Skip to main content
Log in

Formation Mechanism of SiC in the Diffusion Couple Interface during the MG-Si Production Process

  • Original Paper
  • Published:
Silicon Aims and scope Submit manuscript

Abstract

SiC is an important intermediate product in the production process of metallurgical-grade silicon (MG-Si), and is of great significance for the improvement of the efficiency of MG-Si production. In this study, the formation mechanism of SiC is revealed via an experimental system of a silica-charcoal diffusion couple. The phase transition and microscopic characteristics of the contact interface of the diffusion couple indicate that SiC forms on the carbon side, while the silica side is eroded. The element distribution characteristics of the reaction cross-section reveal that SiC forms inside the carbon along the longitudinal direction. Via the combination of thermodynamic calculation and experimental analysis, the formation mechanisms of SiC on the surface and inside the carbon are confirmed; the SiC on the surface is formed by both one-step and two-step reactions, while the internal SiC is formed only by a two-step reaction. Moreover, increasing the temperature is found to be beneficial to the formation of SiC, and the thickness of the SiC layer increased from 130 to 135 μm with the increase of the temperature from 1673 K to 1773 K. SiO is found to be the key intermediate of the two-step reaction. The prevention of the escape of SiO has great significance for the reduction of the costs and the increase of the yield of MG-Si production.

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

Access this article

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

Instant access to the full article PDF.

Similar content being viewed by others

Data Availability

All data generated or analyzed during this study are included in this paper.

References

  1. Bablin JM, Crawford AC, DeMoulpied DC, Lewis LN (2003) Effect of low aluminum silicon on the direct process. Ind Eng Chem Res 42(15):3555–3565

    Article  CAS  Google Scholar 

  2. Lei Y, Ma WH, Wu JJ, Wei KX, Li SY, Morita K (2018) Impurity phases and their removal in Si purification with Al-Si alloy using transition metals as additives. J Alloy Compd 734:250–257

    Article  CAS  Google Scholar 

  3. Yang SC, Wan XH, Wei KX, Ma WH, Wang Z (2021) Silicon recovery from diamond wire saw silicon powder waste with hydrochloric acid pretreatment: an investigation of Al dissolution behavior. Waste Manag 120:820–827

    Article  CAS  Google Scholar 

  4. Han SF, Tan N, Wei KX, Ma WH (2022) Electromagnetic separation of silicon from metallurgical-grade silicon refined slag during the remelting process. Sep Purif Technol 280:119815

    Article  CAS  Google Scholar 

  5. Ding Z, Chen ZQ, Ma TY, Lu CT, Ma WH, Shaw L (2020) Predicting the hydrogen release ability of LiBH4-based mixtures by ensemble machine learning. Energy Storage Mater 27:466–477

    Article  Google Scholar 

  6. Wang DL, Meng WL, Zhou HR, Li GX, Yang Y, Li HW (2021) Green hydrogen coupling with CO2 utilization of coal-to-methanol for high methanol productivity and low CO2 emission. Energy 231:120970

    Article  CAS  Google Scholar 

  7. Ding Z, Yang WJ, Huo KF, Shaw L (2021) Thermodynamics and kinetics tuning of LiBH4 for hydrogen storage. Prog Chem 33(9):1586–1597

    CAS  Google Scholar 

  8. Chen ZJ, Zhou SC, Ma WH, Deng XC, Li SY, Ding WM (2018) The effect of the carbonaceous materials properties on the energy consumption of silicon production in the submerged arc furnace. J Clean Prod 191:240–247

    Article  CAS  Google Scholar 

  9. Zhou SC, Chen ZJ, Ma WH, Li SY, Li C, Wu JJ, Yang X (2020) Effect of K2CO3 as an additive agent on the carbothermic reduction process of silicon production. Silicon-Neth 12:1575–1584

    Article  CAS  Google Scholar 

  10. Yang SC, Wan XH, Wei KX, Ma WH, Wang Z (2021) Silicon recycling and iron, nickel removal from diamond wire saw silicon powder waste: synergistic chlorination with CaO smelting treatment. Miner Eng 196:106966

    Article  Google Scholar 

  11. Broggi A, Tangstad M, Ringdalen E (2019) Characterization of a Si-SiO2 mixture generated from SiO(g) and CO(g). Metall Mater Trans B Process Metall Mater Process Sci 50:2667–2680

    Article  CAS  Google Scholar 

  12. Aarnæs TS, Ringdalen E, Tangstad M (2020) Silicon carbide formation from methane and silicon monoxide. Sci Rep-Uk 10:21831

    Article  Google Scholar 

  13. Ringdalen E, Tangstad M (2016) Softening and melting of SiO2, an important parameter for reactions with quartz in Si production. Advances in Molten Slags, Fluxes, and Salts: Proceedings of the 10th International Conference on Molten Slags, Fluxes and Salts. Pages:41-51 https://doi.org/10.1002/9781119333197.ch4

  14. Cao SJ, Zhou SC, Chen ZJ, Ma WH (2021) Effect of grinding media on the synergistic characteristics of coal and biomass for the carbothermal reduction of silica. Phosphorus Sulfur 196(6):1–10

    Article  Google Scholar 

  15. Li F, Tangstad M, Ringdalen E (2018) Carbothermal reduction of quartz and carbon pellets at elevated temperatures. Metall Mater Trans B Process Metall Mater Process Sci 49:1078–1088

    Article  CAS  Google Scholar 

  16. Sakaguchi Y, Ishizaki M, Kawahara T, Fukai M, Yoshiyagawa M, Aratani F (1992) Production of high purity silicon by carbothermic reduction of silica using AC-arc furnace with heated shaft. ISIJ Int 32(5):643–649

    Article  CAS  Google Scholar 

  17. Jayakumari S, Tangstad M (2020) Transformation of β-SiC from charcoal, coal, and petroleum coke to α-SiC at higher temperatures. Metall Mater Trans B Process Metall Mater Process Sci 51:2673–2688

    Article  Google Scholar 

  18. Folstad MB, Ringdalen E, Tveit H, Tangstad M (2021) Effect of different SiO2 polymorphs on the reaction between SiO2 and SiC in Si production. Metall Mater Trans B Process Metall Mater Process Sci 52:792–803

    Article  CAS  Google Scholar 

  19. Weimer AW, Nilsen KJ, Cochran GA, Roach RP (1993) Kinetics of carbothermal reduction synthesis of beta silicon carbide. AICHE J 39(3):493–503

    Article  CAS  Google Scholar 

  20. Wiik K, Motzfeldt K (1995) Kinetics of reactions between silica and carbon and the formation of silicon carbide. MRS Online Proceedings Library. 410:435-440 https://doi.org/10.1557/proc-410-435

  21. Agarwal A, Pad U (1999) Influence of pellet composition and structure on carbothermic reduction of silica. Metall Mater Trans B Process Metall Mater Process Sci 30(2):295–306

    Article  Google Scholar 

  22. Li F, Tangstad M (2017) Carbothermal reduction of quartz with carbon from natural gas. Metall Mater Trans B Process Metall Mater Process Sci 48:853–869

    Article  CAS  Google Scholar 

  23. Lu PF, Jin ZH, Cui BW, Xu GH, Wu RC (2021) Effect of raw material size on the synthesis of silicon carbide. CIESC Journal 72(4):2300–2308

    CAS  Google Scholar 

  24. Van Dijen FK, Metselaar R (1991) The chemistry of the carbothermal synthesis of β-SiC: reaction mechanism, reaction rate and grain growth. J Eur Ceram Soc 7:177–184

    Article  Google Scholar 

  25. Klinghoffer NB, Castaldi MJ, Nzihou A (2015) Influence of char composition and inorganics on catalytic activity of char from biomass gasification. Fuel 157:37–47

    Article  CAS  Google Scholar 

  26. Li X, Gu YW, Wu S, Chen S, Quan X, Yu HT (2021) Selective reduction of nitrate to ammonium over charcoal electrode derived from natural wood. Chemosphere 285:131501

    Article  CAS  Google Scholar 

  27. Kuang J, Cao W (2013) Silicon carbide whiskers: preparation and high dielectric permittivity. J Am Ceram Soc 96(9):2877–2880

    Article  CAS  Google Scholar 

  28. Seo W, Koumoto K (1996) Stacking faults in β-SiC formed during carbothermal reduction of SiO2. J Am Ceram Soc 79(7):1777–1782

    Article  CAS  Google Scholar 

  29. Zhou SC, Chen ZJ, Yin G, Ma WH, Cao SJ (2021) Influence of the grinding media applying in the soft coal and waste biomass on the carbothermic reduction process of silica. Silicon-Neth 13:3963–3970

    Article  CAS  Google Scholar 

  30. Zhang HW, Guo SJ, Wu JJ, Wu DD, Wei KX, Ma WH (2021) Effect of quartz crystal structure transformations on the removal of iron impurities. Hydrometallurgy 204:105715

    Article  CAS  Google Scholar 

  31. Li XK, Liu L, Zhang YX, Shen SD, Ge S, Ling LC (2001) Synthesis of nanometre silicon carbide whiskers from binary carbonaceous silica aerogels. Carbon 39:159–165

    Article  CAS  Google Scholar 

  32. Milewski JV, Gac FD, Petrovic JJ, Skaggs SR (1985) Growth of beta-silicon carbide whiskers by the VLS process. J Mater Sci 20:1160–1166

    Article  CAS  Google Scholar 

  33. Li X, Zhang G, Tang K, Ostrovski O, Tronstad R (2015) Carbothermal reduction of quartz in methane-hydrogen-argon gas mixture. Metall Mater Trans B Process Metall Mater Process Sci 46:2384–2393

    Article  CAS  Google Scholar 

Download references

Acknowledgments

The authors gratefully acknowledge that this study was supported by the National Natural Science Foundation of China (Grant No. U1902219), the Yunnan Young and Middle-aged Academic and Technical Leader Reserve Talent Project (Grant No. 2018HB009), the Yunnan Outstanding Youth Science Foundation (Grant No. 202101AV070007), and the Major Science and Technology Projects in Yunnan Province (Grant Nos. 2019ZE007 and 202002AB080002).

Funding

Funding was provided by the National Natural Science Foundation of China (Grant No. U1902219), the Yunnan Young and Middle-aged Academic and Technical Leader Reserve Talent Project (Grant No. 2018HB009), the Yunnan Outstanding Youth Science Foundation (Grant No. 202101AV070007), and the Major Science and Technology Projects in Yunnan Province (Grant Nos. 2019ZE007 and 202002AB080002).

Author information

Authors and Affiliations

Authors

Contributions

Dongling Liu: Conceptualization, Formal analysis, Validation, Data curation, Writing–original draft, Writing–review & editing;

Xiaocong Deng: Resources, Data Curation, Resources, Visualization;

Jinsong Tai: Investigation, Resources, Visualization;

Shicong Yang: Investigation, Resources, Visualization;

Kuixian Wei: Supervision, Funding acquisition;

Wenhui Ma: Supervision, Funding acquisition.

Corresponding author

Correspondence to Kuixian Wei.

Ethics declarations

Ethics Approval

The data of this submission required ethics approval and are in compliance with ethical standards.

Consent to Participate

Not applicable.

Consent for Publication

Not applicable.

Conflict of Interest

The authors declare that they have no financial or personal relationships with other people or organizations that may have inappropriately influenced this work. Moreover, there is no professional or other personal interest of any nature or kind in any product, service, and/or company that could be construed as influencing the position presented in, or the review of, the manuscript entitled, “Formation mechanism of SiC in the diffusion couple interface during the MG-Si production process.”

Informed Consent

All authors and associated personnel are aware of and agree to the content of this submission.

Additional information

Publisher’s Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Liu, D., Deng, X., Tai, J. et al. Formation Mechanism of SiC in the Diffusion Couple Interface during the MG-Si Production Process. Silicon 14, 11371–11380 (2022). https://doi.org/10.1007/s12633-022-01876-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12633-022-01876-4

Keywords

Navigation