Abstract
Soil contamination with polycyclic aromatic hydrocarbons (PAHs) is a serious problem in Northeast China, especially in the steel industrial area. The objective of this study was to evaluate the feasibility of using basic oxygen furnace (BOF) slag to activate the Fenton-like remediation of PAH-contaminated soil to achieve the objectives of “waste control by waste” and “resource recycling” in Chinese steel industry. The effects of BOF slag dosages, H2O2 concentrations, and exothermicity-driven evaporation were evaluated with respect to the removal efficiencies of phenanthrene (Phe) and pyrene (Pyr). Results indicated that PAH oxidation was proportional to the BOF slag dosages and was increased exponentially with H2O2 concentrations. Evaporation due to increasing temperature caused by exothermic reaction played an important role in total soil PAH losses. The sequential Fenton-like oxidation with a 3-times application of 15% H2O2 and the same BOF slag repeatedly used were able to remove 65.87% of Phe and 58.33% of Pyr, respectively. Soluble iron oxides containing in BOF slag were reduced, while amorphous iron oxide concentration remained stable during the repeated Fenton-like process. Column study mimics real field applications showing high removal efficiencies of Phe (36.05–83.20%) and Pyr (21.79–68.06%) in 30-cm depth of soil profile. The tests on soluble heavy metal concentrations after the reactions with high slag dosage or high H2O2 concentration confirmed that BOF slag would not cause heavy metal contamination. Consequently, BOF slag may provide an efficient way for enhancing the Fenton-like based remediation of heavily PAH-polluted soil with little risk on collateral heavy metal contamination. However, an external gas collection and purification equipment would be essential to eliminate the evaporated PAHs.
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References
Albanese S, Fontaine B, Chen W, Lima A, Cannatelli C, Piccolo A, Qi S, Wang M, De Vivo B (2015) Polycyclic aromatic hydrocarbons in the soils of a densely populated region and associated human health risks: the Campania Plain (Southern Italy) case study. Environ Geochem Health 37:1–20. https://doi.org/10.1007/s10653-014-9626-3
Anotai J, Sakulkittimasak P, Boonrattanakij N, Lu MC (2009) Kinetics of nitrobenzene oxidation and iron crystallization in fluidized-bed Fenton process. J Hazard Mater 165:874–880. https://doi.org/10.1016/j.jhazmat.2008.10.062
Bokare AD, Choi W (2014) Review of iron-free Fenton-like systems for activating H2O2 in advanced oxidation processes. J Hazard Mater 275:121–135. https://doi.org/10.1016/j.jhazmat.2014.04.054
Boonrattanakij N, Lu MC, Anotai J (2011) Iron crystallization in a fluidized-bed Fenton process. Water Res 45:3255–3262. https://doi.org/10.1016/j.watres.2011.03.045
Bossmann SH, Oliveros E, Göb S, Siegwart S, Dahlen EP, Payawan L, Straub M, Wörner M, Braun AM (1998) New evidence against hydroxyl radicals as reactive intermediates in the thermal and photochemically enhanced Fenton reactions. J Phys Chem A 102:5542–5550. https://doi.org/10.1021/jp980129j
Chen Y, Zhang J, Zhang F, Li F, Zhou M (2018) Polycyclic aromatic hydrocarbons in farmland soils around main reservoirs of Jilin Province, China: occurrence, sources and potential human health risk. Environ Geochem Health 40:791–802. https://doi.org/10.1007/s10653-017-0024-5
Cheng M, Zeng G, Huang D, Lai C, Xu P, Zhang C, Liu Y (2016a) Hydroxyl radicals based advanced oxidation processes (AOPs) for remediation of soils contaminated with organic compounds: a review. Chem Eng J 284:582–598. https://doi.org/10.1016/j.cej.2015.09.001
Cheng M, Zeng G, Huang D, Lai C, Xu P, Zhang C, Liu Y, Wan J, Gong X, Zhu Y (2016b) Degradation of atrazine by a novel Fenton-like process and assessment the influence on the treated soil. J Hazard Mater 312:184–191. https://doi.org/10.1016/j.jhazmat.2016.03.033
Chiou CS, Chang CF, Chang CT, Shie JL, Chen YH (2006) Mineralization of reactive black 5 in aqueous solution by basic oxygen furnace slag in the presence of hydrogen peroxide. Chemosphere 62:788–795. https://doi.org/10.1016/j.chemosphere.2005.04.072
Choi K, Bae S, Lee W (2014) Degradation of pyrene in cetylpyridinium chloride-aided soil washing wastewater by pyrite Fenton reaction. Chem Eng J 249:34–41. https://doi.org/10.1016/j.cej.2014.03.090
Dercová K, Vrana B, Tandlich R, Šubová L (1999) Fenton’s type reaction and chemical pretreatment of PCBs. Chemosphere 39:2621–2628. https://doi.org/10.1016/S0045-6535(99)00174-5
Flotron V, Delteil C, Padellec Y, Camel V (2005) Removal of sorbed polycyclic aromatic hydrocarbons from soil, sludge and sediment samples using the Fenton’s reagent process. Chemosphere 59:1427–1437. https://doi.org/10.1016/j.chemosphere.2004.12.065
Gan S, Lau EV, Ng HK (2009) Remediation of soils contaminated with polycyclic aromatic hydrocarbons (PAHs). J Hazard Mater 172:532–549. https://doi.org/10.1016/j.jhazmat.2009.07.118
Gocht T, Ligouis B, Hinderer M, Grathwohl P (2007) Accumulation of polycyclic aromatic hydrocarbons in rural soils based on mass balances at the catchment scale. Environ Toxicol Chem 26:591–600. https://doi.org/10.1897/06-287R.1
Gonzalez-Olmos R, Holzer F, Kopinke FD, Georgi A (2011) Indications of the reactive species in a heterogeneous Fenton-like reaction using Fe-containing zeolites. Appl Catal A-Gen 398:44–53. https://doi.org/10.1016/j.apcata.2011.03.005
Gozzi F, Machulek A, Ferreira VS, Osugi ME, Santos APF, Nogueira JA, Dantas RF, Esplugas S, de Oliveira SC (2012) Investigation of chlorimuron-ethyl degradation by Fenton, photo-Fenton and ozonation processes. Chem Eng J 210:444–450. https://doi.org/10.1016/j.cej.2012.09.008
Gu X, Yu B, Dong Q, Deng Y (2018) Application of secondary steel slag in subgrade: performance evaluation and enhancement. J Clean Prod 181:102–108. https://doi.org/10.1016/j.jclepro.2018.01.172
He J, Yang X, Men B, Wang D (2016) Interfacial mechanisms of heterogeneous Fenton reactions catalyzed by iron-based materials: a review. J Environ Sci 39:97–109. https://doi.org/10.1016/j.jes.2015.12.003
He H, Tam NFY, Yao A, Qiu R, Li WC, Ye Z (2017) Growth and Cd uptake by rice (Oryza sativa) in acidic and Cd-contaminated paddy soils amended with steel slag. Chemosphere 189:247–254. https://doi.org/10.1016/j.chemosphere.2017.09.069
Hu X, Liu B, Deng Y, Chen H, Luo S, Sun C, Yang P, Yang S (2011) Adsorption and heterogeneous Fenton degradation of 17α-methyltestosterone on nano Fe3O4/MWCNTs in aqueous solution. Appl Catal B-Environ 107:274–283. https://doi.org/10.1016/j.apcatb.2011.07.025
Hu J, Liu C, Guo Q, Yang J, Okoli CP, Lang Y, Zhao Z, Li S, Liu B, Song G (2017) Characteristics, source, and potential ecological risk assessment of polycyclic aromatic hydrocarbons (PAHs) in the Songhua River Basin, Northeast China. Environ Sci Pollut Res 24:17090–17102. https://doi.org/10.1007/s11356-017-9057-7
Huang C-P, Huang Y-H (2008) Comparison of catalytic decomposition of hydrogen peroxide and catalytic degradation of phenol by immobilized iron oxides. Appl Catal A-Gen 346:140–148. https://doi.org/10.1016/j.apcata.2008.05.017
Interstate Technology Regulatory Council (2005) Technical and regulatory guidance for in situ chemical oxidation of contaminated soil and groundwater, ITRC Washington, DC, USA
Karaca G, Tasdemir Y (2013) Effects of temperature and photocatalysts on removal of polycyclic aromatic hydrocarbons (PAHs) from automotive industry sludge. Polycycl Aromat Compd 33:380–395. https://doi.org/10.1080/10406638.2013.782880
Kuppusamy S, Thavamani P, Venkateswarlu K, Lee YB, Naidu R, Megharaj M (2017) Remediation approaches for polycyclic aromatic hydrocarbons (PAHs) contaminated soils: technological constraints, emerging trends and future directions. Chemosphere 168:944–968. https://doi.org/10.1016/j.chemosphere.2016.10.115
Li Y-S (1999) The use of waste basic oxygen furnace slag and hydrogen peroxide to degrade 4-chlorophenol. Waste Manag 19:495–502. https://doi.org/10.1016/S0956-053X(99)00239-1
Li X, Li P, Lin X, Gong Z, Fan S, Zheng L, Verkhozina EA (2008) Spatial distribution and sources of polycyclic aromatic hydrocarbons (PAHs) in soils from typical oil-sewage irrigation area, Northeast China. Environ Monit Assess 143:257–265. https://doi.org/10.1007/s10661-007-9974-x
Li F, Guo S, Wu B, Ye H (2011) Concentrations and sources of polycyclic aromatic hydrocarbons in topsoil of Benxi City, Northeast China. Chin Geogr Sci 21:185–194. https://doi.org/10.1007/s11769-011-0457-1
Li F, Guo S, Hartog N (2012) Electrokinetics-enhanced biodegradation of heavy polycyclic aromatic hydrocarbons in soil around iron and steel industries. Electrochim Acta 85:228–234. https://doi.org/10.1016/j.electacta.2012.08.055
Makela M, Watkins G, Poykio R, Nurmesniemi H, Dahl O (2012) Utilization of steel, pulp and paper industry solid residues in forest soil amendment: relevant physicochemical properties and heavy metal availability. J Hazard Mater 207-208:21–27. https://doi.org/10.1016/j.jhazmat.2011.02.015
McKeague JA, Day JH (1966) Dithionite and oxalate extractable Fe and Al as acids in different various classes of soils. Can J Soil Sci 46:13–22. https://doi.org/10.4141/cjss66-003
Mecozzi R, Di Palma L, Merli C (2006) Experimental in situ chemical peroxidation of atrazine in contaminated soil. Chemosphere 62:1481–1489. https://doi.org/10.1016/j.chemosphere.2005.06.011
Mehra OP, Jackson ML (1958) Iron oxides removed from soils and clays by a dithionite-citrate system buffered with sodium bicarbonate. In: Ingerson E (Hrsg.), Proceedings of the Seventh National Conference on Clays and Clay Minerals. Pergamon, Washington, D.C., USA, pp. 317–327
Ministry of Ecology and Environment of the People’s Republic of China (2018a) Soil environmental quality - risk control standard for soil contamination of agricultural land (GB15618–2018), Ministry of Ecology and Environment of the People's republic of China, Beijing
Ministry of Ecology and Environment of the People’s Republic of China (2018b) Soil environmental quality—risk control standard for soil contamination of development land (GB36600–2018), Ministry of Ecology and Environment of the People’s Republic of China, Beijing
Nadal M, Wargent JJ, Jones KC, Paul ND, Schuhmacher M, Domingo JL (2006) Influence of UV-B radiation and temperature on photodegradation of PAHs: preliminary results. J Atmos Chem 55:241–252. https://doi.org/10.1007/s10874-006-9037-7
Naiya TK, Bhattacharya AK, Das SK (2009) Clarified sludge (basic oxygen furnace sludge)--an adsorbent for removal of Pb(II) from aqueous solutions--kinetics, thermodynamics and desorption studies. J Hazard Mater 170:252–262. https://doi.org/10.1016/j.jhazmat.2009.04.103
Nam K, Rodriguez W, Kukor JJ (2001) Enhanced degradation of polycyclic aromatic hydrocarbons by biodegradation combined with a modified Fenton reaction. Chemosphere 45:11–20. https://doi.org/10.1016/S0045-6535(01)00051-0
Nie Y, Zhang L, Li YY, Hu C (2015) Enhanced Fenton-like degradation of refractory organic compounds by surface complex formation of LaFeO3 and H2O2. J Hazard Mater 294:195–200. https://doi.org/10.1016/j.jhazmat.2015.03.065
Proctor DM, Fehling KA, Shay EC, Wittenborn JL, Green JJ, Avent C, Bigham RD, Connolly M, Lee B, Shepker TO, Zak MA (2000) Physical and chemical characteristics of blast furnace, basic oxygen furnace, and electric arc furnace steel industry slags. Environ Sci Technol 34:1576–1582. https://doi.org/10.1021/es9906002
Qiu H, Gu H-H, He E-K, Wang S-Z, Qiu R-L (2012) Attenuation of metal bioavailability in acidic multi-metal contaminated soil treated with fly ash and steel slag. Pedosphere 22:544–553. https://doi.org/10.1016/s1002-0160(12)60039-3
Quiroga JM, Riaza A, Manzano MA (2009) Chemical degradation of PCB in the contaminated soils slurry: direct Fenton oxidation and desorption combined with the photo-Fenton process. J Environ Sci Heal A 44:1120–1126. https://doi.org/10.1080/10934520903005145
Reijonen I, Hartikainen H (2018) Risk assessment of the utilization of basic oxygen furnace slag (BOFS) as soil liming material: oxidation risk and the chemical bioavailability of chromium species. Environ Technol Innov 11:358–370. https://doi.org/10.1016/j.eti.2018.05.004
Sahl J, Munakata-Marr J (2006) The effects of in situ chemical oxidation on microbiological processes: a review. Remediation 16:57–70. https://doi.org/10.1002/rem.20091
Sanchez-Hachair A, Hofmann A (2018) Hexavalent chromium quantification in solution: comparing direct UV–visible spectrometry with 1,5-diphenylcarbazide colorimetry. CR Chim 21:890–896. https://doi.org/10.1016/j.crci.2018.05.002
Sellers RM (1980) Spectrophotometric determination of hydrogen peroxide using potassium titanium (IV) oxalate. Analyst 105:950–954. https://doi.org/10.1039/AN9800500950
Sirguey C, de Souza e Silva PT, Schwartz C, Simonnot MO (2008) Impact of chemical oxidation on soil quality. Chemosphere 72:282–289. https://doi.org/10.1016/j.chemosphere.2008.01.027
Sun J, Pan L, Tsang DCW, Zhan Y, Zhu L, Li X (2018) Organic contamination and remediation in the agricultural soils of China: a critical review. Sci Total Environ 615:724–740. https://doi.org/10.1016/j.scitotenv.2017.09.271
Szpyrkowicz L, Juzzolino C, Kaul SN (2001) A comparative study on oxidation of disperse dyes by electrochemical process, ozone, hypochlorite and Fenton reagent. Water Res 35:2129–2136. https://doi.org/10.1016/S0043-1354(00)00487-5
Tsai TT, Kao CM (2009) Treatment of petroleum-hydrocarbon contaminated soils using hydrogen peroxide oxidation catalyzed by waste basic oxygen furnace slag. J Hazard Mater 170:466–472. https://doi.org/10.1016/j.jhazmat.2009.04.073
Tsakiridis PE, Papadimitriou GD, Tsivilis S, Koroneos C (2008) Utilization of steel slag for Portland cement clinker production. J Hazard Mater 152:805–811. https://doi.org/10.1016/j.jhazmat.2007.07.093
Usman M, Faure P, Ruby C, Hanna K (2012) Remediation of PAH-contaminated soils by magnetite catalyzed Fenton-like oxidation. Appl Catal B-Environ 117-118:10–17. https://doi.org/10.1016/j.apcatb.2012.01.007
Usman M, Hanna K, Haderlein S (2016) Fenton oxidation to remediate PAHs in contaminated soils: a critical review of major limitations and counter-strategies. Sci Total Environ 569-570:179–190. https://doi.org/10.1016/j.scitotenv.2016.06.135
Wang X, Cai Q-S (2006) Steel slag as an iron fertilizer for corn growth and soil improvement in a pot experiment. Pedosphere 16:519–524. https://doi.org/10.1016/s1002-0160(06)60083-0
Wang J, Zhang X, Ling W, Liu R, Liu J, Kang F, Gao Y (2017) Contamination and health risk assessment of PAHs in soils and crops in industrial areas of the Yangtze River Delta region, China. Chemosphere 168:976–987. https://doi.org/10.1016/j.chemosphere.2016.10.113
Watts RJ, Stanton PC, Howsawkeng J, Teel AL (2002) Mineralization of a sorbed polycyclic aromatic hydrocarbon in two soils using catalyzed hydrogen peroxide. Water Res 36:4283–4292. https://doi.org/10.1016/S0043-1354(02)00142-2
Xu P, Zeng GM, Huang DL, Feng CL, Hu S, Zhao MH, Lai C, Wei Z, Huang C, Xie GX, Liu ZF (2012) Use of iron oxide nanomaterials in wastewater treatment: a review. Sci Total Environ 424:1–10. https://doi.org/10.1016/j.scitotenv.2012.02.023
Xue Y, Hou H, Zhu S (2009) Competitive adsorption of copper(II), cadmium(II), lead(II) and zinc(II) onto basic oxygen furnace slag. J Hazard Mater 162:391–401. https://doi.org/10.1016/j.jhazmat.2008.05.072
Xue Y, Wu S, Zhou M (2013) Adsorption characterization of Cu(II) from aqueous solution onto basic oxygen furnace slag. Chem Eng J 231:355–364. https://doi.org/10.1016/j.cej.2013.07.045
Yan J, Moreno L, Neretnieks I (2000) The long-term acid neutralizing capacity of steel slag. Waste Manag 20:217–223. https://doi.org/10.1016/S0956-053X(99)00318-9
Yap CL, Gan S, Ng HK (2011) Fenton based remediation of polycyclic aromatic hydrocarbons-contaminated soils. Chemosphere 83:1414–1430. https://doi.org/10.1016/j.chemosphere.2011.01.026
Yi H, Xu G, Cheng H, Wang J, Wan Y, Chen H (2012) An overview of utilization of steel slag. Procedia Environ Sci 16:791–801. https://doi.org/10.1016/j.proenv.2012.10.108
Zhang P, Chen Y (2017) Polycyclic aromatic hydrocarbons contamination in surface soil of China: a review. Sci Total Environ 605-606:1011–1020. https://doi.org/10.1016/j.scitotenv.2017.06.247
Zhang L, Xu C, Chen Z, Li X, Li P (2010) Photodegradation of pyrene on soil surfaces under UV light irradiation. J Hazard Mater 173:168–172. https://doi.org/10.1016/j.jhazmat.2009.08.059
Zhuo L, Li H, Cheng F, Shi Y, Zhang Q, Shi W (2011) Co-remediation of cadmium-polluted soil using stainless steel slag and ammonium humate. Environ Sci Pollut Res 19:2842–2848. https://doi.org/10.1007/s11356-012-0790-7
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This work was supported by the Fundamental Research Funds for the Central Universities (N172504021), the Science and Technology Planning Project of Guangdong Province (2017B030314092), and the Natural Science Foundation of Liaoning Province (201602250).
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Hu, E., He, Z., Nan, X. et al. Removal of phenanthrene and pyrene from contaminated sandy soil using hydrogen peroxide oxidation catalyzed by basic oxygen furnace slag. Environ Sci Pollut Res 26, 9281–9292 (2019). https://doi.org/10.1007/s11356-019-04308-w
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DOI: https://doi.org/10.1007/s11356-019-04308-w