Abstract
Highly efficient dewatering is essential to the reduction and reclamation disposal of oily sludge, which is a waste from the extraction, transportation, and refining of crude oil. How to effectively break the water/oil emulsion is a paramount challenge for dewatering of oily sludge. In this work, a Fenton oxidation approach was adopted for the dewatering of oily sludge. The results show that the oxidizing free radicals originated from Fenton agent effectively tailored the native petroleum hydrocarbon compounds into smaller organic molecules, hence destructing the colloidal structure of oily sludge and decreasing the viscosity as well. Meanwhile, the zeta potential of oily sludge was increased, implying the decrease of repulsive electrostatic force to realize easy coalescence of water droplets. Thus, the steric and electrostatic barriers which restrained the coalescence of dispersed water droplets in water/oil emulsion were removed. With these advantages, the Fenton oxidation approach derived the significant decrease of water content, in which 0.294 kg water was removed from per kilogram oily sludge under the optimal operation condition (i.e., pH value of 3, solid–liquid ratio of 1:10, Fe2+ concentration of 0.4 g/L and H2O2/Fe2+ ratio of 10:1, and reaction temperature of 50 °C). In addition, the quality of oil phase was upgraded after Fenton oxidation treatment accompanying with the degradation of native organic substances in oily sludge, and the heating value of oily sludge was increased from 8680 to 9260 kJ·kg−1, which would facilitate to the subsequent thermal conversion like pyrolysis or incineration. Such results demonstrate that the Fenton oxidation approach is efficient for the dewatering as well as the upgrading of oily sludge.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
Data availability
Not applicable.
References
Abdulredha MM, Hussain SA, Abdullah LC (2020) Overview on petroleum emulsions, formation, influence and demulsification treatment techniques. Arabian J Chem 13:3403–3428. https://doi.org/10.1016/j.arabjc.2018.11.014
Babaei AA, Kakavandi B, Rafiee M, Kalantarhormizi F, Purkaram I, Ahmadi E, Esmaeili S (2017) Comparative treatment of textile wastewater by adsorption, Fenton, UV-Fenton and US-Fenton using magnetic nanoparticles-functionalized carbon (MNPs@C). J Ind Eng Chem 56:163–174. https://doi.org/10.1016/j.jiec.2017.07.009
Babuponnusami A, Muthukumar K (2014) A review on Fenton and improvements to the Fenton process for wastewater treatment. J Environ Chem Eng 2:557–572. https://doi.org/10.1016/j.jece.2013.10.011
Binner ER, Robinson JP, Silvester SA, Kingman SW, Lester EH (2014) Investigation into the mechanisms by which microwave heating enhances separation of water-in-oil emulsions. Fuel 116:516–521. https://doi.org/10.1016/j.fuel.2013.08.042
Cao B, Zhang T, Zhang W, Wang D (2021) Enhanced technology based for sewage sludge deep dewatering: a critical review. Water Res 189:116650. https://doi.org/10.1016/j.watres.2020.116650
Cheng S, Wang Y, Gao N, Takahashi F, Li A, Yoshikawa K (2016) Pyrolysis of oil sludge with oil sludge ash additive employing a stirred tank reactor. J Anal Appl Pyrolysis 120:511–520. https://doi.org/10.1016/j.jaap.2016.06.024
de Araujo JL, da Silva JS, Santos FAS, de Carvalho CM, Duarte JLS, Tonholo J, Zanta C (2022) Decontamination of real urban sewage-comparison between Fenton and electrochemical oxidation. Environ Sci Pollut Res Int 29:35061–35072. https://doi.org/10.1007/s11356-022-18718-w
Ding N, Peng C, Ren Y, Liu Y, Wang P, Dong L, Liu H, Wang D (2018) Improving the dew-aterability of citric acid wastewater sludge by Fenton treatment. J Cleaner Prod 196:739–746. https://doi.org/10.1016/j.jclepro.2018.06.139
Ealias AM, Jose JV, Saravanakumar MP (2016) Biosynthesised magnetic iron nanoparticles for sludge dewatering via Fenton process. Environ Sci Pollut Res Int 23:21416–21430. https://doi.org/10.1007/s11356-016-7351-4
Elektorowicz M, Habibi S, Chifrina R (2006) Effect of electrical potential on the electro-demulsification of oily sludge. J Colloid Interface Sci 295:535–541. https://doi.org/10.1016/j.jcis.2005.08.042
Frelichowska J, Bolzinger MA, Chevalier Y (2010) Effects of solid particle content on properti-es of o/w Pickering emulsions. J Colloid Interface Sci 351:348–356. https://doi.org/10.1016/j.jcis.2010.08.019
Gonzalez A, van Lier JB, de Kreuk MK (2022) Effects of mild thermal pre-treatment combined with H2O2 addition on waste activated sludge digestibility. Waste Manage 141:163–172. https://doi.org/10.1016/j.wasman.2022.01.017
Grimme S, Antony J, Ehrlich S, Krieg H (2010) A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J Chem Phys 132:154104. https://doi.org/10.1063/1.3382344
Gu L, Nie J-Y, Zhu N-w, Wang L, Yuan H-P, Shou Z (2012) Enhanced Fenton’s degradation of real naphthalene dye intermediate wastewater containing 6-nitro-1-diazo-2-naphthol-4-sulfonic acid: a pilot scale study. Chem Eng J 189–190:108–116. https://doi.org/10.1016/j.cej.2012.02.038
Guo H, Feng S, Jiang J, Zhang M, Lin H, Zhou X (2014) Application of Fenton’s reagent combined with sawdust on the dewaterability of oily sludge. Environ Sci Pollut Res 21:10706–10712. https://doi.org/10.1007/s11356-014-3070-x
Guo T, Jiang L, Wang K, Li Y, Huang H, Wua X, Zhang G (2021) Efficient persulfate activation by hematite nanocrystals for degradation of organic pollutants under visible light irradiation: facet-dependent catalytic performance and degradation mechanism. Appl Catal B Environ 286:119883. https://doi.org/10.1016/j.apcatb.2021.119883
Hassanzadeh M, Tayebi L, Dezfouli H (2018) Investigation of factors affecting on viscosity reduction of sludge from Iranian crude oil storage tanks. Pet Sci 15:634–643. https://doi.org/10.1007/s12182-018-0247-9
He R, Tian BH, Zhang QQ, Zhang HT (2015) Effect of Fenton oxidation on biodegradability, biotoxicity and dissolved organic matter distribution of concentrated landfill leachate derived from a membrane process. Waste Manag 38:232–239. https://doi.org/10.1016/j.wasman.2015.01.006
He X, Liang C, Liu Q, Xu Z (2019) Magnetically responsive Janus nanoparticles synthesized using cellulosic materials for enhanced phase separation in oily wastewaters and water-in-crude oil emulsions. Chem Eng J 378:122045. https://doi.org/10.1016/j.cej.2019.122045
Hu G, Li J, Zeng G (2013) Recent development in the treatment of oily sludge from petroleum industry: a review. J Hazard Mater 261:470–490. https://doi.org/10.1016/j.jhazmat.2013.07.069
Jerez S, Ventura M, Molina R, Pariente MI, Martínez F, Melero JA (2021) Comprehensive characterization of an oily sludge from a petrol refinery: a step forward for its valorization within the circular economy strategy. J Environ Manag 285:112124. https://doi.org/10.1016/j.jenvman.2021.112124
Jerez S, Ventura M, Molina R, Martinez F, Pariente MI, Melero JA (2022) Application of a Fenton process for the pretreatment of an iron-containing oily sludge: a sustainable management for refinery wastes. J Environ Manag 304:114244. https://doi.org/10.1016/j.jenvman.2021.114244
Jiang T, Hirasaki GJ, Miller CA, Moran K (2008) Using silicate and pH control for removal of the rag layer containing clay solids formed during demulsification. Energy Fuels 22:4158–4164
Jiang Z, Wang L, Lei J, Liu Y, Zhang J (2019) Photo-Fenton degradation of phenol by CdS/rGO/Fe2+ at natural pH with in situ-generated H2O2. Appl Catal B Environ 241:367–374. https://doi.org/10.1016/j.apcatb.2018.09.049
Kakavandi B, Jonidi Jafari A, Rezaei Kalantary R, Nasseri S, Esrafili A, Gholizadeh A, Azari A (2016) Simultaneous adsorption of lead and aniline onto magnetically recoverable carb-on: optimization, modeling and mechanism. J Chem Technol Biotechnol 91:3000–3010. https://doi.org/10.1002/jctb.4925
Katepalli H, John VT, Tripathi A, Bose A (2017) Microstructure and rheology of particle stabilized emulsions: effects of particle shape and inter-particle interactions. J Colloid Interface Sci 485:11–17. https://doi.org/10.1016/j.jcis.2016.09.015
Khan MK, Cahyadi HS, Kim S-M, Kim J (2019) Efficient oil recovery from highly stable toxic oily sludge using supercritical water. Fuel 235:460–472. https://doi.org/10.1016/j.fuel.2018.08.003
Kumar K, Nikolov AD, Wasan DT (2001) Mechanisms of stabilization of water-in-crude oil emulsions. Ind Eng Chem Res 40:3009–3014
Li J, Ai Z, Zhang L (2009) Design of a neutral electro-Fenton system with Fe@Fe2O3/ACF co-mposite cathode for wastewater treatment. J Hazard Mater 164:18–25. https://doi.org/10.1016/j.jhazmat.2008.07.109
Liao Y, Zheng H, Qian L, Sun Y, Dai L, Xue W (2014) UV-initiated polymerization of hydrophobically associating cationic polyacrylamide modified by a surface-active monomer: a comparative study of synthesis, characterization, and sludge dewatering performance. Ind Eng Chem Res 53:11193–11203. https://doi.org/10.1021/ie5016987
Liu XM, Sheng GP, Luo HW, Zhang F, Yuan SJ, Xu J, Zeng RJ, Wu JG, Yu HQ (2010) Contribution of extracellular polymeric substances (EPS) to the sludge aggregation. Environ Sci Technol 44:4355–4360
Liu H, Yang J, Zhu N, Zhang H, Li Y, He S, Yang C, Yao H (2013) A comprehensive insight into the combined effects of Fenton’s reagent and skeleton builders on sludge deep dewatering performance. J Hazard Mater 258–259:144–150. https://doi.org/10.1016/j.jhazmat.2013.04.036
Liu N, Xie H, Wei J, Li Y, Wang J, Yu N, Zhao N, Zhang L, Chen Z (2019) Catalytic activity of a composite metal electrode catalyst for the degradation of real dyeing wastewater by a heterogeneous electro-Fenton process. J Environ Chem Eng 7:102930. https://doi.org/10.1016/j.jece.2019.102930
Liu B, Teng Y, Song W, Wu H (2022a) Novel conditioner for efficient dewaterability and mod-ification of oily sludge with high water content. Environ Sci Pollut Res Int 29:25417–25427. https://doi.org/10.1007/s11356-021-17150-w
Liu Y, Jiang Z, Fu J, Ao W, Ali Siyal A, Zhou C, Liu C, Dai J, Yu M, Zhang Y, Jin Y, Yuan Y, Zhang C (2022) Iron-biochar production from oily sludge pyrolysis and its application for organic dyes removal. Chemosphere 301:134803. https://doi.org/10.1016/j.chemosphere.2022.134803
Lu Y, Zheng G, Wu W, Cui C, Zhou L (2017) Significances of deflocculated sludge flocs as well as extracellular polymeric substances in influencing the compression dewatering of chemically acidified sludge. Sep Purif Technol 176:243–251. https://doi.org/10.1016/j.seppur.2016.12.016
Lu Y, Wu H, Meng Z, Jiang J, Jin Y, Deng Z, Su W, Li Z, Kang W (2018) Salt effect on hydrophobically modified polyacrylamide-containing crude oil emulsions: stability and rheology study. Colloid Polym Sci 296:515–527. https://doi.org/10.1007/s00396-018-4267-1
Luo XM, Gong HY, He ZL, Zhang P, He LM (2020) Research on mechanism and characteristics of oil recovery from oily sludge in ultrasonic fields. J Hazard Mater 399:123137. https://doi.org/10.1016/j.jhazmat.2020.123137
Lv X, Song Z, Yu J, Su Y, Zhao X, Sun J, Mao Y, Wang W (2020) Study on the demulsific-ation of refinery oily sludge enhanced by microwave irradiation. Fuel 279:118417. https://doi.org/10.1016/j.fuel.2020.118417
Martínez F, Molina R, Rodríguez I, Pariente MI, Segura Y, Melero JA (2018) Techno-economical assessment of coupling Fenton/biological processes for the treatment of a pharmaceutical wastewater. J Environ Chem Eng 6:485–494. https://doi.org/10.1016/j.jece.2017.12.008
Mohammadian E, Taju Ariffin TS, Azdarpour A, Hamidi H, Yusof S, Sabet M, Yahya E (2018) Demulsification of light malaysian crude oil emulsions using an electric field method. Ind Eng Chem Res 57:13247–13256. https://doi.org/10.1021/acs.iecr.8b02216
Murungi PI, Sulaimon AA (2022) Petroleum sludge treatment and disposal techniques: a review. Environ Sci Pollut Res Int 29:40358–40372. https://doi.org/10.1007/s11356-022-19614-z
Neyens E, Baeyens J (2003) A review of thermal sludge pre-treatment processes to improve dewaterability. J Hazard Mater 98:51–67. https://doi.org/10.1016/s0304-3894(02)00320-5
Pensini E, Harbottle D, Yang F, Tchoukov P, Li Z, Kailey I, Behles J, Masliyah J, Xu Z (2014) Demulsification mechanism of asphaltene-stabilized water-in-oil emulsions by a polymeric ethylene oxide–propylene oxide demulsifier. Energy Fuels 28:6760–6771. https://doi.org/10.1021/ef501387k
Qin JH, Lin CX, Almebayedh H, Albader M (2019) Decomposition of long-chain petroleum hydrocarbons by Fenton-like processes: effects of ferrous iron source, salinity and temperature. Ecotoxicol Environ Saf 169:764–769. https://doi.org/10.1016/j.ecoenv.2018.11.086
Rashid TU, Fijul Kabir SM, Biswas MC, Rahman Bhuiyan MA (2020) Sustainable wastewater treatment via dye–surfactant interaction: a critical review. Ind Eng Chem Res 59:9719–9745
Romero V, Acevedo S, Marco P, Gimenez J, Esplugas S (2016) Enhancement of Fenton and photo-Fenton processes at initial circumneutral pH for the degradation of the beta-blocker metoprolol. Water Res 88:449–457. https://doi.org/10.1016/j.watres.2015.10.035
Shi P, Gou Y, Li J, Zheng Q, Zhong X, Duan M, Pu W (2022) Recycling of crude oil from oily wastewater via a novel hydrogel coalescer. Fuel 313:123040. https://doi.org/10.1016/j.fuel.2021.123040
Singh SK, Tang WZ (2013) Statistical analysis of optimum Fenton oxidation conditions for landfill leachate treatment. Waste Manag 33:81–88. https://doi.org/10.1016/j.wasman.2012.08.005
Su CC, Chang AT, Bellotindos LM, Lu MC (2012) Degradation of acetaminophen by Fenton a-nd electro-Fenton processes in aerator reactor. Sep Purif Technol 99:8–13. https://doi.org/10.1016/j.seppur.2012.07.004
Teng Q, Zhang D, Yang C (2021) A review of the application of different treatment processes for oily sludge. Environ Sci Pollut Res Int 28:121–132. https://doi.org/10.1007/s11356-020-11176-2
Varjani S, Joshi R, Srivastava VK, Ngo HH, Guo W (2020) Treatment of wastewater from petroleum industry: current practices and perspectives. Environ Sci Pollut Res Int 27:27172–27180. https://doi.org/10.1007/s11356-019-04725-x
Wang Z, Xie L, Liu K, Wang J, Zhu H, Song Q, Shu X (2019) Co-pyrolysis of sewage sludge and cotton stalks. Waste Manag 89:430–438. https://doi.org/10.1016/j.wasman.2019.04.033
Wang D, Yang D, Huang C, Huang Y, Yang D, Zhang H, Liu Q, Tang T, Gamal El-Din M, Kemppi T, Perdicakis B, Zeng H (2021a) Stabilization mechanism and chemical demulsification of water-in-oil and oil-in-water emulsions in petroleum industry: a review. Fuel 286:119390. https://doi.org/10.1016/j.fuel.2020.119390
Wang Z, Jiang L, Wang K, Li Y, Zhang G (2021b) Novel AgI/BiSbO4 heterojunction for efficient photocatalytic degradation of organic pollutants under visible light: interfacial electron transfer pathway, DFT calculation and degradation mechanism study. J Hazard Mater 410:124948. https://doi.org/10.1016/j.jhazmat.2020.124948
Wang Z, Wang Z, Sun Z, Ma K, Du L, Yuan R (2022) Evolution of S/N containing compounds in pyrolysis of highly oily petroleum sludge. Fuel 318:123687. https://doi.org/10.1016/j.fuel.2022.123687
Xiao C, Li X, Li Q, Hu Y, Cheng J, Chen Y (2022) Ni-doped FeC2O4 for efficient photo-Fenton simultaneous degradation of organic pollutants and reduction of Cr(VI): accelerated Fe(III)/Fe(II) cycle, enhanced stability and mechanism insight. J Cleaner Prod 340:130775. https://doi.org/10.1016/j.jclepro.2022.130775
Xu XR, Li XY, Li XZ, Li HB (2009) Degradation of melatonin by UV, UV/H2O2, Fe2+/H2O2 and UV/Fe2+/H2O2 processes. Sep Purif Technol 68:261–266. https://doi.org/10.1016/j.seppur.2009.05.013
Xu H, Jia W, Ren S, Wang J (2018) Novel and recyclable demulsifier of expanded perlite grafted by magnetic nanoparticles for oil separation from emulsified oil wastewaters. Chem Eng J 337:10–18. https://doi.org/10.1016/j.cej.2017.12.084
Yang Z, Wang Z, Wang J, Li Y, Zhang G (2022) Facet-dependent activation of oxalic acid over magnetic recyclable Fe3S4 for efficient pollutant removal under visible light irradiation: enhanced catalytic activity, DFT calculations, and mechanism insight. Environ Sci Technol 56:18008–18017. https://doi.org/10.1021/acs.est.2c06571
Zhang H, Choi HJ, Huang CP (2005) Optimization of Fenton process for the treatment of landfill leachate. J Hazard Mater 125:166–174. https://doi.org/10.1016/j.jhazmat.2005.05.025
Zhang G, Gao Y, Zhang Y, Guo Y (2010) Fe2O3-pillared rectorite as an efficient and stable fenton-like heterogeneous catalyst for photodegradation of organic contaminants. Environ Sci Technol 44:6384–6389
Zhang J, Li J, Thring RW, Hu X, Song X (2012) Oil recovery from refinery oily sludge via ultrasound and freeze/thaw. J Hazard Mater 203–204:195–203. https://doi.org/10.1016/j.jhazmat.2011.12.016
Zhang L, Zhang B, Wu T, Sun D, Li Y (2015) Adsorption behavior and mechanism of chloro-phenols onto organoclays in aqueous solution. Colloids Surf A 484:118–129. https://doi.org/10.1016/j.colsurfa.2015.07.055
Zheng X, Ying Z, Cui J, Wang B, Chen J, Zhang Q (2017) Simultaneous dewatering and rec-overing oil from high-viscosity oily sludge through the combination process of demul-sification, viscosity reduction, and centrifugation. Energy Fuels 31:14401–14407. https://doi.org/10.1021/acs.energyfuels.7b02481
Zhou L, Jiang X, Liu J (2009) Characteristics of oily sludge combustion in circulating fluidized beds. J Hazard Mater 170:175–179. https://doi.org/10.1016/j.jhazmat.2009.04.109
Funding
This work was supported by the National Natural Science Foundation of China (52276145, 52276144, 51906260), the Natural Science Foundation of Hunan Province, China (2021JJ30851, 2022JJ20072, 2022JJ40575), and the Science and Technology Innovation Program of Hunan Province (2021RC4005).
Author information
Authors and Affiliations
Contributions
Jianping Yang: writing—review and editing, supervision, funding acquisition.
Xiaolei Zhu: methodology, investigation, writing—original draft.
Zejian Ai: formal analysis, data curation, validation.
Lijian Leng: visualization, data curation.
Hailong Li: methodology, resources, writing—review and editing, funding acquisition.
Corresponding author
Ethics declarations
Ethical approval
I have not submitted my manuscript to a preprint server and other journals before submitting it to Environmental Science and Pollution Research.
Consent to participate
All authors have read and approved the final manuscript.
Consent for publication
All authors agree to publish if the paper is accepted.
Competing interests
The authors declare no competing interests.
Additional information
Responsible Editor: Ricardo A. Torres-Palma
Publisher's note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Yang, J., Zhu, X., Ai, Z. et al. Deep dewatering of refinery oily sludge by Fenton oxidation and its potential influence on the upgrading of oil phase. Environ Sci Pollut Res 30, 76617–76630 (2023). https://doi.org/10.1007/s11356-023-27773-w
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-023-27773-w