Singlet oxygen synergistic surface-adsorbed hydroxyl radicals for phenol degradation in CoP catalytic photo-Fenton

doi:10.1016/S1872-2067(22)64117-2

Abstract

Abstract:

In recent years, there have been numerous studies on Fenton or Fenton-like reactions mediated by nonfree radicals such as singlet oxygen (¹O₂); however, there are few studies on the synergistic effect of ¹O₂ and free radicals on the degradation of organic molecules, such as phenol in Fenton reaction. In this study, a cocatalyst, CoP, commonly used in photocatalysis was synthesized using a simple two-step method, and a CoP/Fe²⁺/AM1.5 system was constructed by introducing Fe²⁺ and simulated sunlight (AM1.5) irradiation. The newly constructed CoP/Fe²⁺/AM1.5 system could effectively degrade various organic pollutants, including dyes, phenols, and antibiotics. Radical quenching experiments and electron paramagnetic resonance detection confirmed that there were three reactive oxygen species (ROS) in the CoP/Fe²⁺/AM1.5 system, including •OH_ads, •O₂^-, and ¹O₂. Further, combined with the liquid chromatogram of phenol, its intermediate products, and the fluorescence diagram of o-hydroxybenzoic acid, it can be concluded that a synergistic effect exists between ¹O₂ and the surface-adsorbed •OH_ads in the CoP/Fe²⁺/AM1.5 system. The controllable formation of surface ¹O₂ and •OH_ads was achieved through the oxidation (Co³⁺) and reduction (P^δ^-) centers exposed on the CoP surface, and the synergistic effect between them results in phenol’s hydroxylation, ring-opening, and degradation. The study of this new mechanism provides a new perspective for revealing the surface interface reaction between ROS and organic pollutants.

Key words: Surface hydroxyl radical, Singlet oxygen, Synergistic effect, Hydroxylation, Photo-Fenton

Haoran Yu, Danxu Liu, Hengyi Wang, Haishuang Yu, Qingyun Yan, Jiahui Ji, Jinlong Zhang, Mingyang Xing. Singlet oxygen synergistic surface-adsorbed hydroxyl radicals for phenol degradation in CoP catalytic photo-Fenton[J]. Chinese Journal of Catalysis, 2022, 43(10): 2678-2689.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64117-2

https://www.cjcatal.com/EN/Y2022/V43/I10/2678

Figures/Tables 4

Fig. 1. Preparation and characterization of CoP. (a) Schematic of CoP preparation process and corresponding SEM imagine. (b) Powder XRD pattern. (c) HRTEM. (d) Zeta potential at different pH. (e) High resolution Co 2p spectrum. (f) High resolution P 2p spectrum. (g) FT-IR spectrum.

Fig. 2. Degradation of organic pollutants and exploration of reactive oxygen species. (a) Difference of phenol degradation in different systems. (b) Different degradation rates of RhB, SD, 4-CP, and phenol in the CoP/Fe2+/AM1.5 system. (c) Inhibition effect of different free radical scavengers on phenol degradation in CoP/Fe2+/AM1.5 system. (d) EPR spectra of DMPO-•OH in CoP/AM1.5 and CoP/Fe2+/AM1.5 systems. (e) EPR spectra of DMPO•-O2- in CoP/AM1.5 and CoP/Fe2+/AM1.5 systems. (f) EPR spectra of TEMP-1O2 in CoP, CoP/AM1.5, and CoP/Fe2+/AM1.5 systems. (g) Changes in PMSO and PMSO2 concentrations in the CoP/Fe2+/AM1.5 system. (h) H2O2 production of the CoP, CoP/AM1.5, and CoP/Fe2+/AM1.5 systems. (i) Effect of O2 on phenol degradation in the CoP/Fe2+/AM1.5 system. General conditions: [CoP]0 = 1.0 g/L, [Fe2+]0 = 40 mg/L, pHi = 3.0, [phenol/RhB/SD/4-CP]0 = 10 mg/L, [TBA/p-BQ/TEMP]0 = 0.5 mmol/L, [PMSO]0 = 0.1 mmol/L.

Fig. 3. Mechanism exploration, circulation, and anti-interference ability of CoP. (a) Liquid chromatogram of phenol and its degradation intermediates in CoP, CoP/AM1.5, CoP/Fe2+, and CoP/Fe2+/AM1.5 systems. Fluorescence spectra of hydroxybenzoic acid formed by benzoic acid capturing •OH in CoP, CoP/AM1.5, CoP/Fe2+, and CoP/Fe2+/AM1.5 systems (b), CoP + TEMP system (c), CoP/AM1.5 + TEMP system (d). (e) Cyclic degradation experiment of CoP. (f) the anti-interference ability of CoP/Fe2+/AM1.5 system. Note: the peaks of o-diphenol, m-diphenol, and p-diphenol in liquid chromatography are at 2.85, 3.30, and 3.65 min, respectively. General conditions: [CoP]0 = 1.0 g/L, [Fe2+]0 = 40 mg/L, pHi = 3.0, [phenol]0 = 10 mg/L, [benzoic acid]0 = 2.0 mmol/L, [Cl-/SO42-/NO3-/H2PO4-]0 = 10 mmol/L.

Scheme 1. Mechanism diagram of phenol degradation by the synergistic effect of 1O2 and •OHads.

References

[1]	G. Gao, Y. Tian, X. Gong, Z. Pan, K. Yang, B. Zong, Chin. J. Catal., 2020, 41, 1039-1047.
[2]	L. Li, Z. Hu, J. C. Yu, Angew. Chem. Int. Ed., 2020, 59, 20538-20544.
[3]	D. Ma, H. Yi, C. Lai, X. Liu, X. Huo, Z. An, L. Li, Y. Fu, B. Li, M. Zhang, L. Qin, S. Liu, L. Yang, Chemosphere, 2021, 275, 130104.
[4]	J. An, N. Li, Y. Wu, S. Wang, C. Liao, Q. Zhao, L. Zhou, T. Li, X. Wang, Y. Feng, Environ. Sci. Technol., 2020, 54, 10916-10925.
[5]	H. Lee, H. J. Lee, J. Seo, H. E. Kim, Y. K. Shin, J. H. Kim, C. Lee, Environ. Sci. Technol., 2016, 50, 8231-8238.
[6]	J. S. Jirkovský, I. Panas, E. Ahlberg, M. Halasa, S. Romani, D. J. Schiffrin, J. Am. Chem. Soc., 2011, 133, 19432-19441.
[7]	S. Li, G. Dong, R. Hailili, L. Yang, Y. Li, F. Wang, Y. Zeng, C. Wang, Appl. Catal. B, 2016, 190, 26-35.
[8]	Y. Wang, H. Ji, W. Liu, T. Xue, C. Liu, Y. Zhang, L. Liu, Q. Wang, F. Qi, B. Xu, D. C. W. Tsang, W. Chu, ACS Appl. Mater. Inter., 2020, 12, 20522-20535.
[9]	G. K. Ziyatdinova, D. M. Gil'metdinova, G. K. Budnikov, J. Anal. Chem., 2005, 60, 49-52.
[10]	Q. Yi, J. Ji, B. Shen, C. Dong, J. Liu, J. Zhang, M. Xing, Environ. Sci. Technol., 2019, 53, 9725-9733.
[11]	D. Guo, Y. Liu, H. Ji, C. C. Wang, B. Chen, C. Shen, F. Li, Y. Wang, P. Lu, W. Liu, Environ. Sci. Technol., 2021, 55, 4045-4053.
[12]	J. Ji, Q. Yan, P. Yin, S. Mine, M. Matsuoka, M. Xing, Angew. Chem. Int. Ed., 2021, 60, 2903-2908.
[13]	Q. Yan, C. Lian, K. Huang, L. Liang, H. Yu, P. Yin, J. Zhang, M. Xing, Angew. Chem. Int. Ed., 2021, 60, 17155-17163.
[14]	J. Wang, Z. Liu, Y. Zheng, L. Cui, W. Yang, J. Liu, J. Mater. Chem. A, 2017, 5, 22913-22932.
[15]	S. T. Oyama, T. Gott, H. Zhao, Y.-K. Lee, Catal. Today, 2009, 143, 94-107.
[16]	L. Zhang, G. Wang, X. Hao, Z. Jin, Y. Wang, Chem. Eng. J., 2020, 395, 125113.
[17]	H. Kim, J. Lim, S. Lee, H. H. Kim, C. Lee, J. Lee, W. Choi, Environ. Sci. Technol., 2019, 53, 2918-2925.
[18]	P. Wang, S. Zhan, H. Wang, Y. Xia, Q. Hou, Q. Zhou, Y. Li, R. R. Kumar, Appl. Catal. B, 2018, 230, 210-219.
[19]	X. Yue, S. Yi, R. Wang, Z. Zhang, S. Qiu, Small, 2017, 13, 1603301.
[20]	W. Li, Q. Yang, S. Chou, J. Wang, H. Liu, J. Power Sources, 2015, 294, 627-632.
[21]	T. Liu, K. Wang, G. Du, A. M. Asiri, X. Sun, J. Mater. Chem. A, 2016, 4, 13053-13057.
[22]	R. Liang, Y. Wang, C. Qin, X. Chen, Z. Ye, L. Zhu, Langmuir, 2021, 37, 3321-3330.
[23]	H. B. M. Sidek, X. Jin, M. S. Islam, S. J. Hwang, ChemCatChem, 2019, 11, 6099-6104.
[24]	D. Zhu, L. Wang, M. Qiao, J. Liu, Chem. Commun., 2020, 56, 7159-7162.
[25]	D. Zhu, Q. Zhen, J. Xin, H. Ma, L. Tan, H. Pang, X. Wang, Sensor. Actuat. B, 2020, 321, 128541.
[26]	B. Pradhan, G. S. Kumar, A. Dalui, A. H. Khan, B. Satpati, Q. Ji, L. K. Shrestha, K. Ariga, S. Acharya, J. Mater. Chem. C, 2016, 4, 4967-4977.
[27]	W. Maneeprakorn, M. A. Malik, P. O'Brien, J. Mater. Chem. A, 2010, 20, 2329-2335.
[28]	D. Dai, H. Xu, L. Ge, C. Han, Y. Gao, S. Li, Y. Lu, Appl. Catal. B, 2017, 217, 429-436.
[29]	H. Li, J. Shang, Z. Yang, W. Shen, Z. Ai, L. Zhang, Environ. Sci. Technol., 2017, 51, 5685-5694.
[30]	X. Xu, X. Li, X. Li, H. Li, Sep. Purif. Technol., 2009, 68, 261-266.
[31]	L. Clarizia, D. Russo, I. Di Somma, R. Marotta, R. Andreozzi, Appl. Catal. B, 2017, 209, 358-371.
[32]	M. P. Bradshaw, C. Barril, A. C. Clark, P. D. Prenzler, G. R. Scollary, Crit. Rev. Food Sci. Nutr., 2011, 51, 479-498.
[33]	L. Xu, L. Meng, X. Zhang, X. Mei, X. Guo, W. Li, P. Wang, L. Gan, J. Hazard. Mater., 2019, 379, 120795.
[34]	K. Maeda, H. Hashiguchi, H. Masuda, R. Abe, K. Domen, J. Phys. Chem. C, 2008, 112, 3447-3452.
[35]	R. C. Gilson, K. C. Black, D. D. Lane, S. Achilefu, Angew. Chem. Int. Ed., 2017, 129, 10857-10860.
[36]	T. Liu, L. Zou, D. Feng, Y. Chen, S. Fordham, X. Wang, Y. Liu, H. Zhou, J. Am. Chem. Soc., 2014, 136, 7813-7816.
[37]	L. Chen, X. Li, J. Zhang, J. Fang, Y. Huang, P. Wang, J. Ma, Environ. Sci. Technol., 2015, 49, 10373-10379.
[38]	G. Huang, J. Si, C. Qian, W. Wang, S. Mei, C. Wang, H. Yu, Anal. Chem., 2018, 90, 14439-14446.
[39]	K. Briviba, T. P. A. Devasagayam, H. Sies, S. Steenken, Chem. Res. Toxicol., 1993, 6, 548-553.
[40]	Y. Zhou, J. Jiang, Y. Gao, S. Pang, Y. Yang, J. Ma, J. Gu, J. Li, Z. Wang, L. Wang, L. Yuan, Y. Yang,, Water Res., 2017, 125, 209-218.
[41]	A. Takayanagi, M. Kobayashi, Y. Kawase, Environ. Sci. Pollut. Res., 2017, 24, 8087-8097.