Study on modified graphene oxide-based emulsion cleaner for oily sludge

Shuang Zheng; Xin Li; Yang Chen; Rongjiao Zhu; Xia Feng

doi:10.1515/tsd-2023-2566

Article

Study on modified graphene oxide-based emulsion cleaner for oily sludge

Shuang Zheng
Shuang Zheng is a graduate student Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include the modification of graphene oxide and the application of its emulsion in the cleaning of oily sludge.
, Xin Li
Xin Li a student in the Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include emulsifier flooding, and flooding from medium and low permeability reservoirs.
, Yang Chen
Yang Chen is a student at the Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include the application of polyacrylamide in oil flooding, and graphene oxide flooding.
, Rongjiao Zhu
Rongjiao Zhu is an associate professor at the Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include the synthesis and application of oilfield chemicals and controllable chemical conversion and energy catalysis of nanomaterials.
and Xia Feng
Xia Feng is an associate professor at the Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include nano-self-assembled drug delivery systems, preparation and application of nano-functional materials, biocatalysis and bioconversion.

Published/Copyright: April 24, 2024

Published by

Become an author with De Gruyter Brill

Author Information

From the journal Tenside Surfactants Detergents Volume 61 Issue 4

Abstract

Oily sludge is a complex system that is inevitably generated during the process of oil extracting and processing. It will cause serious environmental pollution and waste of resources if untreated sludge is discharged. In this paper, a composite emulsion cleaner based on modified graphite oxide and surfactants was developed for cleaning oily sludge. First, graphite oxide (GO) was functionally modified with butylamine, and its structures were verified by Fourier transform infrared spectroscopy (FTIR), X-ray electron spectroscopy (XPS), thermogravimetric analysis (TGA), and environmental scanning electron microscopy (SEM). Then, the oil-in-water composite emulsion cleaner was prepared by using butylamine modified graphite oxide and surfactants. The conditions for emulsion preparation and oil sludge cleaning were modelled and optimized by the response surface methodology. The obtained optimal formulations were: surfactant content was 2.17 ‰ with SDS/AEO-3 ratio of 9:1, GO-A4 content was 0.96 ‰, water-oil ratio was 5:5, and the oil removal rate was 97.45 %. The optimal cleaning conditions were: liquid-solid ratio of 3.2:1, cleaning time of 32 min, cleaning temperature of 28.7 °C, and oil removal rate of 99.02 %. The solid sediments were characterized by FTIR and SEM, which proved the feasibility of cleaning oily sludge with the emulsion.

Keywords: chemically modified graphite oxide; detergent prepared from emulsion; oily sludge; response surface methodology (RSM)

Corresponding author: Rongjiao Zhu, Department of Chemistry, School of Science, Tianjin University, Tianjin 300072, China; and Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China, E-mail: zhurongjiao@tju.edu.cn

Funding source: Sinopec’s Key Scientific and Technological Research Project “Development of Modified Graphene Oxide Control and Displacement System”

Award Identifier / Grant number: No. 2020GKF-0657

About the authors

Shuang Zheng

Shuang Zheng is a graduate student Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include the modification of graphene oxide and the application of its emulsion in the cleaning of oily sludge.

Xin Li

Xin Li a student in the Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include emulsifier flooding, and flooding from medium and low permeability reservoirs.

Yang Chen

Yang Chen is a student at the Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include the application of polyacrylamide in oil flooding, and graphene oxide flooding.

Rongjiao Zhu

Rongjiao Zhu is an associate professor at the Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include the synthesis and application of oilfield chemicals and controllable chemical conversion and energy catalysis of nanomaterials.

Xia Feng

Xia Feng is an associate professor at the Department of Chemistry, School of Science, Tianjin University. The fields of interest in scientific research include nano-self-assembled drug delivery systems, preparation and application of nano-functional materials, biocatalysis and bioconversion.

List of abbreviations

RSM: response surface methodology
GO: graphite oxide
GO-A4: butylamine modified graphite oxide
SDS: sodium dodecyl sulfonate
AEO-3: polyoxyethylene lauryl ether
FTIR: fourier transform infrared spectroscopy
XPS: X-ray electron spectroscopy
TGA: thermogravimetric analysis
SEM: scanning electron microscopy

Acknowledgments

The authors acknowledge Tianjin University for providing laboratories and allowing researchers to use experimental instruments and equipment.

Research ethics: Not applicable.
Author contributions: The authors have accepted responsibility for the entire content of this manuscript and approved its submission.
Competing interests: The authors state no conflict of interest.
Research funding: This work was supported by Sinopec’s Key Scientific and Technological Research Project “Development of Modified Graphene Oxide Control and Displacement System” (No. 2020GKF-0657).
Data availability: The raw data can be obtained on request from the corresponding author.

References

1. Mazlova, E. A.; Meshcheryakov, S. V. Ecological Characteristics of Oil Sludges. Chem. Tech. Fuels Oils 1999, 35, 49–53. https://doi.org/10.1007/BF02694263.Search in Google Scholar

2. Liu, J. W.; Li, L.; Xu, Z. Z.; Chen, J.; Zhao, M. W.; Dai, C. L. CO2-responsive Zwitterionic Copolymer for Effective Emulsification and Facile Demulsification of Crude Heavy Oil. J. Mol. Liq. 2021, 325, 115166. https://doi.org/10.1016/j.molliq.2020.115166.Search in Google Scholar

3. Nezhdbahadori, F.; Abdoli, M. A.; Baghdadi, M.; Ghazban, F. A Comparative Study on the Efficiency of Polar and Non-polar Solvents in Oil Sludge Recovery Using Solvent Extraction. Environ. Monit. Assess. 2018, 190, 389. https://doi.org/10.1007/s10661-018-6748-6.Search in Google Scholar PubMed

4. Zhang, X. W.; Zhang, H.; Wang, H. X.; Cao, Y. J.; Zhang, L. A Makeup Remover-Inspired Chitosan-Based Emulsion for Heavy Oil Removal in Oily Sludge Treatment. Fuel 2022, 330, 125588. https://doi.org/10.1016/j.fuel.2022.125588.Search in Google Scholar

5. Egazar’yants, S. V.; Vinokurov, V. A.; Vutolkina, A. V.; Talanova, M. Y.; Frolov, V. I.; Karakhanov, E. A. Oil Sludge Treatment Processes. Chem. Tech. Fuels Oils 2015, 51, 506–515. https://doi.org/10.1007/s10553-015-0632-7.Search in Google Scholar

6. Gong, Z. Q.; Zhang, H. T.; Juan, Y. L.; Zhu, L. K.; Zheng, W.; Ding, J. Q.; Tian, M. C.; Li, X. Y.; Zhang, J. Q.; Guo, Y. Z.; Li, G. E. A Review of Application and Development of Combustion Technology for Oil Sludge. J. Environ. Sci. Health Part A-Toxic/Hazard. Subst. Environ. Eng. 2022, 57, 396–412. https://doi.org/10.1080/10934529.2022.2071067.Search in Google Scholar PubMed

7. Wang, Z. B.; Wang, Z. Y.; Sun, J. W.; Wang, Y.; Sun, Z. Q.; Ma, K. S.; Wei, L. C. Investigation of Oxygen-Enriched Atmosphere Combustion of Oily Sludge: Performance, Mechanism, Emission of the S/N-containing Compound, and Residue Characteristics. J. Clean Prod. 2022, 378, 134233. https://doi.org/10.1016/j.jclepro.2022.134233.Search in Google Scholar

8. Ishaque, F.; Ripa, I. J.; Hossain, A.; Sarker, A. R.; Uddin, G. T.; Rahman, H.; Baidya, J. Application of Transform Software for Downscaling Global Climate Model EdGCM Results in North-Eastern Bangladesh. Environ. Eng. Res. 2021, 26, 190383. https://doi.org/10.4491/eer.2019.383.Search in Google Scholar

9. Tang, X. X.; Wei, X. S.; Chen, S. Y. Continuous Pyrolysis Technology for Oily Sludge Treatment in the Chain-Slap Conveyors. Sustainability 2019, 11, 3614. https://doi.org/10.3390/su11133614.Search in Google Scholar

10. Al-Doury, M. M. I. Treatment of Oily Sludge Using Solvent Extraction. Pet. Sci. Technol. 2019, 37, 190–196. https://doi.org/10.1080/10916466.2018.1533859.Search in Google Scholar

11. Hamidi, Y.; Ataei, S. A.; Sarrafi, A. A Simple, Fast and Low-Cost Method for the Efficient Separation of Hydrocarbons from Oily Sludge. J. Hazard. Mater. 2021, 413, 125328. https://doi.org/10.1016/j.jhazmat.2021.125328.Search in Google Scholar PubMed

12. Su, H. F.; Lin, J. F.; Wang, Q. Y. A Clean Production Process on Oily Sludge with a Novel Collaborative Process via Integrating Multiple Approaches. J. Clean Prod. 2021, 322, 128983. https://doi.org/10.1016/j.jclepro.2021.128983.Search in Google Scholar

13. Naik, B.S.; Mishra, I. M.; Bhattacharya, S. D. Biodegradation of Total Petroleum Hydrocarbons from Oily Sludge. Bioremediat. J. 2011, 15, 140–147. https://doi.org/10.1080/10889868.2011.598484.Search in Google Scholar

14. Hentati, D.; Abed, R. M. M.; Abotalib, N.; El Nayal, A. M.; Ashraf, I.; Ismail, W. Biotreatment of Oily Sludge by a Bacterial Consortium: Effect of Bioprocess Conditions on Biodegradation Efficiency and Bacterial Community Structure. Front. Microbiol. 2022, 13, 998076. https://doi.org/10.3389/fmicb.2022.998076.Search in Google Scholar PubMed PubMed Central

15. Jing, G. L.; Chen, T. T.; Luan, M. M. Studying Oily Sludge Treatment by Thermo Chemistry. Arab. J. Chem. 2016, 9, S457–S460. https://doi.org/10.1016/j.arabjc.2011.06.007.Search in Google Scholar

16. Liang, J. L.; Zhao, L. X.; Hou, W. G. Solid Effect in Chemical Cleaning Treatment of Oily Sludge. Colloid Surf. A-Physicochem. Eng. Asp. 2017, 522, 38–42. https://doi.org/10.1016/j.colsurfa.2017.02.038.Search in Google Scholar

17. Gou, X. Y.; Zheng, G. C.; Tang, J. J.; Tao, C. Y.; Liu, R. L.; Liu, Z. H. Electric Field Efficiently Enhanced Thermochemical Cleaning for Oil Recovery from Oily Sludge. Chem. Eng. Process. 2023, 185, 109314. https://doi.org/10.1016/j.cep.2023.109314.Search in Google Scholar

18. Ramsden, W. Separation of Solids in the Surface-Layers of Solutions and ‘suspensions’ (Observations on Surface-Membranes, Bubbles, Emulsions, and Mechanical coagulation) — Preliminary Account. Proc. R. Soc. Lond. 1904, 72, 156–164. https://doi.org/10.1098/rspl.1903.0034.Search in Google Scholar

19. Pickering, S. U. CXCVI — Emulsions. J. Chem. Soc., Trans. 1907, 91, 2001–2021. https://doi.org/10.1039/CT9079102001.Search in Google Scholar

20. Winuprasith, T.; Suphantharika, M. Properties and Stability of Oil-In-Water Emulsions Stabilized by Microfibrillated Cellulose from Mangosteen Rind. Food Hydrocolloids 2015, 43, 690–699. https://doi.org/10.1016/j.foodhyd.2014.07.027.Search in Google Scholar

21. Aveyard, R.; Binks, B. P.; Clint, J. H. Emulsions Stabilised Solely by Colloidal Particles. Adv. Colloid Interface Sci. 2003, 100-102, 503–546. https://doi.org/10.1016/S0001-8686(02)00069-6.Search in Google Scholar

22. Yang, Y.; Liu, Z.; Wu, D. Y.; Wu, M.; Tian, Y.; Niu, Z. W.; Huang, Y. Edge-modified Amphiphilic Laponite Nano-Discs for Stabilizing Pickering Emulsions. J. Colloid Interface Sci. 2013, 410, 27–32. https://doi.org/10.1016/j.jcis.2013.07.060.Search in Google Scholar PubMed

23. Yang, Y. Q.; Fang, Z. W.; Chen, X.; Zhang, W. W.; Xie, Y. M.; Chen, Y. H.; Liu, Z. G.; Yuan, W. E. An Overview of Pickering Emulsions: Solid-Particle Materials, Classification, Morphology, and Applications. Front. Pharmacol 2017, 8, 287. https://doi.org/10.3389/fphar.2017.00287.Search in Google Scholar PubMed PubMed Central

24. Albert, C.; Beladjine, M.; Tsapis, N.; Fattal, E.; Agnely, F.; Huang, N. Pickering Emulsions: Preparation Processes, Key Parameters Governing Their Properties and Potential for Pharmaceutical Applications. J. Control. Release 2019, 309, 302–332. https://doi.org/10.1016/j.jconrel.2019.07.003.Search in Google Scholar PubMed

25. Ni, L.; Yu, C.; Wei, Q. B.; Liu, D. M.; Qiu, J. S. Pickering Emulsion Catalysis: Interfacial Chemistry, Catalyst Design, Challenges, and Perspectives. Angew. Chem.-Int. Edit. 2022, 61, e202115885. https://doi.org/10.1002/anie.202115885.Search in Google Scholar PubMed

26. He, Y. Q.; Wu, F.; Sun, X. Y.; Li, R. Q.; Guo, Y. Q.; Li, C. B.; Zhang, L.; Xing, F. B.; Wang, W.; Gao, J. P. Factors that Affect Pickering Emulsions Stabilized by Graphene Oxide. ACS Appl. Mater. Interfaces 2013, 5, 4843–4855. https://doi.org/10.1021/am400582n.Search in Google Scholar PubMed

27. Tang, M. Y.; Wang, X. R.; Wu, F.; Liu, Y.; Zhang, S.; Pang, X. B.; Li, X. X.; Qiu, H. X. Au Nanoparticle/graphene Oxide Hybrids as Stabilizers for Pickering Emulsions and Au Nanoparticle/graphene Oxide@polystyrene Microspheres. Carbon 2014, 71, 238–248. https://doi.org/10.1016/j.carbon.2014.01.034.Search in Google Scholar

28. Shanmugharaj, A. M.; Yoon, J. H.; Yang, W. J.; Ryu, S. H. Synthesis, Characterization, and Surface Wettability Properties of Amine Functionalized Graphene Oxide Films with Varying Amine Chain Lengths. J. Colloid Interface Sci. 2013, 401, 148–154. https://doi.org/10.1016/j.jcis.2013.02.054.Search in Google Scholar PubMed

29. Zheng, Z.; Zheng, X. H.; Wang, H. T.; Du, Q. G. Macroporous Graphene Oxide-Polymer Composite Prepared through Pickering High Internal Phase Emulsions. ACS Appl. Mater. Interfaces 2013, 5, 7974–7982. https://doi.org/10.1021/am4020549.Search in Google Scholar PubMed

30. Chen, L. F.; Zhu, X. M.; Wang, L.; Yang, H.; Wang, D. G.; Fu, M. L. Experimental Study of Effective Amphiphilic Graphene Oxide Flooding for an Ultralow-Permeability Reservoir. Energy Fuels 2018, 32, 11269–11278. https://doi.org/10.1021/acs.energyfuels.8b02576.Search in Google Scholar

31. Wang, H. J.; Liu, J.; Xu, H. Y.; Ma, Z. W.; Jia, W. H.; Ren, S. L. Demulsification of Heavy Oil-In-Water Emulsions by Reduced Graphene Oxide Nanosheets. RSC Adv. 2016, 6, 106297–106307. https://doi.org/10.1039/C6RA18898B.Search in Google Scholar

32. Liu, J.; Wang, H. J.; Li, X. C.; Jia, W. H.; Zhao, Y. P.; Ren, S. L. Recyclable Magnetic Graphene Oxide for Rapid and Efficient Demulsification of Crude Oil-In-Water Emulsion. Fuel 2017, 189, 79–87. https://doi.org/10.1016/j.fuel.2016.10.066.Search in Google Scholar

33. Liu, J.; Li, X. C.; Jia, W. H.; Li, Z. Y.; Zhao, Y. P.; Ren, S. L. Demulsification of Crude Oil-In-Water Emulsions Driven by Graphene Oxide Nanosheets. Energy Fuels 2015, 29, 4644–4653. https://doi.org/10.1021/acs.energyfuels.5b00966.Search in Google Scholar

Supplementary Material

This article contains supplementary material (https://doi.org/10.1515/tsd-2023-2566).

Received: 2023-11-02

Accepted: 2024-03-26

Published Online: 2024-04-24

Published in Print: 2024-07-26

You are currently not able to access this content.

Supplementary Material Details

Articles in the same Issue

https://doi.org/10.1515/tsd-2023-2566

Keywords for this article

chemically modified graphite oxide; detergent prepared from emulsion; oily sludge; response surface methodology (RSM)