Abstract
A large number of stable oil-in-water (O/W) emulsions are generated by the petroleum industry each year, resulting in a series of operational and environmental challenges. In this study, a RH-NH2 demulsifier was prepared for the separation of O/W emulsions by grafting ethylenediamine onto natural rice husk. RH-NH2 was characterized using Fourier transform infrared spectroscopy (FT-IR) and scanning electron microscopy (SEM). When the dosage of RH-NH2 was 50 mg/L, the light transmittance (WT) and corresponding oil removal efficiency (WR) of the separated water were 90.2 ± 1.8% and 94.82 ± 0.95%, respectively, in the emulsion-0.2 (containing 0.2% crude oil). When the dosage was 200 mg/L, the WT and WR values of the emulsion-1 (with 1% crude oil) were 91.9 ± 0.9% and 99.14 ± 0.1%, respectively. In addition, dynamic interfacial tension (IFT), wettability, zeta potential, interfacial activity and adsorption capability of RH-NH2 at the interface were also investigated. The results showed that the IFT values of asphaltene and RH-NH2 (200 mg/L) was 22.58 mN/m and 16.42 mN/m, respectively. The zeta potential of the O/W emulsion was − 37 ± 1.8 mV while that of RH-NH2 was 20.8 ± 1.0 mV, which facilitated the electrostatic neutralization and reduced the electrostatic repulsion between oil droplets. A possible demulsification mechanism was proposed, which indicated that RH-NH2 was amphiphilic, with high interfacial activity and stronger capability to reduce IFT. It migrated rapidly to the oil–water interface and disrupted the interfacial film via synergistic effect of the π-π/n-π interaction, leading to demulsification. RH-NH2 has a potential industrial application due to its low-cost and high demulsification efficiency.
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References
Adewunmi AA, Kamal MS, Solling TI (2021) Application of magnetic nanoparticles in demulsification: a review on synthesis, performance, recyclability, and challenges. J Pet Sci Eng 196:107680–107688. https://doi.org/10.1016/j.petrol.2020.107680
Agah M, Binazadeh M, Baghulifard N, Sarani M (2022) Demulsification of saline-in-crude oil via biocompatible cellulose derivative polymers. Fuel 311:122533–112544. https://doi.org/10.1016/j.fuel.2021.122533
Alver E, Metin AU, Brouers F (2020) Methylene blue adsorption on magnetic alginate/rice husk bio-composite. Int J Biol Macromol 154:104–113. https://doi.org/10.1016/j.ijbiomac.2020.02.330
Cai Q, Zhu Z, Chen B, Zhang B (2019) Oil-in-water emulsion breaking marine bacteria for demulsifying oily wastewater. Water Res 149:292–301. https://doi.org/10.1016/j.watres.2018.11.023
Fang S, Chen T, Wang R, **ong Y, Chen B, Duan M (2016) Assembly of graphene oxide at the crude oil/water interface: a new approach to efficient demulsification. Energy Fuels 30:3355–3364. https://doi.org/10.1021/acs.energyfuels.6b00195
Feng L, Gao Y, Dai Z, Dan H, **ao F, Yue Q, Gao B, Wang S (2021a) Preparation of a rice straw-based green separation layer for efficient and persistent oil-in-water emulsion separation. J Hazard Mater 415:125594–125607. https://doi.org/10.1016/j.jhazmat.2021.125594
Feng X, Jiang S, Li B, Yang Y, Shen L, Zhang Z, Yuan H, Ye F, Mi Y (2021b) Synthesis of a hyperbranched polymer with a dihydroxyl nucleus and its demulsifying performance. Chem Eng Res Des 174:267–275. https://doi.org/10.1016/j.cherd.2021.08.014
Gurav R, Bhatia SK, Choi TR, Choi YK, Kim HJ, Song HS, Park SL, Lee HS, Lee SM, Choi KY, Yang YH (2021) Adsorptive removal of crude petroleum oil from water using floating pinewood biochar decorated with coconut oil-derived fatty acids. Sci Total Environ 781:146636–146644. https://doi.org/10.1016/j.scitotenv.2021.146636
Hassan SA, Abdalla BK, Mustafa MA (2019) Addition of silica nano-particles for the enhancement of crude oil demulsification process. Petrol Sci Technol 37:1603–1611. https://doi.org/10.1080/10916466.2019.1602634
He X, Liu Q, Xu Z (2021) Cellulose-coated magnetic Janus nanoparticles for dewatering of crude oil emulsions. Chem Eng Sci 230:116215–116249. https://doi.org/10.1016/j.ces.2020.116215
Hu W, Zhou W, Lei X, Zhou P, Zhang M, Chen T, Zeng H, Zhu J, Dai S, Yang S, Yang S (2019) Low-temperature in situ amino functionalization of TiO2 nanoparticles sharpens electron management achieving over 21% efficient planar perovskite solar cells. Adv Mater 31:1806095–1806102. https://doi.org/10.1002/adma.201806095
Li ZL, Chakraborty A, Fuentes J, Zamora E, Vazquez F, Xu ZH, Liu QX, Flores C, McCaffrey WC (2021) Study on demulsifier crude oil interactions at oil-water interface for crude oil dehydration. Colloids Surf A Physicochem Eng Asp 630:127526–127535. https://doi.org/10.1016/j.colsurfa.2021.127526
Lin L, Zhai SR, **ao ZY, Song Y, An QD, Song XW (2013) Dye adsorption of mesoporous activated carbons produced from NaOH-pretreated rice husks. Bioresour Technol 136:437–443. https://doi.org/10.1016/j.biortech.2013.03.048
Liu J, Huang XF, Lu LJ, Li MX, Xu JC, Deng HP (2011) Turbiscan Lab (R) Expert analysis of the biological demulsification of a water-in-oil emulsion by two biodemulsifiers. J Hazard Mater 190:214–221. https://doi.org/10.1016/j.jhazmat.2011.03.028
Liu J, Liu J, Zhong J, Shen J, Ren S (2021) Preparation of graphene oxide/attapulgite composites and their demulsification performance for oil-in-water emulsion. Energy Fuels 35:5172–5180. https://doi.org/10.1021/acs.energyfuels.1c00042
Lu J, Gao Z, Xu T, Zhu X, Miao X, Song Y, Ren G, Li X (2020a) Robust Hydrogel Coating with Oil-Repellent Property in Air, Water, and Oil Surroundings. ACS Appl Mater Interfaces 12:49138–49145. https://doi.org/10.1021/acsami.0c16410
Lu J, Zhu X, Wang B, Liu L, Song Y, Miao X, Ren G, Li X (2020b) A slippery oil-repellent hydrogel coating. Cellulose 27:2817–2827. https://doi.org/10.1007/s10570-019-02953-5
Lu J, Li F, Miao G, Miao X, Ren G, Wang B, Song Y, Li X, Zhu X (2021) Superhydrophilic/superoleophobic shell powder coating as a versatile platform for both oil/water and oil/oil separation. J Membr Sci 637:119624–119632. https://doi.org/10.1016/j.memsci.2021.119624
Luo X, Gong H, He Z, Zhang P, He L (2021) Recent advances in applications of power ultrasound for petroleum industry. Ultrason Sonochem 70:105337–105347. https://doi.org/10.1016/j.ultsonch.2020.105337
Onaizi SA (2022) Effect of salinity on the characteristics, pH-triggered demulsification and rheology of crude oil/water nanoemulsions. Sep Purif Technol 281:119956–119964. https://doi.org/10.1016/j.seppur.2021.119956
Poteau S, Argillier J-F, Langevin D, Pincet F, Perez E (2005) Influence of pH on Stability and Dynamic Properties of Asphaltenes and Other Amphiphilic Molecules at the Oil – Water Interface†. Energy Fuels 19:1337–1341. https://doi.org/10.1021/ef0497560
Ren G, Song Y, Li X, Zhou Y, Zhang Z, Zhu X (2018) A superhydrophobic copper mesh as an advanced platform for oil-water separation. Appl Surf Sci 428:520–525. https://doi.org/10.1016/j.apsusc.2017.09.140
Saruchi, Kaith BS, **dal R, Kumar V (2015) The Adsorption of Crude Oil From an Aqueous Solution Using aGum tragacanthPolyacrylic Acid Based Hydrogel. Petrol Sci Technol 33:278–286. https://doi.org/10.1080/10916466.2014.976310
Saruchi KV, Vikas P, Kumar R, Kumar B, Kaur M (2016) Low cost natural polysaccharide and vinyl monomer based IPN for the removal of crude oil from water. J Pet Sci Eng 141:1–8. https://doi.org/10.1016/j.petrol.2016.01.007
Saruchi V, Kumar V (2019) Separation of crude oil from water using chitosan based hydrogel. Cellulose 26:6229–6239. https://doi.org/10.1007/s10570-019-02539-1
Saruchi V, Kumar V, Ghfar AA, Pandey S (2022) Oil spill remediation by grafted natural polysaccharide gum tragacanth: its kinetics and isotherms studies. Biomass Convers Biorefin. https://doi.org/10.1007/s13399-022-02665-0
Shen L, Ai G, Ao Y, Zeng G, Yang Y, Feng X, Zhang Z, Yuan H, Ye F, Mi Y (2021a) Treatment of water-in-crude oil emulsion driven by SiO2 modified rice bran. Colloids Surf A Physicochem Eng Asp 631:127708–127717. https://doi.org/10.1016/j.colsurfa.2021.127708
Shen L, Hu W, Lei Z, Peng J, Zhu E, Zhang X, Yang M, Feng X, Yang Y, Mi Y (2021b) Nanoscale silica-coated graphene oxide and its demulsifying performance in water-in-oil and oil-in-water emulsions. Environ Sci Pollut Res Int 28:55454–55464. https://doi.org/10.1007/s11356-021-14888-1
Shrestha L, Thapa M, Shrestha R, Maji S, Pradhananga R, Ariga K (2019) Rice Husk-Derived High Surface Area Nanoporous Carbon Materials with Excellent Iodine and Methylene Blue Adsorption Properties. C-J Carbon Res 5:10–22. https://doi.org/10.3390/c5010010
Sun H, Wang Q, Li X, He X (2020) Novel polyether-polyquaternium copolymer as an effective reverse demulsifier for O/W emulsions: demulsification performance and mechanism. Fuel 263:116770–116776. https://doi.org/10.1016/j.fuel.2019.116770
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 (2021) Stabilization mechanism and chemical demulsification of water-in-oil and oil-in-water emulsions in petroleum industry: a review. Fuel 286:119390–119409. https://doi.org/10.1016/j.fuel.2020.119390
Wang X, Liu W, Liu X, Luo J (2020) Study on demulsification and deoiling for O/W emulsion by microbubble pretreated resin. Water Sci Technol 81:148–158. https://doi.org/10.2166/wst.2020.095
Wang Z, Elimelech M, Lin S (2016) Environmental Applications of Interfacial Materials with Special Wettability. Environ Sci Technol 50:2132–2176. https://doi.org/10.1021/acs.est.5b04351
Wu M, Mu P, Li B, Wang Q, Yang Y, Li J (2020) Pine powders-coated PVDF multifunctional membrane for highly efficient switchable oil/water emulsions separation and dyes adsorption. Sep Purif Technol 248:117028–117035. https://doi.org/10.1016/j.seppur.2020.117028
Xu H, Jia W, Ren S, Wang J (2019a) Magnetically responsive multi-wall carbon nanotubes as recyclable demulsifier for oil removal from crude oil-in-water emulsion with different pH levels. Carbon 145:229–239. https://doi.org/10.1016/j.carbon.2019.01.024
Xu H, Wang J, Ren S (2019b) Removal of oil from a crude oil-in-water emulsion by a magnetically recyclable diatomite demulsifier. Energy Fuels 33:11574–11583. https://doi.org/10.1021/acs.energyfuels.9b02440
Xu H, Wang J, Yang X, Ning L (2021) Magnetically recyclable graphene oxide demulsifier adapting wide pH conditions on detachment of oil in the crude oil-in-water emulsion. ACS Appl Mater Interfaces 13:6748–6757. https://doi.org/10.1021/acsami.0c18115
Xu Y, Wang G, Zhu L, Deng W, Wang C, Ren T, Zhu B, Zeng Z (2022) Desert beetle-like microstructures bridged by magnetic Fe3O4 grains for enhancing oil-in-water emulsion separation performance and solar-assisted recyclability of graphene oxide. Chem Eng J 427:130904–130928. https://doi.org/10.1016/j.cej.2021.130904
Yang S, Sun J, Wu K, Hu C (2021a) Enhanced oil droplet aggregation and demulsification by increasing electric field in electrocoagulation. Chemosphere 283:131123–131131. https://doi.org/10.1016/j.chemosphere.2021.131123
Yang Y, Li B, Peng J, Lei Z, Zhu E, Zhang X, Feng X, Mi Y (2021b) The demulsification of crude oil emulsion driven by a natural lotus leaf grafted with nano-SiO2. J Environ Chem Eng 9:105586–105594. https://doi.org/10.1016/j.jece.2021.105586
Yang Y, Ao Y, Shen L, Feng X, Yuan H, Zhang Z, Ye F, Mi Y (2022) Preparation of a demulsifier using rice straw as raw materials via a simple acid treatment process. Colloids Surf A Physicochem Eng Asp 636:128160–128169. https://doi.org/10.1016/j.colsurfa.2021.128160
Ye F, Jiang X, Mi Y, Kuang J, Huang Z, Yu F, Zhang Z, Yuan H (2019) Preparation of oxidized carbon black grafted with nanoscale silica and its demulsification performance in water-in-oil emulsion. Colloids Surf A Physicochem Eng Asp 582:123878–123886. https://doi.org/10.1016/j.colsurfa.2019.123878
Ye F, Wang Z, Mi Y, Kuang J, Jiang X, Huang Z, Luo Y, Shen L, Yuan H, Zhang Z (2020) Preparation of reduced graphene oxide/titanium dioxide composite materials and its application in the treatment of oily wastewater. Colloids Surf A Physicochem Eng Asp 586:124251–124261. https://doi.org/10.1016/j.colsurfa.2019.124251
Ye F, Mi Y, Liu H, Zeng G, Shen L, Feng X, Yang Y, Zhang Z, Yuan H, Yan X (2021a) Demulsification of water-in-crude oil emulsion using natural lotus leaf treated via a simple hydrothermal process. Fuel 295:120596–120602. https://doi.org/10.1016/j.fuel.2021.120596
Ye F, Wang G, Ao Y, Shen L, Yang Y, Feng X, Zhang Z, Yuan H, Mi Y, Yan X (2021) Recyclable amine-functionalized carbon nanotubes for the separation of oily wastewater. Chemosphere 288:132571–132578. https://doi.org/10.1016/j.chemosphere.2021.132571
Ye F, Zhang Z, Ao Y, Li B, Chen L, Shen L, Feng X, Yang Y, Yuan H, Mi Y (2022) Demulsification of water-in-crude oil emulsion driven by a carbonaceous demulsifier from natural rice husks. Chemosphere 288:132656–132665. https://doi.org/10.1016/j.chemosphere.2021.132656
Ying T, Su J, Jiang Y, Ke Q, Xu H (2020) A pre-wetting induced superhydrophilic/superlipophilic micro-patterned electrospun membrane with self-cleaning property for on-demand emulsified oily wastewater separation. J Hazard Mater 384:121475–121485. https://doi.org/10.1016/j.jhazmat.2019.121475
Zhang Z, Feng X, Zeng G, Liu H, Shen L, Yang Y, Yuan H, Yan X, Mi Y (2021) Hyperbranched poly(amido amine) demulsifiers using diaminonaphthalene as the central core and their demulsification performance in oil-in-water and water-in-oil emulsions. Energy Fuels 35:3095–3103. https://doi.org/10.1021/acs.energyfuels.0c03912
Zhou J, Sui H, Ma J, Li X, Al-Shiaani NHA, He L (2021) Fast demulsification of oil-water emulsions at room temperature by functionalized magnetic nanoparticles. Sep Purif Technol 274:118967–119009. https://doi.org/10.1016/j.seppur.2021.118967
Zhu T, Kang W, Yang H, Li Z, Wang T, Fan Y, Kang X, Jia R, Kenzhebek I, Issakhov M (2021) Fabrication of a pH-responsive emulsifier for heavy oil recovery based on dynamic imine bond. J Mol Liq 332:115916–115922. https://doi.org/10.1016/j.molliq.2021.115916
Zou X, Li M, **ao H, Zhou S, Chen C, Zhao Y (2021) Simulation study on real laminar assembly of g-C3N4 high performance free standing membrane with bio-based materials. Sep Purif Technol 278:119598–119607. https://doi.org/10.1016/j.seppur.2021.119598
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This study was supported by the project of joint research institute of Chuanqing drilling engineering company -Yangtze university (CQCJ-2021-08).
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LS: Conceptualization, Investigation, Methodology, Writing original draft. YM: Supervision, Writing review & editing. TL: Data curation, Writing review & editing. KH: Resource. DZ: Resource. XL: Resource. YY: Visualization, Investigation. XF: Software, Visualization. ZZ: Formal analysis, Investigation. FY: Data curation, Visualization.
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Shen, L., Liu, T., Huang, K. et al. Separation of crude oil-in-water emulsions using ethylenediamine modified rice husks. Cellulose 29, 9803–9817 (2022). https://doi.org/10.1007/s10570-022-04860-8
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DOI: https://doi.org/10.1007/s10570-022-04860-8