A peculiar mechanism for the photocatalytic reduction of decabromodiphenyl ether over reduced graphene oxide-TiO2 photocatalyst

作者: Ming Lei , Nan Wang , Lihua Zhu , Changsheng Xie , Heqing Tang

DOI: 10.1016/J.CEJ.2013.12.032

关键词: PhotocatalysisGrapheneDecabromodiphenyl etherMethanolOxideDegradation (geology)Tio2 photocatalystChemistryPhotochemistryIrradiation

摘要: Abstract There remains a significant need for new approaches to photocatalytically destroy refractory halogenated pollutants. Here, efficient photocatalysts (RGO/TiO2) were prepared by UV treatment of graphene oxide (GO) mixed with Degussa P25 TiO2, and used reduce decabromodiphenyl ether (BDE209). The optimized composite yielded BDE209 degradation 72.0% debromination 59.4% in anoxic water methanol as electron donors after 12 h irradiation, being 2 4 times that over naked respectively. reduction generated 3Br–9Br PBDEs congeners, which further debrominated. This led 90% at 24 h reaction. Unlike the stepwise manner commonly observed UV–TiO2, generation, accumulation distribution intermediates time course implied skipped some steps. A novel mechanism multi-electron induced pathway was proposed. originated from abilities reduced GO storing transporting electrons. RGO not only trapped electrons improve charge separation on but also shuttled accumulated initiate transfer BDE209. markedly enhanced demonstrates RGO/TiO2 provide green method remove

参考文章(47)
Yuan Yao, Gonghu Li, Shannon Ciston, Richard M. Lueptow, Kimberly A. Gray, Photoreactive TiO2/Carbon Nanotube Composites: Synthesis and Reactivity Environmental Science & Technology. ,vol. 42, pp. 4952- 4957 ,(2008) , 10.1021/ES800191N
Quanjun Xiang, Jiaguo Yu, Mietek Jaroniec, Graphene-based semiconductor photocatalysts Chemical Society Reviews. ,vol. 41, pp. 782- 796 ,(2012) , 10.1039/C1CS15172J
Nan Wang, Yaozhuo Xu, Lihua Zhu, Xiantao Shen, Heqing Tang, Reconsideration to the deactivation of TiO2 catalyst during simultaneous photocatalytic reduction of Cr(VI) and oxidation of salicylic acid Journal of Photochemistry and Photobiology A-chemistry. ,vol. 201, pp. 121- 127 ,(2009) , 10.1016/J.JPHOTOCHEM.2008.10.002
Hee K Chae, Diana Y Siberio-Pérez, Jaheon Kim, YongBok Go, Mohamed Eddaoudi, Adam J Matzger, Michael O'keeffe, Omar M Yaghi, Materials Design and Discovery Group, None, A route to high surface area, porosity and inclusion of large molecules in crystals Nature. ,vol. 427, pp. 523- 527 ,(2004) , 10.1038/NATURE02311
Brendan Enright, Gareth Redmond, Donald Fitzmaurice, Spectroscopic determination of flatband potentials for polycrystalline TiO2 electrodes in mixed solvent systems The Journal of Physical Chemistry. ,vol. 98, pp. 6195- 6200 ,(1994) , 10.1021/J100075A023
Lisa Granelli, Johan Eriksson, Åke Bergman, Sodium borohydride reduction of individual polybrominated diphenyl ethers Chemosphere. ,vol. 86, pp. 1008- 1012 ,(2012) , 10.1016/J.CHEMOSPHERE.2011.11.037
Pascale M.L. Bonin, Patrick Edwards, Dorin Bejan, Chun Chi Lo, Nigel J. Bunce, Alexandre D. Konstantinov, Catalytic and electrocatalytic hydrogenolysis of brominated diphenyl ethers Chemosphere. ,vol. 58, pp. 961- 967 ,(2005) , 10.1016/J.CHEMOSPHERE.2004.09.099
Tsutomu Hirakawa, Prashant V. Kamat, Charge Separation and Catalytic Activity of Ag@TiO2 Core−Shell Composite Clusters under UV−Irradiation Journal of the American Chemical Society. ,vol. 127, pp. 3928- 3934 ,(2005) , 10.1021/JA042925A
Goki Eda, Manish Chhowalla, Chemically derived graphene oxide: towards large-area thin-film electronics and optoelectronics. Advanced Materials. ,vol. 22, pp. 2392- 2415 ,(2010) , 10.1002/ADMA.200903689
Juan Bezares-Cruz, Chad T. Jafvert, Inez Hua, Solar Photodecomposition of Decabromodiphenyl Ether:  Products and Quantum Yield Environmental Science & Technology. ,vol. 38, pp. 4149- 4156 ,(2004) , 10.1021/ES049608O