Abstract
We developed a graphene oxide-free synthetic route to hybridize TiO2/graphene at nanoscale with an excellent visible-light photocatalytic activity for the degradation of methylene blue; however, the mechanism behind this superior activity was a mystery. In this study, we performed radical scavenger tests, electron paramagnetic resonance measurements, and photoluminescence measurements in order to uncover the origin of the excellent activity of the TiO2/graphene nanocomposite. The TiO2/graphene nanocomposite exhibited an excellent ability in absorbing organic pollutants, a high efficiency of charge carrier separation, and a great ability to activate adsorbed oxygen molecules and subsequently trap superoxide radicals. We have found that the high ability to activate adsorbed oxygen molecules and trap superoxide radicals of the TiO2/graphene nanocomposite was the key factor contributing to its superior visible-light photocatalytic activity.
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S. González, R. López-Roldán, J.L. Cortina, Environ. Pollut. 161, 83 (2012)
O. Üner, Ü. Geçgel, Y. Bayrak, Water Air Soil Pollut. 227, 1 (2016)
M. Sarkar, A.K.M.L. Rahman, N.C. Bhoumik, Water Resour. Ind. 17, 1 (2017)
M.E. Khan, M.M. Khan, M.H. Cho, J. Colloid Interface Sci. 482, 221 (2016)
M.R. Sohrabi, M. Ghavami, J. Hazard. Mater. 153, 1235 (2008)
S. Sher, M. Waseem, M.K. Leta, Environments 10, 40 (2023)
Z. Abdeen, S.G. Mohammad, Open J. Org. Polym. Mater. 4, 16 (2014)
B. Chen, M. Yuan, H. Liu, J. Hazard. Mater. 188, 436 (2011)
S. Valili, G. Siavalas, H.K. Karapanagioti, I.D. Manariotis, K. Christanis, J. Environ. Manage. 128, 252 (2013)
G.K. Nagda, A.M. Diwan, V.S. Ghole, Appl. Ecol. Environ. Res. 5, 1 (2007)
E.S.M. Mouele, J.O. Tijani, O.O. Fatoba, L.F. Petrik, Environ. Sci. Pollut. Res. 22, 18345 (2015)
H. Lin, W. Gao, F. Meng, B.Q. Liao, K.T. Leung, L. Zhao et al., Crit. Rev. Environ. Sci. Technol. 42, 677 (2012)
T. Gullinkala, I.C. Escobar, ACS Symp. Ser. 1078, 155 (2011)
C.J. Hapeman-Somich, ACS Symp. Ser. 510, 157 (1992)
L.G. Devi, R. Kavitha, Appl. Catal. B Environ. 140, 559 (2013)
S.S.A. Amr, H.A. Aziz, M.N. Adlan, S.Q. Aziz, Clean: Soil, Air, Water 41, 148 (2013)
K. Kalyanasundaram, M. Grätzel, Coord. Chem. Rev. 177, 347 (1998)
S. Hamad, C.R.A. Catlow, S.M. Woodley, S. Lago, J.A. Mejías, J. Phys. Chem. B 109, 15741 (2005)
M. Adachi, Y. Murata, J. Takao, J. Jiu, M. Sakamoto, F. Wang, J. Am. Chem. Soc. 126, 14943 (2004)
O.K. Varghese, M. Paulose, T.J. LaTempa, C.A. Grimes, Nano Lett. 9, 731 (2009)
K. Zakrzewska, Thin Solid Films 391, 229 (2001)
H. Dong, G. Zeng, L. Tang, C. Fan, C. Zhang, X. He, Y. He, Water Res. 79, 128 (2015)
K. Zhou, Y. Zhu, X. Yang, X. Jiang, C. Li, New J. Chem. 35, 353 (2011)
J. Zhao, C. Chen, W. Ma, Top. Catal. 35, 269 (2005)
H.M. Yadav, T.V. Kolekar, S.H. Pawar, J.S. Kim, J. Mater. Sci. Mater. Med. 27, 1 (2016)
D. Chen, Z. Jiang, J. Geng, Q. Wang, D. Yang, Ind. Eng. Chem. Res. 46, 2741 (2007)
F. Dong, S. Guo, H. Wang, X. Li, Z. Wu, J. Phys. Chem. C 115, 13285 (2011)
Y. Bessekhouad, D. Robert, J.V. Weber, J. Photochem. Photobiol. A: Chem. 163, 569 (2004)
S. Kim, S.J. Hwang, W. Choi, J. Phys. Chem. B 109, 24260 (2005)
N. Sobana, M. Muruganadham, M. Swaminathan, J. Mol. Catal. A Chem. 258, 124 (2006)
B. Chen, Y. Meng, J. Sha, C. Zhong, W. Hu, N. Zhao, Nanoscale 10, 34 (2018)
C. Donga, S.B. Mishra, A.S. Abd-El-Aziz, A.K. Mishra, J. Inorg. Organomet. Polym. Mater. 31, 463 (2021)
T. Wu, S. Liu, H. Li, L. Wang, X. Sun, J. Nanosci. Nanotechnol. 11, 10078 (2011)
W. Chen, L. Yan, P.R. Bangal, Carbon 48, 1146 (2010)
Y. Han, T. Wang, X. Gao, T. Li, Q. Zhang, Compos. Appl. Sci. Manuf. 84, 336 (2016)
C. Han, N. Zhang, Y.J. Xu, Nano Today 11, 351 (2016)
Q. Quan, X. Lin, N. Zhang, Y.J. Xu, Nanoscale 9, 2398 (2017)
X. Xin, S.H. Li, N. Zhang, Z.R. Tang, Y.J. Xu, Appl. Catal. B Environ. 245, 343 (2019)
N. Zhang, M.Q. Yang, S. Liu, Y. Sun, Y.J. Xu, Chem. Rev. 115, 10307 (2015)
N. Sobahi, M. Imran, M.E. Khan, A. Mohammad, M.M. Alam, T. Yoon et al., Materials 16, 2770 (2023)
F. Sordello, E. Odorici, K. Hu, C. Minero, M. Cerruti, P. Calza, Nanoscale 8, 3407 (2016)
N.T. Padmanabhan, P. Ganguly, S.C. Pillai, H. John, Mater. Today Ener. 17, 100447 (2020)
T. Sugimoto, X. Zhou, A. Muramatsu, J. Colloid Interface Sci. 259, 53 (2003)
X. Cao, G. Tian, Y. Chen, J. Zhou, W. Zhou, C. Tian, H. Fu, J. Mater. Chem. A 2, 4366 (2014)
J. Sun, H. Zhang, L.-H. Guo, L. Zhao, ACS Appl. Mater. Interfaces 5, 13035 (2013)
L. Chen, L. Tian, J. Xie, C. Zhang, J. Chen, Y. Wang, Q. Li, K. Lv, K. Deng, Appl. Surf. Sci. 504, 144353 (2020)
Q. Zhang, N. Bao, X. Wang, X. Hu, X. Miao, M. Chaker, Sci. Rep. 6, 1 (2016)
N.N.T. Ton, A.T.N. Dao, K. Kato, T. Ikenaga, D.X. Trinh, T. Taniike, Carbon 133, 109 (2018)
X. Liu, L. Pan, T. Lv, G. Zhu, T. Lu, Z. Sun, C. Sun, RSC Adv. 1, 1245 (2011)
R. Larciprete, S. Fabris, T. Sun, P. Lacovig, A. Baraldi, S. Lizzit, J. Am. Chem. Soc. 133, 17315 (2011)
T. Xu, L. Zhang, H. Cheng, Y. Zhu, Appl. Catal. B Environ. 101, 382 (2011)
G. Jiang, Z. Lin, C. Chen, L. Zhu, Q. Chang, N. Wang, W. Wei, H. Tang, Carbon 49, 2693 (2011)
H. Bai, J. Zhou, H. Zhang, G. Tang, Colloids Surf. B 150, 68 (2017)
D. Zhang, R. Qiu, L. Song, B. Eric, Y. Mo, X. Huang, J. Hazard. Mater. 163, 843 (2009)
H.H. Mohamed, D.W. Bahnemann, Appl. Catal. B Environ. 128, 91 (2012)
M. Korycka-Dahl, T. Richardson, J. Dairy Sci. 63, 1181 (1980)
J.J. Pignatello, E. Oliveros, A. MacKay, Crit. Rev. Environ. Sci. Technol. 36, 1 (2006)
H. Tang, H. Berger, P.E. Schmid, F. Levy, G. Burri, Solid State Commun. 87, 847 (1993)
H. Tang, K. Prasad, R. Sanjines, P.E. Schmid, F. Levy, J. Appl. Phys. 75, 2042 (1994)
M. Anpo, N. Aikawan, Y. Kubokaway, M. Che, C. Louis, E. Giamello, J. Phys. Chem. 89, 5017 (1985)
Z. Zhang, Y. Huang, K. Liu, L. Guo, Q. Yuan, B. Dong, Adv. Mater. 27, 5906 (2015)
E. Morra, E. Giamello, M. Chiesa, J. Magn. Reson. 280, 89 (2017)
M. Chiesa, M.C. Paganini, S. Livraghi, E. Giamello, Phys. Chem. Chem. Phys. 15, 9435 (2013)
S. Livraghi, M. Chiesa, M.C. Paganini, E. Giamello, J. Phys. Chem. C 115, 25413 (2011)
X. Wang, C. Liow, A. Bisht, X. Liu, T.C. Sum, X. Chen, S. Li, Adv. Mater. 27, 2207 (2015)
T. Takahashi, A. Kudo, S. Kuwabata, A. Ishikawa, H. Ishihara, Y. Tsuboi, T. Torimoto, J. Phys. Chem. C 117, 2511 (2013)
M.Q. Yang, Y.J. Xu, W. Lu, K. Zeng, H. Zhu, Q.H. Xu, G.W. Ho, Nat. Commun. 8, 1 (2017)
S. Wang, B.Y. Guan, X.W.D. Lou, J. Am. Chem. Soc. 140, 5037 (2018)
N.P. Rajkumari, S. Dolakashoria, P. Goswami, ACS Omega 6, 2686 (2021)
G. Sujatha, S. Shanthakumar, F. Chiampo, Environments 7, 47 (2020)
Acknowledgements
The authors would like to offer special thanks to Mr. Le Cong Duy for helping with the time-resolved photoluminescence measurements.
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NNTT was involved in methodology, investigation, formal analysis, visualization, data curation, and writing—review. MC was involved in formal analysis, visualization, data curation, and writing—review. MCP was involved in visualization, data curation, and writing—review. TT was involved in conceptualization, supervision, and writing—review.
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Ton, N.N.T., Paganini, M.C., Chiesa, M. et al. Insight into the mechanism of excellent visible-light photocatalytic activity of TiO2/graphene nanocomposite for photodegradation of organic pollutants in water. Res Chem Intermed 49, 3867–3880 (2023). https://doi.org/10.1007/s11164-023-05075-7
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DOI: https://doi.org/10.1007/s11164-023-05075-7