Zero-valent manganese nanoparticles coupled with different strong oxidants for thallium removal from wastewater

Highlights

• Nano zero-valent manganese (nZVMn, Mn⁰) is synthesized via borohydrides reduction.

• Mn⁰ combined with persulfate/hypochlorite is effective for Tl removal at pH 6-12.

• Mn⁰ can activate persulfate to form hydroxyl and sulfate radicals.

• Oxidation-induced precipitation and surface complexation contribute to Tl removal.

• Combined Mn⁰-oxidants process is promising in the environmental field.

Abstract

Nano zero-valent manganese (nZVMn, Mn⁰) was prepared through a borohydride reduction method and coupled with different oxidants (persulfate (S₂O₈²⁻), hypochlorite (ClO⁻), or hydrogen peroxide (H₂O₂)) to remove thallium (Tl) from wastewater. The surface of Mn⁰ was readily oxidized to form a core-shell composite (MnO_x@Mn⁰), which consists of Mn⁰ as the inner core and MnO_x (MnO, Mn₂O₃, and Mn₃O₄) as the outer layer. When Mn⁰ was added alone, effective Tl(I) removal was achieved at high pH levels (>12). The Mn⁰-H₂O₂ system was only effective in Tl(I) removal at high pH (>12), while the Mn⁰-S₂O₈²⁻ or Mn⁰-ClO⁻ system had excellent Tl(I) removal (>96%) over a broad pH range (4–12). The Mn⁰-S₂O₈²⁻ oxidation system provided the best resistance to interference from an external organic matrix. The isotherm of Tl(I) removal through the Mn⁰-S₂O₈²⁻ system followed the Freundlich model. The Mn⁰ nanomaterials can activate persulfate to produce sulfate radicals and hydroxyl radicals. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy suggested that oxidation-induced precipitation, surface adsorption, and electrostatic attraction are the main mechanisms for Tl(I) removal resulting from the combination of Mn⁰ and oxidants. Mn⁰ coupled with S₂O₈²⁻/ClO⁻ is a novel and effective technique for Tl(I) removal, and its application in other fields is worthy of further investigation.

Graphical abstract

Keywords

Nano zero-valent manganese / Thallium / Adsorption / Oxidation / Sulfate radical / Hydroxyl radical

References

[1] Adio S O, Asif M, Mohammed A R I, Baig N, Al-Arfaj A A, Saleh T A (2019). Poly (amidoxime) modified magnetic activated carbon for chromium and thallium adsorption: Statistical analysis and regeneration. Process Safety and Environmental Protection, 121: 254–262

[2] Belzile N, Chen Y W (2017). Thallium in the environment: A critical review focused on natural waters, soils, sediments and airborne particles. Applied Geochemistry, 84: 218–243

[3] Bernofsky C, Bandara B M, Hinojosa O (1990). Electron spin resonance studies of the reaction of hypochlorite with 5,5-dimethyl-1-pyrroline-N-oxide. Free Radical Biology & Medicine, 8(3): 231–239

[4] Campanella B, D’Ulivo A, Ghezzi L, Onor M, Petrini R, Bramanti E (2018). Influence of environmental and anthropogenic parameters on thallium oxidation state in natural waters. Chemosphere, 196: 1–8

[5] Casella I G, Spera R (2005). Electrochemical deposition of nickel and nickel–thallium composite oxides films from EDTA alkaline solutions. Journal of Electroanalytical Chemistry, 578(1): 55–62doi.org/10.1016/j.jelechem.2004.11.043

[6] Cheam V (2001). Thallium contamination of water in Canada. Water Quality Research Journal, 36(4): 851–877

[7] Chen M, Wu P, Yu L, Liu S, Ruan B, Hu H, Zhu N, Lin Z (2017). FeOOH-loaded MnO₂ nano-composite: An efficient emergency material for thallium pollution incident. Journal of Environmental Management, 192: 31–38

[8] Chen Y D, Ho S H, Wang D, Wei Z S, Chang J S, Ren N Q (2018). Lead removal by a magnetic biochar derived from persulfate-ZVI treated sludge together with one-pot pyrolysis. Bioresource Technology, 247: 463–470

[9] Cheong Y W, Min J S, Kwon K S (1998). Metal removal efficiencies of substrates for treating acid mine drainage of the Dalsung mine, South Korea. Journal of Geochemical Exploration, 64(1–3): 147–152

[10] Chi T, Zuo J, Liu F L (2017). Performance and mechanism for cadmium and lead adsorption from water and soil by corn straw biochar. Frontiers of Environmental Science & Engineering, 11(2): 15

[11] Chu H A, Sackett H, Babcock G T (2000). Identification of a Mn-O-Mn cluster vibrational mode of the oxygen-evolving complex in photosystem II by low-frequency FTIR spectroscopy. Biochemistry, 39(47): 14371–14376

[12] Coetzee P, Fischer J, Hu M (2004). Simultaneous separation and determination of Tl (I) and Tl (III) by IC–ICP-OES and IC–ICP-MS. Water S.A., 29(1): 17–22

[13] Dada A, Adekola F, Odebunmi E (2014). Investigation of the synthesis and characterization of manganese nanoparticles and its ash rice husk supported nanocomposite. In: Proceedings of 1st African International Conference/Workshop on Applications of Nanotechnology to Energy, Health and Environment 2014, Nsukka, Nigeria. Nsukka: UNN, 138–149

[14] Dadfarnia S, Assadollahi T, Haji Shabani A M (2007). Speciation and determination of thallium by on-line microcolumn separation/preconcentration by flow injection-flame atomic absorption spectrometry using immobilized oxine as sorbent. Journal of Hazardous Materials, 148(1–2): 446–452

[15] Dashti Khavidaki H, Aghaie H (2013). Adsorption of Thallium (I) ions using eucalyptus leaves powder. CLEAN–Soil, Air, Water, 41(7): 673–679

[16] DelValls T A, Sáenz V, Arias A M (1999). Thallium in the marine environment: first ecotoxicological assessments in the Guadalquivir estuary and its potential adverse effect on the Do�ana European Natural Reserve after the Aznalcñllar mining spill (SW spain). Ciencias Marinas, 25(2): 161–175

[17] Diao Z H, Xu X R, Chen H, Jiang D, Yang Y X, Kong L J, Sun Y X, Hu Y X, Hao Q W, Liu L (2016). Simultaneous removal of Cr(VI) and phenol by persulfate activated with bentonite-supported nanoscale zero-valent iron: Reactivity and mechanism. Journal of Hazardous Materials, 316: 186–193

[18] Georgi A, Kopinke F D (2005). Interaction of adsorption and catalytic reactions in water decontamination processes: Part I. Oxidation of organic contaminants with hydrogen peroxide catalyzed by activated carbon. Applied Catalysis B: Environmental, 58(1–2): 9–18

[19] Grygo-Szymanko E, Tobiasz A, Walas S (2016). Speciation analysis and fractionation of manganese: A review. TrAC Trends in Analytical Chemistry, 80: 112–124

[20] Huang J, Zhang H (2019). Oxidant or catalyst for oxidation? The role of manganese oxides in the activation of peroxymonosulfate (PMS). Frontiers of Environmental Science & Engineering, 13(5): 65

[21] Huangfu X, Jiang J, Lu X, Wang Y, Liu Y, Pang S Y, Cheng H, Zhang X, Ma J (2015). Adsorption and oxidation of thallium(I) by a nanosized manganese dioxide. Water, Air, & Soil Pollution, 226(1): 2272

[22] Huangfu X, Ma C, Ma J, He Q, Yang C, Zhou J, Jiang J, Wang Y (2017). Effective removal of trace thallium from surface water by nanosized manganese dioxide enhanced quartz sand filtration. Chemosphere, 189: 1–9

[23] Kalaivani S, Muthukrishnaraj A, Sivanesan S, Ravikumar L (2016). Novel hyperbranched polyurethane resins for the removal of heavy metal ions from aqueous solution. Process Safety and Environmental Protection, 104: 11–23

[24] Kaplan D I, Mattigod S V (1998). Aqueous geochemistry of thallium. In: Nriagu J O, ed. Thallium in the Environment. New York, NY, ETATS-UNIS: John Wiley & Sons, 15–30

[25] Lan C H, Lin T S (2005). Acute toxicity of trivalent thallium compounds to Daphnia magna. Ecotoxicology and Environmental Safety, 61(3): 432–435

[26] Li D, Jin Z, Zhou Q, Chen J, Lei Y, Sun S (2010). Discrimination of five species of Fritillaria and its extracts by FT-IR and 2D-IR. Journal of Molecular Structure, 974(1–3): 68–72

[27] Li H, Chen Y, Long J, Jiang D, Liu J, Li S, Qi J, Zhang P, Wang J, Gong J, Wu Q, Chen D (2017a). Simultaneous removal of thallium and chloride from a highly saline industrial wastewater using modified anion exchange resins. Journal of Hazardous Materials, 333: 179–185

[28] Li H, Chen Y, Long J, Li X, Jiang D, Zhang P, Qi J, Huang X, Liu J, Xu R, Gong J (2017b). Removal of thallium from aqueous solutions using Fe-Mn binary oxides. Journal of Hazardous Materials, 338: 296–305

[29] Li H, Li X, Long J, Li K, Chen Y, Jiang J, Chen X, Zhang P (2019a). Oxidation and removal of thallium and organics from wastewater using a zero-valent-iron-based Fenton-like technique. Journal of Cleaner Production, 221: 89–97

[30] Li H, Xiong J, Xiao T, Long J, Wang Q, Li K, Liu X, Zhang G, Zhang H (2019b). Biochar derived from watermelon rinds as regenerable adsorbent for efficient removal of thallium(I) from wastewater. Process Safety and Environmental Protection, 127: 257–266

[31] Li H, Xiong J, Zhang G, Liang A, Long J, Xiao T, Chen Y, Zhang P, Liao D, Lin L, Zhang H (2020a). Enhanced thallium(I) removal from wastewater using hypochlorite oxidation coupled with magnetite-based biochar adsorption. Science of the Total Environment, 698: 134166

[32] Li H S, Li X W, Chen Y H, Long J Y, Zhang G S, Xiao T F, Zhang P, Li C L, Zhuang L Z, Huang W Y (2018a). Removal and recovery of thallium from aqueous solutions via a magnetite-mediated reversible adsorption-desorption process. Journal of Cleaner Production, 199: 705–715

[33] Li H S, Li X W, Xiao T F, Chen Y H, Long J Y, Zhang G S, Zhang P, Li C L, Zhuang L Z, Li K K (2018b). Efficient removal of thallium(I) from wastewater using flower-like manganese dioxide coated magnetic pyrite cinder. Chemical Engineering Journal, 353: 867–877

[34] Li H S, Long J Y, Li X W, Li K K, Xu L L, Lai J P, Chen Y H, Zhang P (2018c). Aqueous biphasic separation of thallium from aqueous solution using alcohols and salts. Desalination and Water Treatment, 123: 330–337

[35] Li H S, Zhang H G, Long J Y, Zhang P, Chen Y H (2019c). Combined Fenton process and sulfide precipitation for removal of heavy metals from industrial wastewater: Bench and pilot scale studies focusing on in-depth thallium removal. Frontiers of Environmental Science & Engineering, 13(4): 49

[36] Li K, Li H, Xiao T, Long J, Zhang G, Li Y, Liu X, Liang Z, Zheng F, Zhang P (2019d). Synthesis of manganese dioxide with different morphologies for thallium removal from wastewater. Journal of Environmental Management, 251: 109563

[37] Li K, Li H, Xiao T, Zhang G, Long J, Luo D, Zhang H, Xiong J, Wang Q (2018d). Removal of thallium from wastewater by a combination of persulfate oxidation and iron coagulation. Process Safety and Environmental Protection, 119: 340–349

[38] Li S, Qi L, Lu L, Wang H (2012). Facile preparation and performance of mesoporous manganese oxide for supercapacitors utilizing neutral aqueous electrolytes. RSC Advances, 2(8): 3298–3308

[39] Li S, Wang W, Liang F, Zhang W X (2017c). Heavy metal removal using nanoscale zero-valent iron (nZVI): Theory and application. Journal of Hazardous Materials, 322(Pt A): 163–171

[40] Li Y,Li H, Liu F, Zhang G, Xu Y, Xiao T, Long J, Chen Z, Liao D, Zhang J, Lin L, Zhang P. (2020b)Zero-valent iron-manganese bimetallic nanocomposites catalyze hypochlorite for enhanced thallium(I) oxidation and removal from wastewater: materials characterization, process optimization and removal mechanisms. Journal of Hazardous Materials, 386: 121900

[41] Liu J, Wang J, Chen Y, Lippold H, Xiao T, Li H, Shen C C, Xie L, Xie X, Yang H (2017a). Geochemical transfer and preliminary health risk assessment of thallium in a riverine system in the Pearl River Basin, South China. Journal of Geochemical Exploration, 176: 64–75

[42] Liu Y, Wang L, Wang X, Huang Z, Xu C, Yang T, Zhao X, Qi J, Ma J (2017b). Highly efficient removal of trace thallium from contaminated source waters with ferrate: Role of in situ formed ferric nanoparticle. Water Research, 124: 149–157

[43] Martin L A, Wissocq A, Benedetti M F, Latrille C (2018). Thallium (Tl) sorption onto illite and smectite: Implications for Tl mobility in the environment. Geochimica et Cosmochimica Acta, 230: 1–16

[44] Memon S Q, Memon N, Solangi A R, Memon J U R (2008). Sawdust: A green and economical sorbent for thallium removal. Chemical Engineering Journal, 140(1–3): 235–240

[45] Nilchi A, Shariati TDehaghan S, Rasouli Garmarodi (2013). Kinetics, isotherm and thermodynamics for uranium and thorium ions adsorption from aqueous solutions by crystalline tin oxide nanoparticles. Desalination, 321: 67–71

[46] Nriagu J O (1998). Thallium in the Environment. New York, NY, ETATS-UNIS: John Wiley & Sons

[47] Pan Z, Qiu Y, Yang J, Ye F, Xu Y, Zhang X, Liu M, Zhang Y (2016). Ultra-endurance flexible all-solid-state asymmetric supercapacitors based on three-dimensionally coated MnO_x nanosheets on nanoporous current collectors. Nano Energy, 26: 610–619

[48] Panda A P, Rout P, Jena K K, Alhassan S M, Kumar S A, Jha U, Dey R, Swain S (2019). Core–shell structured zero-valent manganese (ZVM): A novel nanoadsorbent for efficient removal of As (iii) and As (v) from drinking water. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 7(16): 9933–9947

[49] Parida K M, Mallick S, Mohapatra B K, Misra V N (2004). Studies on manganese-nodule leached residues; 1. Physicochemical characterization and its adsorption behavior toward Ni²⁺ in aqueous system. Journal of Colloid and Interface Science, 277(1): 48–54

[50] Peter A L, Viraraghavan T (2005). Thallium: a review of public health and environmental concerns. Environment International, 31(4): 493–501

[51] Rao P, Mak M S, Liu T, Lai K C, Lo I M (2009). Effects of humic acid on arsenic(V) removal by zero-valent iron from groundwater with special references to corrosion products analyses. Chemosphere, 75(2): 156–162

[52] Reddy A L M, Ramaprabhu S (2007). Hydrogen storage properties of nanocrystalline Pt dispersed multi-walled carbon nanotubes. International Journal of Hydrogen Energy, 32(16): 3998–4004

[53] Rodríguez-Mercado J J, Mosqueda-Tapia G, Altamirano-Lozano M A (2017). Genotoxicity assessment of human peripheral Lymphocytes induced by thallium(I) and thallium(III). Toxicological and Environmental Chemistry, 99(5–6): 987–998

[54] Shah N S, Ali Khan J, Sayed M, Ul Haq Khan Z, Sajid Ali H, Murtaza B, Khan H M, Imran M, Muhammad N (2019). Hydroxyl and sulfate radical mediated degradation of ciprofloxacin using nano zerovalent manganese catalyzed S₂O₈^2–. Chemical Engineering Journal, 356: 199–209

[55] Smith I C, Carson B L (1977). Volume I. Thallium. In: Smith I C, Carson B L, editors, Trace Metals in the Environment. Michigan: 72 Ann Arbor Science Publishers Inc. Ann Arbor, 406

[56] Sorge A R, Turco M, Pilone G, Bagnasco G (2004). Decomposition of hydrogen peroxide on MnO₂/TiO₂ catalysts. Journal of Propulsion and Power, 20(6): 1069–1075

[57] Taşar Ş, Kaya F, Özer A (2014). Biosorption of lead (II) ions from aqueous solution by peanut shells: equilibrium, thermodynamic and kinetic studies. Journal of Environmental Chemical Engineering, 2(2): 1018–1026

[58] Tripathy S S, Bersillon J L, Gopal K (2006). Adsorption of Cd²⁺ on hydrous manganese dioxide from aqueous solutions. Desalination, 194(1–3): 11–21

[59] Tyagi R, Rana P, Khan A R, Bhatnagar D, Devi M M, Chaturvedi S, Tripathi R P, Khushu S (2011). Study of acute biochemical effects of thallium toxicity in mouse urine by NMR spectroscopy. Journal of Applied Toxicology, 31(7): 663–670

[60] Vaněk A, Grösslová Z, Mihaljevič M, Ettler V, Trubač J, Chrastný V, Penížek V, Teper L, Cabala J, Voegelin A, Zádorová T, Oborná V, Drábek O, Holubík O, Houška J, Pavlů L, Ash C (2018). Thallium isotopes in metallurgical wastes/contaminated soils: A novel tool to trace metal source and behavior. Journal of Hazardous Materials, 343: 78–85

[61] Verstraeten S V, Lucangioli S, Galleano M (2009). ESR characterization of thallium(III)-mediated nitrones oxidation. Inorganica Chimica Acta, 362(7): 2305–2310

[62] Wan S, Ma M, Lv L, Qian L, Xu S, Xue Y, Ma Z (2014). Selective capture of thallium (I) ion from aqueous solutions by amorphous hydrous manganese dioxide. Chemical Engineering Journal, 239: 200–206

[63] Wang X, Lian W, Sun X, Ma J, Ning P (2018a). Immobilization of NZVI in polydopamine surface-modified biochar for adsorption and degradation of tetracycline in aqueous solution. Frontiers of Environmental Science & Engineering, 12(4): 9

[64] Wang Z, Xiong W, Tebo B M, Giammar D E (2014). Oxidative UO₂ dissolution induced by soluble Mn(III). Environmental Science & Technology, 48(1): 289–298

[65] Wang Z, Zhang B, Jiang Y, Li Y, He C (2018b). Spontaneous thallium (I) oxidation with electricity generation in single-chamber microbial fuel cells. Applied Energy, 209: 33–42

[66] Wei G, Zhang J, Luo J, Xue H, Huang D, Cheng Z, Jiang X (2019). Nanoscale zero-valent iron supported on biochar for the highly efficient removal of nitrobenzene. Frontiers of Environmental Science & Engineering, 13(4): 61

[67] Wick S, Baeyens B, Marques Fernandes M, Voegelin A (2018). Thallium adsorption onto illite. Environmental Science & Technology, 52(2): 571–580

[68] Xiao T, Yang F, Li S, Zheng B, Ning Z (2012). Thallium pollution in China: A geo-environmental perspective. Science of the Total Environment, 421– 422: 51–58

[69] Xu R B, Su M H, Huang X X, Chen D Y, Long J Y, Liu Y H, Kong L J, Li H S (2019). Efficient removal of thallium and EDTA from aqueous solution via the Fenton process. Desalination and Water Treatment, 154: 166–176

[70] Yu H Y, Chang C, Li F, Wang Q, Chen M, Zhang J (2018). Thallium in flowering cabbage and lettuce: Potential health risks for local residents of the Pearl River Delta, South China. Environmental Pollution, 241: 626–635

[71] Zeng H, Tian S, Liu H, Chai B, Zhao X (2016). Photo-assisted electrolytic decomplexation of Cu-EDTA and Cu recovery enhanced by H₂O₂ and electro-generated active chlorine. Chemical Engineering Journal, 301: 371–379

[72] Zhang G, Fan F, Li X, Qi J, Chen Y (2018). Superior adsorption of thallium(I) on titanium peroxide: Performance and mechanism. Chemical Engineering Journal, 331: 471–479

[73] Zhang H, Li M, Yang Z, Sun Y, Yan J, Chen D, Chen Y (2017). Isolation of a non-traditional sulfate reducing-bacteria Citrobacter freundii sp. and bioremoval of thallium and sulfate. Ecological Engineering, 102: 397–403

[74] Zhao Y S, Lin L, Hong M (2019). Nitrobenzene contamination of groundwater in a petrochemical industry site. Frontiers of Environmental Science & Engineering, 13(2): 29

[75] Zhi S, Tian L, Li N, Zhang K (2018). A novel system of MnO₂-mullite-cordierite composite particle with NaClO for Methylene blue decolorization. Journal of Environmental Management, 213: 392–399

Acknowledgements

This research was supported by the National Natural Science Foundation of China (Grant Nos. 51808144, 51678562, and 41830753), the Science and Technology Program of Guangzhou (Nos. 201906010037 and 201804010281), and the Guangdong Natural Science Foundation (No. 2018A0303130265).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-019-1213-5 and is accessible for authorized users.

RIGHTS & PERMISSIONS

2020 Higher Education Press and Springer-Verlag GmbH Germany, part of Springer Nature