Catalytic Degradation of Phenol by Persulfate Activation Using Cu2(NO3)(OH)3

Abstract Advanced oxidation processes have attracted more and more attention in the treatment of wastewater with high phenol concentration via the activation of persulfate. In this study, we investigated the degradation effect and mechanism of phenol in wastewater by Cu₂(NO₃)(OH)₃ and persulfate. The results show that Cu₂(NO₃)(OH)₃-persulfate systems exhibit high degradation efficiency of phenol in a wide pH range from weak acid to base (pH 5.0—10.0). Analyses of total organic carbon (TOC) show that the system could completely mineralize the phenol with the initial concentration of 100 mg·L^-1 within 4 h at pH 8.0 in the coexistence of 1 g·L^-1 persulfate and 1 g·L^-1 Cu₂(NO₃)(OH)₃. Quenching experiments and electron paramagnetic resonance (EPR) further suggest that O₂^·-, SO₄^·- and ¹O₂ make mainly contribution in the removal of phenol.

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	Wang Xiangming
	Wu Songhai
	Wang Cong
	Li Rui
	Sun Shiwei
	Meng Zihe
	Han Xu

Keywords： phenol； persulfate； Cu₂(NO₃)(OH)₃

Received 2020-03-13;

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Wang Xiangming, Wu Songhai, Wang Cong, Li Rui, Sun Shiwei, Meng Zihe, Han Xu.Catalytic Degradation of Phenol by Persulfate Activation Using Cu₂(NO₃)(OH)₃[J] Chemcial Industry and Engineering, 2021,V38(1): 69-78

[1] Esplugas S, Giménez J, Contreras S, et al. Comparison of different advanced oxidation processes for phenol degradation[J]. Water Research, 2002, 36(4):1034-1042
[2] Sprynskyy M, Lebedynets M, Namie J, et al. Phenolics occurrence in surface water of the Dniester river basin (West Ukraine):Natural background and industrial pollution[J]. Environmental Geology, 2007, 53(1):67-75
[3] Wu C, Liu X, Wei D, et al. Photosonochemical degradation of phenol in water[J]. Water Research, 2001, 35(16):3927-3933
[4] Li Z, Wu M, Jiao Z, et al. Extraction of phenol from wastewater by N-octanoylpyrrolidine[J]. Journal of Hazardous Materials, 2004, 114(1/2/3):111-114
[5] Alzaydien A S, Manasreh W. Equilibrium, kinetic and thermodynamic studies on the adsorption of phenol onto activated phosphate rock[J]. International Journal of Physical Sciences, 2009, 4(4):172-181
[6] Banat F A, Al-Bashir B, Al-Asheh S et al. Adsorption of phenol by bentonite[J]. Environ Pollut, 2000, 107(3):391-398
[7] Cahn R P, Li N. Separation of phenol from waste water by the liquid membrane technique[J]. Separation Science, 1974, 9(6):505-519
[8] Klibanov A M, Tu T M, Scott K P. Peroxidase-Catalyzed removal of phenols from coal-conversion waste waters[J]. Science, 1983, 221(4607):259-261
[9] Marrot B, Barrios-Martinez A, Moulin P, et al. Biodegradation of high phenol concentration by activated sludge in an immersed membrane bioreactor[J]. Biochemical Engineering Journal, 2006, 30(2):174-183
[10] De Sucre V S, Watkinson A P. Anodic oxidation of phenol for waste water treatment[J]. The Canadian Journal of Chemical Engineering, 1980, 58(6):52-59
[11] Liu Y, He X, Fu Y, et al. Degradation kinetics and mechanism of oxytetracycline by hydroxyl radical-based advanced oxidation processes[J]. Chemical Engineering Journal, 2016, 284:1317-1327
[12] Hu P, Long M. Cobalt-Catalyzed sulfate radical-based advanced oxidation:A review on heterogeneous catalysts and applications[J]. Applied Catalysis B:Environmental, 2016, 181:103-117
[13] Dewil R, Appels L, Baeyens J. Improving the heat transfer properties of waste activated sludge by advanced oxidation processes[EB/OL]. 2007
[14] Neyens E, Baeyens J. A review of classic Fenton's peroxidation as an advanced oxidation technique[J]. Journal of Hazardous Materials, 2003, 98(1/2/3):33-50
[15] Haber F, Weiss J. The catalytic decomposition of hydrogen peroxide by iron salts[J]. Proceedings of the Royal Society of London Series A-Mathematical and Physical Sciences, 1934, 147(861):332-351
[16] Walling C. Fenton's reagent revisited[J]. Accounts of Chemical Research, 1975, 8(4):125-131
[17] House D A. Kinetics and mechanism of oxidations by peroxydisulfate[J]. Chem Rev, 1962, 62(3):185-203
[18] Rao Y, Qu L, Yang H, et al. Degradation of carbamazepine by Fe(Ⅱ)-activated persulfate process[J]. Journal of Hazardous Materials, 2014, 268:23-32
[19] Liang C, Liang C, Chen C. pH dependence of persulfate activation by EDTA/Fe(Ⅲ) for degradation of trichloroethylene[J]. Journal of Contaminant Hydrology, 2009, 106(3/4):173-182
[20] Wang W, Song J, Han X. Schwertmannite as a new Fenton-like catalyst in the oxidation of phenol by H₂O₂[J]. Journal of Hazardous Materials, 2013, 262:412-419
[21] Wang Q, Cao Y, Zeng H, et al. Ultrasound-Enhanced zero-valent copper activation of persulfate for the degradation of bisphenol AF[J]. Chemical Engineering Journal, 2019, doi:10.1016/j.cej.2019.122143
[22] Lau T K, Chu W, Graham N. The aqueous degradation of butylated hydroxyanisole by UV/S₂O₈^2-:Study of reaction mechanisms via dimerization and mineralization[J]. Environmental Science & Technology, 2007, 41(2):613-619
[23] Moradi M, Ghanbari F, Manshouri M et al. Photocatalytic degradation of azo dye using nano-ZrO₂/UV/Persulfate:Response surface modeling and optimization[J]. Korean J. Chem. Eng. 2015, 33:539-546
[24] Yang S, Yang X, Shao X, et al. Activated carbon catalyzed persulfate oxidation of Azo dye acid orange 7 at ambient temperature[J]. Journal of Hazardous Materials, 2011, 186(1):659-666
[25] Furman O S, Teel A L, Ahmad M, et al. Effect of basicity on persulfate reactivity[J]. Journal of Environmental Engineering, 2011, 137(4):241-247
[26] Liu C, Shih K, Sun C, et al. Oxidative degradation of propachlor by ferrous and copper ion activated persulfate[J]. Science of the Total Environment, 2012, 416:507-512
[27] Lin Y, Liang C, Chen J. Feasibility study of ultraviolet activated persulfate oxidation of phenol[J]. Chemosphere, 2011, 82(8):1168-1172
[28] Lei Y, Chen C, Tu Y, et al. Heterogeneous degradation of organic pollutants by persulfate activated by CuO-Fe₃O₄:Mechanism, stability, and effects of pH and bicarbonate ions[J]. Environmental Science & Technology, 2015, 49(11):6838-6845
[29] Bovio B, Locchi S. Crystal structure of the orthorhombic basic copper nitrate, Cu₂(OH)₃NO₃[J]. Journal of Crystallographic and Spectroscopic Research, 1982, 12(6):507-517
[30] Zhan Y, Zhou X, Fu B, et al. Catalytic wet peroxide oxidation of azo dye (Direct Blue 15) using solvothermally synthesized copper hydroxide nitrate as catalyst[J]. Journal of Hazardous Materials, 2011, 187(1/2/3):348-354
[31] Shen L, Liang S, Wu W, et al. Multifunctional NH₂^- mediated zirconium metal-organic framework as an efficient visible-light-driven photocatalyst for selective oxidation of alcohols and reduction of aqueous Cr(Ⅵ)[J]. Dalton Transactions, 2013, 42(37):13649-13657
[32] Henrist C, Traina K, Hubert C, et al. Study of the morphology of copper hydroxynitrate nanoplatelets obtained by controlled double jet precipitation and urea hydrolysis[J]. Journal of Crystal Growth, 2003, 254(1/2):176-187
[33] Petersen A B, Gniadecki R, Vicanova J, et al. Hydrogen peroxide is responsible for UVA-induced DNA damage measured by alkaline comet assay in HaCaT keratinocytes[J]. Journal of Photochemistry and Photobiology B:Biology, 2000, 59(1/2/3):123-131
[34] Liang C, Su H. Identification of sulfate and hydroxyl radicals in thermally activated persulfate[J]. Industrial & Engineering Chemistry Research, 2009, 48(11):5558-5562
[35] Devi P, Das U, Dalai A K. In-situ chemical oxidation:Principle and applications of peroxide and persulfate treatments in wastewater systems[J]. Science of The Total Environment, 2016, 571:643-657
[36] Buxton G V, Greenstock C L, Helman W P, et al. Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (·OH/·O-in aqueous solution[J]. Journal of Physical and Chemical Reference Data, 1988, 17(2):513-886
[37] Neta P, Huie R E, Ross A B. Rate constants for reactions of inorganic radicals in aqueous solution[J]. Journal of Physical and Chemical Reference Data, 1988, 17(3):1027-1284
[38] Xu T, Kamat P V, O'Shea K E. Mechanistic evaluation of arsenite oxidation in TiO₂Assisted photocatalysis[J]. The Journal of Physical Chemistry A, 2005, 109(40):9070-9075
[39] Duan X, Ao Z, Zhang H, et al. Nanodiamonds in sp2/sp3 configuration for radical to nonradical oxidation:Core-Shell layer dependence[J]. Applied Catalysis B:Environmental, 2018, 222:176-181
[40] Cheng X, Guo H, Zhang Y, et al. Non-Photochemical production of singlet oxygen via activation of persulfate by carbon nanotubes[J]. Water Research, 2017, 113:80-88
[41] Gsponer H E, Previtali C M, García N A. Kinetics of the photosensitized oxidation of polychlorophenols in alkaline aqueous solution[J]. Toxicological & Environmental Chemistry, 1987, 16(1):23-37
[42] Qi C, Liu X, Ma J, et al. Activation of peroxymonosulfate by base:Implications for the degradation of organic pollutants[J]. Chemosphere, 2016, 151:280-288
[43] Wang J, Wang S. Activation of persulfate (PS) and peroxymonosulfate (PMS) and application for the degradation of emerging contaminants[J]. Chemical Engineering Journal, 2018, 334:1502-1517
[44] Yang Y, Pignatello J J, Ma J, et al. Comparison of halide impacts on the efficiency of contaminant degradation by sulfate and hydroxyl radical-based advanced oxidation processes (AOPs)[J]. Environmental Science & Technology, 2014, 48(4):2344-2351
[45] Herrmann H, Reese A, Zellner R. Time-Resolved UV/VIS diode array absorption spectroscopy of SO^-_x(x=3, 4, 5) radical anions in aqueous solution[J]. Journal of Molecular Structure, 1995, 348:183-186
[46] Mehdi A, Farshid G. Degradation of organic pollutants by photoelectro-peroxone/ZVI process:Synergistic, kinetic and feasibility studies[J]. J Environ Manage, 2018, 228:32-39
[47] Wei Z, Villamena F A, Weavers L K. Kinetics and mechanism of ultrasonic activation of persulfate:An in situ EPR spin trapping study[J]. Environmental Science & Technology, 2017, 51(6):3410-3417
[48] Furman O S, Teel A L, Watts R J. Mechanism of base activation of persulfate[J]. Environmental Science & Technology, 2010, 44(16):6423-6428
[49] Ike I A, Linden K G, Orbell J D, et al. Critical review of the science and sustainability of persulphate advanced oxidation processes[J]. Chemical Engineering Journal, 2018, 338:651-669
[50] Yang W, Jiang Z, Hu X, et al. Enhanced activation of persulfate by nitric acid/annealing modified multi-walled carbon nanotubes via non-radical process[J]. Chemosphere, 2019, 220:514-522