂O₃/双氧水体系的最佳光催化降解条件：在pH值为3.06~10.34的范围内，投加0.02g催化剂，5mol/L双氧水.结果表明，在最佳条件下，亚甲基蓝在80 min内脱色率能达到98.9%，矿化率能达到71%.浸出实验的结果表明，C₆₀-Fe₂O₃复合光催化剂中的铁浸出量可以忽略不计.经过5次循环使用后，C₆₀-Fe₂O₃复合光催化剂仍具有较高的光催化活性.为了进一步验证C₆₀-Fe₂O₃复合光催化剂的应用广泛性，本文在可见光/C₆₀-Fe₂O₃/双氧水体系下，开展了降解RhB，MO和苯酚的试验，结果发现，该催化剂它们也具有高的降解效果.机理研究发现，C₆₀-Fe₂O₃复合光催化剂的高效催化能力可归因于C₆₀和Fe₂O₃的协同效应：在可见光辐射下，由于C₆₀具有独特的光敏性特征，能够接收电子并把它们转移到Fe₂O₃的Fe3d轨道，并通过一系列反应，达到Fe³⁺/Fe²⁺循环平衡.利用活性组分捕集实验，对光催化反应过程中的主要活性氧化剂进行了区分.结果表明，羟基自由基在整个过程中发挥了最主要的作用.

关键词: C₆₀-Fe₂O₃, 多相光催化, 光-芬顿, 可见光, 活性成份的捕获

Abstract:

Iron oxide (Fe₂O₃) was doped onto fullerene[60] (C₆₀) to form a C₆₀-Fe₂O₃ composite using an easy and scalable impregnation method. The as-prepared C₆₀-Fe₂O₃ samples were characterized by powder X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, high-resolution transmission electron microscopy, UV-vis absorption spectroscopy, Raman spectroscopy, and Fourier transform infrared spectroscopy. The photocatalytic activity of the C₆₀-Fe₂O₃ catalyst was evaluated by examining the degradation of methylene blue (MB), rhodamine B (RhB), methyl orange (MO), and phenol under visible light (λ > 420 nm) in the presence of hydrogen peroxide. The results showed that the catalyst exhibited excellent catalytic properties over a wide pH range 3.06-10.34. Under optimal conditions, 98.9% discoloration and 71% mineralization of MB were achieved in 80 min. Leaching test results indicated that the leaching of iron from the catalyst was negligible and that the catalyst had a high photocatalytic activity after five reaction cycles. The catalyst was also efficient in the degradation of RhB, MO, and phenol. These findings could be attributed to the synergetic effects of C₆₀ and Fe₂O₃. We used active species trapping experiments to determine the main active oxidant in the photocatalytic reaction process and found that hydroxyl radicals played a major role in the entire process.

Key words: C₆₀-Fe₂O₃, Heterogeneous photocatalysis, Photo-Fenton, Visible light, Active species trapping

邹丛阳, 孟则达, 纪文超, 刘守清, 申哲民, 张园, 蒋妮姗. 可见光辐射下富勒烯[60]-氧化铁复合催化剂的制备及光芬顿法降解有机污染物研究[J]. 催化学报, 2018, 39(6): 1051-1059.

Cong-yang Zou, Ze-da Meng, Wen-chao Ji, Shou-qing Liu, Zhemin Shen, Yuan Zhang, Ni-shan Jiang. Preparation of a fullerene[60]-iron oxide complex for the photo-fenton degradation of organic contaminants under visible-light irradiation[J]. Chinese Journal of Catalysis, 2018, 39(6): 1051-1059.

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参考文献

[1] R. P. Schwarzenbach, B. I. Escher, K. Fenner, T. B. Hofstetter, C. A. Johnson, U. von Gunten, B. Wehrli, Science, 2006, 313, 1072-1077.
[2] D. B. Lu, Y. Zhang, S. Lin, L. Wang, C. Wang, J. Alloys. Compd., 2013, 579, 336-342.
[3] A. A. Farghali, M. Bahgat, W. M. A El Rouby, M. H. Khedr, J. Alloys. Compd., 2013, 555, 193-200.
[4] Y. Chen, N. Li, Y. Zhang, L. Zhang, J. Colloid. Interfaces Sci., 2014, 422, 9-15.
[5] F. B. Li, X. Z. Li, X. M. Li, T. X. Liu, J. Dong, J. Colloid. Interfaces Sci., 2007, 311, 481-490.
[6] W. Jiang, W. S. Zhu, H. M. Li, Y. H. Chao,S. H. Xun, Y. H. Chang, H. Liu, Z. Zhao, J. Mol. Catal. A, 2014, 382, 8-14.
[7] N. M. Mahmoodi, Environ. Monit. Assess., 2014, 186, 5595-5604.
[8] C. Singh, S. Bansal, V. Kumar, S Singhal, Ceram. Intern., 2015, 41, 3595-3604.
[9] J. Ma, L. Z. Zhang, Y. H. Wang, S. L. Lei, X. B. Luo, S. H. Chen, G. S. Zeng, J. P. Zou, S. L. Luo, C. T. Au, Chem. Eng. J., 2014, 251, 371-380.
[10] S. B. Zhu, T. G. Xu, H. B. Fu, J. Zhao, Y. Zhu, Environ. Sci. Technol., 2007, 41, 6234-6239.
[11] G. Li, B. Jiang, X. Li, Z. C. Lian, S. N. Xiao, J. Zhu, D. Q. Zhang, H. X. Li, ACS App. Mater. Interfaces, 2013, 5, 7190-7197.
[12] P. Bouras, E. Stathatos, P. Lianos, App. Catal. B, 2007, 73, 51-59.
[13] L. W. Zhang, Y. J. Wang, T. G. Xu, S. B. Zhu, Y. F. Zhu, J. Mol. Catal. A, 2010, 331, 7-14.
[14] G. Yu, J. Gao, J. C. Hummelen, F. Wudl, A. J. Heeger, Science, 1995, 1789-1791.
[15] M. Wang, Z. W. Wang, L. Wei, J. W. Li, X. S. Zhao, Chin. J. Catal., 2017, 38, 1680-1687.
[16] X. Zhao, H. J. Liu, Y. L. Shen, J. H. Qu, App. Catal. B, 2011, 106, 63-68.
[17] Z. D. Meng, L. Zhu, J. G. Choi, C. Y. Park, W. C. Oh, Nanoscale Res. Lett., 2011, 6, 459.
[18] B. Chai, X. Liao, F. K. Song, H. Zhou, Dalton Trans., 2014, 43, 982-989.
[19] M. Barroso, A. J. Cowan, S. R. Pendlebury, M. Grätzel, D. R. Klug, J. R. Durrant, J. A. Chem. Soc., 2011, 133, 14868-14871.
[20] M. A. Gondal, A. Hameed, Z. H. Yamani, A. Suwaiyan, App. Catal. A, 2004, 268(1), 159-167.
[21] O. Akhavan, Appl. Surf. Sci., 2010, 257, 1724-1728.
[22] Y. X. Deng, H. X. Huangfu, S. H. Tang, J. Li, Chin. J. Catal., 2017, 38, 1668-1679.
[23] C. Chen, J. Hu, D. Shao, J. Li, X. Wang, J. Hazard. Mater., 2009, 164, 923-928.
[24] L. H. Ai, C. Y. Zhang, Z. L. Chen, J. Hazard. Mater., 2011, 192, 1515-1524.
[25] G. Q. Xie,J. Cheng, Y. F. Li, P. X. Xi, F. J. Chen, H. Y. Liu, F. P. Hou, Y. J. Shi, L. Huang, Z. H. Xu, D. C. Bai, Z. Z. Zeng J. Mater. Chem., 2012, 22, 1033-1039.
[26] S. P. West, T. Poon, J. L. Anderson, M, A, West, C. S. Foote, J. Chem. Educ., 1997, 74, 311-312.
[27] H. Veisi, R. Masti, D. Kordestani, M. Safaei, O. Sahin, J. Mol. Catal. A, 2014, 385, 61-67.
[28] U. Holzwarth, N. Gibson, Nat. Nanotechnol., 2011, 6, 534-534.
[29] D. Patil, V. Patil, P. Patil, Sens. Actuat. B, 2011, 152, 299-306.
[30] O. Akhavan, R. Azimirad, App. Catal. A, 2009, 369, 77-82.
[31] X. Song, Y. Yan, X. Q. Li, J. Zhang, P. P. Yao, S. Z. Kang, J. Mu, Chin. J. Inorg. Chem., 2011, 27, 1047-1052.
[32] H. Orita, N. Itoh, App. Catal. A, 2004, 258, 17-23.
[33] V. Chhabra, P. Ayyub, S. Chattopadhyay, A. N. Maitra, Mater. Lett., 1996, 26, 21-26.
[34] X. Y. Yang, X. Y. Zhang, Y. F. Ma, Y. Huang, Y. Wang, Y. Chen, J. Mater. Chem., 2009, 19, 2710-2714.
[35] Y. H. Zhang, Z. R. Tang, X. Z. Fu, Y. J. Xu, ACS Nano, 2010, 4, 7303-7314
[36] J. L. Zhang, G. L. Chen, Q. Zhang, F. Kang, Y. Bo, ACS Appl. Mater. Interfaces, 2015, 7, 12760-12766.
[37] R. Rahimi, S. Zargan, A. Ghaffarinejad, A. Morsali, Environ. Prog. Sustain. Energy, 2016, 35, 642-652.
[38] M. S. Hamdy, G. Mul, App. Catal. B, 2015, 174, 413-420.
[39] A. Asghar, A. R. Abdul Aziz, W. M. A. W. Daud, J. Cleaner Prod., 2015, 87, 826-838.
[40] L. Ren, Y. Z. Li, J. T. Hou, X. J. Zhao, X. C. Pan, ACS Appl. Mater. Interfaces, 2014, 6, 1608-1615.
[41] Y. Z. Li, W. Xie, X. L. Hu, G. F. Shen, X. Zhou, Y. Xiang, X. J. Zhao, P. F. Fang, Langmuir, 2010, 26, 591-597.

可见光辐射下富勒烯[60]-氧化铁复合催化剂的制备及光芬顿法降解有机污染物研究

Preparation of a fullerene[60]-iron oxide complex for the photo-fenton degradation of organic contaminants under visible-light irradiation

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