Skip to main content
SpringerLink
Log in

Chemical reactions of oily sludge catalyzed by iron oxide under supercritical water gasification condition

  • Research Article
  • Published:
Frontiers of Chemical Science and Engineering Aims and scope Submit manuscript

Abstract

Supercritical water gasification is a promising technology in dealing with the degradation of hazardous waste, such as oily sludge, accompanied by the production of fuel gases. To evaluate the mechanism of Fe2O3 catalyst and the migration pathways of heteroatoms and to investigate the systems during the process, reactive force field molecular dynamics simulations are adopted. In terms of the catalytic mechanisms of Fe2O3, the surface lattice oxygen is consumed by small carbon fragments to produce CO and CO2, improving the catalytic performance of the cluster due to more unsaturated coordination Fe sites exposed. Lattice oxygen combines with •H radicals to form water molecules, improving the catalytic performance. Furthermore, the pathway of asphaltene degradation was revealed at an atomic level, as well as products. Moreover, the adsorption of hydroxyl radical on the S atom caused breakage of the two C-S bonds in turn, forming •HSO intermediate, so that the organic S element was fixed into the inorganic liquid phase. The heteroatom O was removed under the effects of supercritical water. Heavy metal particles presented in the oily sludge, such as iron in association with Fe2O3 catalyst, helped accelerate the degradation of asphaltenes.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

References

  1. Gao N, Li J, Quan C, Tan H. Product property and environmental risk assessment of heavy metals during pyrolysis of oily sludge with fly ash additive. Fuel, 2020, 266: 117090

    Article  CAS  Google Scholar 

  2. Hamidi Y, Ataei S A, Sarrafi A. A highly efficient method with low energy and water consumption in biodegradation of total petroleum hydrocarbons of oily sludge. Journal of Environmental Management, 2021, 293: 112911

    Article  CAS  PubMed  Google Scholar 

  3. Liu J, Zhang Y, Peng K, Zhao X, Xiong Y, Huang X. A review of the interfacial stability mechanism of aging oily sludge: heavy components, inorganic particles, and their synergism. Journal of Hazardous Materials, 2021, 415: 125624

    Article  CAS  PubMed  Google Scholar 

  4. Zou H, Liu C, Evrendilek F, He Y, Liu J. Evaluation of reaction mechanisms and emissions of oily sludge and coal co-combustions in O2/CO2 and O2/N2 atmospheres. Renewable Energy, 2021, 171: 1327–1343

    Article  CAS  Google Scholar 

  5. Gao N, Li J, Quan C, Wang X, Yang Y. Oily sludge catalytic pyrolysis combined with fine particle removal using a Ni-ceramic membrane. Fuel, 2020, 277: 118134

    Article  CAS  Google Scholar 

  6. Li Z, Zhou Y, Meng X, Wang S. Harmless and efficient treatment of oily drilling cuttings. Journal of Petroleum Science Engineering, 2021, 202: 108542

    Article  CAS  Google Scholar 

  7. Gao Y, Ding R, Wu S, Wu Y, Zhang Y, Yang M. Influence of ultrasonic waves on the removal of different oil components from oily sludge. Environmental Technology, 2015, 36(13–16): 1771–1775

    Article  CAS  PubMed  Google Scholar 

  8. Chen G, Li J, Li K, Lin F, Tian W, Che L, Yan B, Ma W, Song Y. Nitrogen, sulfur, chlorine containing pollutants releasing characteristics during pyrolysis and combustion of oily sludge. Fuel, 2020, 273: 117772

    Article  CAS  Google Scholar 

  9. Kruse A, Dahmen N. Water—a magic solvent for biomass conversion. Journal of Supercritical Fluids, 2015, 96: 36–45

    Article  CAS  Google Scholar 

  10. Okolie J A, Nanda S, Dalai A K, Kozinski J A. Optimization and modeling of process parameters during hydrothermal gasification of biomass model compounds to generate hydrogen-rich gas products. International Journal of Hydrogen Energy, 2020, 45(36): 18275–18288

    Article  CAS  Google Scholar 

  11. Ding W, Shi J, Wei W, Cao C, Jin H. A molecular dynamics simulation study on solubility behaviors of polycyclic aromatic hydrocarbons in supercritical water/hydrogen environment. International Journal of Hydrogen Energy, 2021, 46(3): 2899–2904

    Article  CAS  Google Scholar 

  12. Khan M K, Cahyadi H S, Kim S M, Kim J. Efficient oil recovery from highly stable toxic oily sludge using supercritical water. Fuel, 2019, 235: 460–472

    Article  CAS  Google Scholar 

  13. Adar E, Ince M, Bilgili M S. Supercritical water gasification of sewage sludge by continuous flow tubular reactor: a pilot scale study. Chemical Engineering Journal, 2020, 391: 123499

    Article  CAS  Google Scholar 

  14. Hantoko D, Antoni, Kanchanatip E, Yan M, Weng Z, Gao Z, Zhong Y. Assessment of sewage sludge gasification in supercritical water for H2-rich syngas production. Process Safety and Environmental Protection, 2019, 131: 63–72

    Article  CAS  Google Scholar 

  15. Lin J, Liao Q, Hu Y, Ma R, Cui C, Sun S, Liu X. Effects of process parameters on sulfur migration and H2S generation during supercritical water gasification of sludge. Journal of Hazardous Materials, 2021, 403: 123678

    Article  CAS  PubMed  Google Scholar 

  16. Chen Y, Yi L, Li S, Yin J, Jin H. Catalytic gasification of sewage sludge in near and supercritical water with different catalysts. Chemical Engineering Journal, 2020, 388: 124292

    Article  CAS  Google Scholar 

  17. Qian L, Wang S, Xu D, Guo Y, Tang X, Wang L. Treatment of municipal sewage sludge in supercritical water: a review. Water Research, 2016, 89: 118–131

    Article  CAS  PubMed  Google Scholar 

  18. Cao C, Xie Y, Mao L, Wei W, Shi J, Jin H. Hydrogen production from supercritical water gasification of soda black liquor with various metal oxides. Renewable Energy, 2020, 157: 24–32

    Article  CAS  Google Scholar 

  19. Han Y, Wang Y, Ma T, Li W, Zhang J, Zhang M. Mechanistic understanding of Cu-based bimetallic catalysts. Frontiers of Chemical Science and Engineering, 2020, 14(5): 689–748

    Article  CAS  Google Scholar 

  20. Gao Y, Zhu W, Liu J, Lin P, Zhang J, Huang T, Liu K. Mesoporous sulfur-doped CoFe2O4 as a new Fenton catalyst for the highly efficient pollutants removal. Applied Catalysis B: Environmental, 2021, 295: 120273

    Article  CAS  Google Scholar 

  21. van Duin A C T, Dasgupta S, Lorant F, Goddard W A. ReaxFF: a reactive force field for hydrocarbons. Journal of Physical Chemistry A, 2001, 105(41): 9396–9409

    Article  CAS  Google Scholar 

  22. Han Y, Jiang D, Zhang J, Li W, Gan Z, Gu J. Development, application and challenges of ReaxFF reactive force field in molecular simulations. Frontiers of Chemical Science and Engineering, 2016, 10(1): 16–38

    Article  CAS  Google Scholar 

  23. Zhang J, Weng X, Han Y, Li W, Cheng J, Gan Z, Gu J. The effect of supercritical water on coal pyrolysis and hydrogen production: a combined ReaxFF and DFT study. Fuel, 2013, 108: 682–690

    Article  CAS  Google Scholar 

  24. Han Y, Ma T, Chen F, Li W, Zhang J. Supercritical water gasification of naphthalene over iron oxide catalyst: a ReaxFF molecular dynamics study. International Journal of Hydrogen Energy, 2019, 44(57): 30486–30498

    Article  CAS  Google Scholar 

  25. Zhang J, Gu J, Han Y, Li W, Gan Z, Gu J. Supercritical water oxidation vs supercritical water gasification: which process is better for explosive wastewater treatment? Industrial & Engineering Chemistry Research, 2015, 54(4): 1251–1260

    Article  CAS  Google Scholar 

  26. Han Y, Chen F, Ma T, Gong H, Al-Shwafy K W A, Li W, Zhang J, Zhang M. Size effect of a Ni nanocatalyst on supercritical water gasification of lignin by reactive molecular dynamics simulations. Industrial & Engineering Chemistry Research, 2019, 58(51): 23014–23024

    Article  CAS  Google Scholar 

  27. Jiang D, Wang Y, Zhang M, Zhang J, Li W, Han Y. H2 and CO production through coking wastewater in supercritical water condition: ReaxFF reactive molecular dynamics simulation. International Journal of Hydrogen Energy, 2017, 42(15): 9667–9678

    Article  CAS  Google Scholar 

  28. Han Y, Ma T, Chen F, Li W, Zhang J. Synergistic mechanism of Ni catalyst and supercritical water during refractory organic wastewater treatment. Industrial & Engineering Chemistry Research, 2019, 58(4): 1535–1547

    Article  CAS  Google Scholar 

  29. Bai Y, Sui H, Liu X, He L, Li X, Thormann E. Effects of the N, O, and S heteroatoms on the adsorption and desorption of asphaltenes on silica surface: a molecular dynamics simulation. Fuel, 2019, 240: 252–261

    Article  CAS  Google Scholar 

  30. Schuler B, Meyer G, Pena D, Mullins O C, Gross L. Unraveling the molecular structures of asphaltenes by atomic force microscopy. Journal of the American Chemical Society, 2015, 137(31): 9870–9876

    Article  CAS  PubMed  Google Scholar 

  31. Stephens P J, Devlin F J, Chabalowski C F, Frisch M J. Ab initio calculation of vibrational absorption and circular dichroism spectra using density functional force fields. Journal of Chemical Physics, 1994, 98(45): 11623–11627

    Article  CAS  Google Scholar 

  32. Krishnan R, Binkley J S, Seeger R, Pople J A. Self-consistent molecular orbital methods. XX. A basis set for correlated wave functions. Journal of Chemical Physics, 1980, 72(1): 650–654

    Article  CAS  Google Scholar 

  33. Shin Y K, Kwak H, Vasenkov A V, Sengupta D, van Duin A C T. Development of a ReaxFF reactive force field for Fe/Cr/O/S and application to oxidation of butane over a pyrite-covered Cr2O3 catalyst. ACS Catalysis, 2015, 5(12): 7226–7236

    Article  CAS  Google Scholar 

  34. Hu Y, Qi L, Rao K T V, Zhao B, Li H, Zeng Y, Xu C. Supercritical water gasification of biocrude oil from low-temperature liquefaction of algal lipid extraction residue. Fuel, 2020, 276: 118017

    Article  CAS  Google Scholar 

  35. Sorensen M R, Voter A F. Temperature-accelerated dynamics for simulations of infrequent events. Journal of Chemical Physics, 2000, 112(21): 9599–9606

    Article  CAS  Google Scholar 

  36. Wang X, Xue X, Zhang C. Early events of the carburization of Fe nanoparticles in ethylene pyrolysis: reactive force field molecular dynamics simulations. Journal of Physical Chemistry C, 2018, 122(20): 10835–10845

    Article  CAS  Google Scholar 

  37. Bentria E T, Akande S O, Becquart C S, Mousseau N, Bouhali O, El-Mellouhi F. Capturing the iron carburization mechanisms from the surface to bulk. Journal of Physical Chemistry C, 2020, 124(52): 28569–28579

    Article  CAS  Google Scholar 

  38. Liu X, Wen X, Hoffmann R. Surface activation of transition metal nanoparticles for heterogeneous catalysis: what we can learn from molecular dynamics. ACS Catalysis, 2018, 8(4): 3365–3375

    Article  CAS  Google Scholar 

  39. Chen H, He Z, Zhang B, Feng H, Kandasamy S, Wang B. Effects of the aqueous phase recycling on bio-oil yield in hydrothermal liquefaction of spirulina platensis, α-cellulose, and lignin. Energy, 2019, 179: 1103–1113

    Article  CAS  Google Scholar 

  40. Meng N, Jiang D, Liu Y, Gao Z, Cao Y, Zhang J, Gu J, Han Y. Sulfur transformation in coal during supercritical water gasification. Fuel, 2016, 186: 394–404

    Article  CAS  Google Scholar 

  41. Dasireddy V D B C, Likozar B. Direct methanol production from mixed methane/H2O/N2O feedstocks over Cu−Fe/Al2O3 catalysts. Fuel, 2021, 301: 121084

    Article  CAS  Google Scholar 

  42. Kou J, Yi L, Li G, Cheng K, Wang R, Zhang D, Jin H, Guo L. Structural effect of ZrO2 on supported Ni-based catalysts for supercritical water gasification of oil-containing wastewater. International Journal of Hydrogen Energy, 2021, 46(24): 12874–12885

    Article  CAS  Google Scholar 

  43. Mastuli M S, Kamarulzaman N, Kasim M F, Mahat A M, Matsumura Y, Taufiq-Yap Y H. Catalytic supercritical water gasification of oil palm frond biomass using nanosized MgO doped Zn catalysts. Journal of Supercritical Fluids, 2019, 154: 104610

    Article  CAS  Google Scholar 

  44. Samiee-Zafarghandi R, Hadi A, Karimi-Sabet J. Graphene-supported metal nanoparticles as novel catalysts for syngas production using supercritical water gasification of microalgae. Biomass and Bioenergy, 2019, 121: 13–21

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant Nos. 21978210 and U20A20151), Tianjin Natural Science Foundation, China (Grant No. 19JCYBJC20000) and the National Key R&D Program of China (Grant No. 2018YFA0702403). The Gaussian 09 software was supported by the National Supercomputing Center in Shenzhen.

Author information

Authors and Affiliations

  1. School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China

    Houjun Zhang, Fang Chen, Jipeng Xu, Jinli Zhang & You Han

  2. Tianjin Key Laboratory of Membrane Science and Desalination Technology, Tianjin University, Tianjin, 300072, China

    You Han

Authors
  1. Houjun Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Fang Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Jipeng Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Jinli Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. You Han
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to You Han.

Electronic supplementary material

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, H., Chen, F., Xu, J. et al. Chemical reactions of oily sludge catalyzed by iron oxide under supercritical water gasification condition. Front. Chem. Sci. Eng. 16, 886–896 (2022). https://doi.org/10.1007/s11705-021-2125-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11705-021-2125-z

Keywords

Search

Navigation