Efficient degradation of orange II by ZnMn₂O₄ in a novel photo-chemical catalysis system

Abstract

A ZnMn₂O₄ catalyst has been synthesized via a sucrose-aided combustion method and characterized by various analytical techniques. It is composed of numerous nanoparticles (15–110 nm) assembled into a porous structure with a specific surface area (SSA) of 19.1 m²·g^–1. Its catalytic activity has been investigated for the degradation of orange II dye using three different systems, i.e., the photocatalysis system with visible light, the chemocatalysis system with bisulfite, and the photo-chemical catalysis system with both visible light and bisulfite. The last system exhibits the maximum degradation efficiency of 90%, much higher than the photocatalysis system (15%) and the chemocatalysis system (67%). The recycling experiments indicate that the ZnMn₂O₄ catalyst has high stability and reusability and is thus a green and eximious catalyst. Furthermore, the potential degradation mechanisms applicable to the three systems are discussed with relevant theoretical analysis and scavenging experiments for radicals. The active species such as Mn(III), O₂^•−, h⁺, e_aq^–, SO₄^•− and HO^• are proposed to be responsible for the excellent degradation results in the photo-chemical catalysis system with the ZnMn₂O₄ catalyst.

Key words： ZnMn₂O₄; photo-chemical catalysis; bisulfite; dye degradation

Acknowledgments

This work was supported by the National Natural Science Foundation of China (Grant No. 21477009), Natural Science Foundation of Jiangsu Province (No. SBK2016021419), “333 project” of Jiangsu Province and the Opening Project of Guangxi Key Laboratory of Green Processing of Sugar Resources (No. GXTZY201803). One of us (SK) was supported by the College of Agricultural Sciences under Station Research Project No. PEN04566.

References

1 Gupta V K, Ali I, Saleh T A, Nayak A, Agarwal S. Chemical treatment technologies for waste-water recycling: An overview. RSC Advances, 2012, 2(16): 6380–6388

2 Li J P, Xu Y, Liu Y, Wu D, Sun Y H. Synthesis of hydrophilic ZnS nanocrystals and their application in photocatalytic degradation of dye pollutants. China Particuology, 2004, 2(6): 266–269

3 Chong M N, Jin B, Chow C W K, Saint C. Recent developments in photocatalytic water treatment technology: A review. Water Research, 2010, 44(10): 2997–3027

4 Shukla P R, Wang S, Ang H M, Tadé M O. Photocatalytic oxidation of phenolic compounds using zinc oxide and sulphate radicals under artificial solar light. Separation and Purification Technology, 2010, 70(3): 338–344

5 Ludi B, Niederberger M. Zinc oxide nanoparticles: Chemical mechanisms and classical and non-classical crystallization. Dalton Transactions (Cambridge, England), 2013, 42(35): 12554–12568

6 Liu S W, Li C, Yu J G, Xiang Q J. Improved visible-light photocatalytic activity of porous carbon self-doped ZnO nanosheet-assembled flowers. CrystEngComm, 2011, 13(7): 2533–2541

7 Duan L, Sun B, Wei M, Luo S, Pan F, Xu A, Li X. Catalytic degradation of acid orange 7 by manganese oxide octahedral molecular sieves with peroxymonosulfate under visible light irradiation. Journal of Hazardous Materials, 2015, 285: 356–365

8 Hocking R K, Brimblecombe R, Chang L Y, Singh A, Cheah M H, Glover C, Casey W H, Spiccia L. Water-oxidation catalysis by manganese in a geochemical-like cycle. Nature Chemistry, 2011, 3(6): 461–466

9 Zhang L, Yang C, Xie Z, Wang X. Cobalt manganese spinel as an effective cocatalyst for photocatalytic water oxidation. Applied Catalysis B: Environmental, 2018, 224: 886–894

10 Cheng F, Shen J, Peng B, Pan Y, Tao Z, Chen J. Rapid room-temperature synthesis of nanocrystalline spinels as oxygen reduction and evolution electrocatalysts. Nature Chemistry, 2011, 3(1): 79–84

11 Menaka, Samal S L, Ramanujachary K V, Lofland S E, Govind , Ganguli A K. Stabilization of Mn(IV) in nanostructured zinc manganese oxide and their facile transformation from nanospheres to nanorods. Journal of Materials Chemistry, 2011, 21(24): 8566–8573

12 Cady C W, Gardner G, Maron Z O, Retuerto M, Go Y B, Segan S, Greenblatt M, Dismukes G C. Tuning the electrocatalytic water oxidation properties of AB₂O₄ spinel nanocrystals: A (Li, Mg, Zn) and B (Mn, Co) site variants of LiMn₂O₄. ACS Catalysis, 2015, 5(6): 3403–3410

13 Cui B, Lin H, Liu Y Z, Li J B, Sun P, Zhao X C, Liu C J. Photophysical and photocatalytic properties of core-ring structured NiCo₂O₄ nanoplatelets. Journal of Physical Chemistry C, 2009, 113(32): 14083–14087

14 Khaksar M, Amini M, Boghaei D M. Efficient and green oxidative degradation of methylene blue using Mn-doped ZnO nanoparticles (Zn_1−xMn_xO). Journal of Experimental Nanoscience, 2015, 10(16): 1256–1268

15 Qiu M, Chen Z, Yang Z, Li W, Tian Y, Zhang W, Xu Y, Cheng H. ZnMn₂O₄ nanorods: An effective Fenton-like heterogeneous catalyst with t_2g³e_g¹ electronic configuration. Catalysis Science & Technology, 2018, 8(10): 2557–2566

16 Borhade A V, Tope D R, Dabhade G B. Removal of erioglaucine dye from aqueous medium using ecofriendly synthesized ZnMnO₃ photocatalyst. e-Journal of Surface Science and Nanotechnology, 2017, 15: 74–80

17 Li C J, Xu G R. Zn-Mn-O heterostructures: Study on preparation, magnetic and photocatalytic properties. Materials Science and Engineering B, 2011, 176(7): 552–558

18 Yuan S, Fan Y, Zhang Y, Tong M, Liao P. Pd-catalytic in situ generation of H₂O₂ from H₂ and O₂ produced by water electrolysis for the efficient electro-fenton degradation of rhodamine B. Environmental Science & Technology, 2011, 45(19): 8514–8520

19 Sun H, Liu S Z, Zhou G, Ang M, Tade M, Wang S. Reduced graphene oxide for catalytic oxidation of aqueous organic pollutants. ACS Applied Materials & Interfaces, 2012, 4(10): 5466–5471

20 Guo Y, Lou X, Fang C, Xiao D, Wang Z, Liu J. Novel photo-sulfite system: Toward simultaneous transformations of inorganic and organic pollutants. Environmental Science & Technology, 2013, 47(19): 11174–11181

21 Zhang B T, Zhang Y, Teng Y, Fan M. Sulfate radical and its application in decontamination technologies. Critical Reviews in Environmental Science and Technology, 2015, 45(16): 1756–1800

22 Anipsitakis G P, Dionysiou D D. Degradation of organic contaminants in water with sulfate radicals generated by the conjunction of peroxymonosulfate with cobalt. Environmental Science & Technology, 2003, 37(20): 4790–4797

23 Antoniou M G, de la Cruz A A, Dionysiou D D. Degradation of microcystin-LR using sulfate radicals generated through photolysis, thermolysis and e-transfer mechanisms. Applied Catalysis B: Environmental, 2010, 96(3): 290–298

24 Tan C, Gao N, Deng Y, Zhang Y, Sui M, Deng J, Zhou S. Degradation of antipyrine by UV, UV/H₂O₂ and UV/PS. Journal of Hazardous Materials, 2013, 260: 1008–1016

25 Qi C, Liu X, Ma J, Lin C, Li X, Zhang H. Activation of peroxymonosulfate by base: Implications for the degradation of organic pollutants. Chemosphere, 2016, 151: 280–288

26 Furman O S, Teel A L, Watts R J. Mechanism of base activation of persulfate. Environmental Science & Technology, 2010, 44(16): 6423–6428

27 Yang Q, Choi H, Al-Abed S R, Dionysiou D D. Iron-cobalt mixed oxide nanocatalysts: Heterogeneous peroxymonosulfate activation, cobalt leaching, and ferromagnetic properties for environmental applications. Applied Catalysis B: Environmental, 2009, 88(3-4): 462–469

28 Chen X, Chen J, Qiao X, Wang D, Cai X. Performance of nano-Co₃O₄/peroxymonosulfate system : Kinetics and mechanism study using acid orange 7 as a model compound. Applied Catalysis B: Environmental, 2008, 80(1-2): 116–121

29 Govindan K, Raja M, Noel M, James E J. Degradation of pentachlorophenol by hydroxyl radicals and sulfate radicals using electrochemical activation of peroxomonosulfate, peroxodisulfate and hydrogen peroxide. Journal of Hazardous Materials, 2014, 272(4): 42–51

30 Jie W, Hui Z, Qiu J. Degradation of acid orange 7 in aqueous solution by a novel electro/Fe²⁺/peroxydisulfate process. Journal of Hazardous Materials, 2012, 215-216(4): 138–145

31 Liu X, Zhang X, Zhang K, Qi C. Sodium persulfate-assisted mechanochemical degradation of tetrabromobisphenol A: Efficacy, products and pathway. Chemosphere, 2016, 150: 551–558

32 Yan X, Liu X, Qi C, Wang D, Lin C. Mechanochemical destruction of a chlorinated polyfluorinated ether sulfonate (F-53B, a PFOS alternative) assisted by sodium persulfate. RSC Advances, 2015, 5(104): 85785–85790

33 Qi C, Liu X, Li Y, Lin C, Ma J, Li X, Zhang H. Enhanced degradation of organic contaminants in water by peroxydisulfate coupled with bisulfite. Journal of Hazardous Materials, 2017, 328(Complete): 98–107

34 Sun B, Guan X, Fang J, Tratnyek P G. Activation of manganese oxidants with bisulfite for enhanced oxidation of organic contaminants: The involvement of Mn(III). Environmental Science & Technology, 2015, 49(20): 12414–12421

35 Sun B, Li D, Linghu W, Guan X. Degradation of ciprofloxacin by manganese(III) intermediate: Insight into the potential application of permanganate/bisulfite process. Chemical Engineering Journal, 2018, 339: 144–152

36 Sun B, Dong H, He D, Rao D, Guan X. Modeling the kinetics of contaminants oxidation and the generation of manganese(III) in the permanganate/bisulfite process. Environmental Science & Technology, 2016, 50(3): 1473–1482

37 Zhao C, Hu Z, Teng Z, Liu K, Zhao D. Porous ZnMnO₃ plates prepared from Zn/Mn-sucrose composite as high-performance lithium-ion battery anodes. Micro & Nano Letters, 2016, 11(9): 494–497

38 Cai C, Zhang Z, Liu J, Shan N, Zhang H, Dionysiou D D. Visible light-assisted heterogeneous Fenton with ZnFe₂O₄ for the degradation of orange II in water. Applied Catalysis B: Environmental, 2016, 182: 456–468

39 Ni Q, Ma J, Fan C, Kong Y, Peng M, Komarneni S. Spinel-type cobalt-manganese oxide catalyst for degradation of orange II using a novel heterogeneous photo-chemical catalysis system. Ceramics International, 2018, 44(16): 19474–19480

40 Oh W D, Dong Z, Lim T T. Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal: Current development, challenges and prospects. Applied Catalysis B: Environmental, 2016, 194: 169–201

41 Xie B, Li X, Huang X, Xu Z, Zhang W, Pan B. Enhanced debromination of 4-bromophenol by the UV/sulfite process: Efficiency and mechanism. Journal of Environmental Sciences (China), 2017, 54(4): 231–238

42 Ma H, Wang M, Yang R, Wang W, Zhao J, Shen Z, Yao S. Radiation degradation of Congo red in aqueous solution. Chemosphere, 2007, 68(6): 1098–1104

43 Xu T, Zhu R, Zhu G, Zhu J, Liang X, Zhu Y, He H. Mechanisms for the enhanced photo-Fenton activity of ferrihydrite modified with BiVO₄ at neutral pH. Applied Catalysis B: Environmental, 2017, 212: 50–58

44 Rauf M A, Ashraf S S. Radiation induced degradation of dyes-An overview. Journal of Hazardous Materials, 2009, 166(1): 6–16

45 Xu T, Zhu R, Zhu J, Liang X, Liu Y, Xu Y, He H. Ag₃PO₄ immobilized on hydroxy-metal pillared montmorillonite for the visible light driven degradation of acid red 18. Catalysis Science & Technology, 2016, 6(12): 4116–4123

46 Sun S, Pang S, Jiang J, Ma J, Huang Z, Zhang J, Liu Y, Xu C, Liu Q, Yuan Y. The combination of ferrate(VI) and sulfite as a novel advanced oxidation process for enhanced degradation of organic contaminants. Chemical Engineering Journal, 2018, 333: 11–19

47 Ranguelova K, Rice A B, Khajo A, Triquigneaux M, Garantziotis S, Magliozzo R S, Mason R P. Formation of reactive sulfite-derived free radicals by the activation of human neutrophils: An ESR study. Free Radical Biology & Medicine, 2012, 52(8): 1264–1271

48 Zou J, Ma J, Chen L W, Li X C, Guan Y H, Xie P C, Pan C. Rapid acceleration of ferrous iron/peroxymonosulfate oxidation of organic pollutants by promoting Fe(III)/Fe(II) cycle with hydroxylamine. Environmental Science & Technology, 2013, 47(20): 11685–11691

49 Liu M, Du Y, Ma L, Jing D, Guo L. Manganese doped cadmium sulfide nanocrystal for hydrogen production from water under visible light. International Journal of Hydrogen Energy, 2012, 37(1): 730–736

50 Paul S, Chetri P, Choudhury A. Effect of manganese doping on the optical property and photocatalytic activity of nanocrystalline titania: Experimental and theoretical investigation. Journal of Alloys and Compounds, 2014, 583: 578–586

51 Mezyk S P, Neubauer T J, Cooper W J, Peller J R. Free-radical-induced oxidative and reductive degradation of sulfa drugs in water: absolute kinetics and efficiencies of hydroxyl radical and hydrated electron reactions. Journal of Physical Chemistry A, 2007, 111(37): 9019–9024