SpringerLink
Log in

In situ synthesis of melt-grown mullite ceramics using directed laser deposition

  • Ceramics
  • Published:
Journal of Materials Science Aims and scope Submit manuscript

Abstract

While mullite is a significant oxide ceramic material, its current preparation process has many limitations such as complicated process, low efficiency, and high cost. In this paper, directed laser deposition (DLD) was used to prepare mullite ceramics directly using α-Al2O3 and SiO2 powder as raw materials. The phase composition, microstructure, and primary defects of prepared samples were investigated by XRD, Raman spectroscopy, and SEM/EDS. Vickers indentation and three-point bending experiments were used to evaluate mechanical properties. The results showed that microstructure was mainly composed of a mullite crystal phase and Si-rich glass phase. It is shown that mullite ceramics were successfully synthesized in situ during the DLD process with the use of Al2O3 and SiO2 powder. Morphology of mullite crystal inside cylindrical sample was particular “tabular cellular,” which transformed into “rod cellular” at the edge. Two mullite crystals were arranged along deposition direction basically, surrounded by the Si-rich glass phase. The defects included pores with various sizes and crack, in which large pores were mainly distributed at the edge of the sample, and small pores were throughout the section. The crack was distributed in the center of the sample and spread to the edge. Mechanical properties test showed flexural strength, microhardness, and fracture toughness were 62.8 ± 30.3 MPa, 12.7 ± 0.34 GPa, and 1.84 ± 0.14 MPa·m1/2, respectively. It is considered that pores and crack were responsible for poor mechanical properties. This research is expected to provide a new option for the rapid preparation of mullite ceramics.

Graphic abstract

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

Access this article

Log in via an institution

Subscribe and save

Springer+ Basic
EUR 32.99 /Month
  • Get 10 units per month
  • Download Article/Chapter or Ebook
  • 1 Unit = 1 Article or 1 Chapter
  • Cancel anytime
Subscribe now

Buy Now

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

Instant access to the full article PDF.

Institutional subscriptions

Figure 1
Figure 2
Figure 3
Figure 4
Figure 5
Figure 6
Figure 7
Figure 8
Figure 9
Figure 10
Figure 11
Figure 12
Figure 13
Figure 14
Figure 15

Similar content being viewed by others

Data availability

The raw/processed data required to reproduce these findings cannot be shared at this time due to technical or time limitations.

References

  1. Aksay IA, Dabbs DM, Sarikaya M (1991) Mullite for structural, electronic, and optical applications. J Am Ceram Soc 74:2343–2358. https://doi.org/10.1111/j.1151-2916.1991.tb06768.x

    Article  CAS  Google Scholar 

  2. Schneider H, Schreuer J, Hildmann B (2008) Structure and properties of mullite—a review. J Eur Ceram Soc 28:329–344. https://doi.org/10.1016/j.jeurceramsoc.2007.03.017

    Article  CAS  Google Scholar 

  3. Ma BY, Su C, Ren X, Gao Z, Qian F, Yang W, Liu G, Li H, Yu J, Zhu Q (2019) Preparation and properties of porous mullite ceramics with high-closed porosity and high strength from fly ash via reaction synthesis process. J Alloy Compd 803:981–991. https://doi.org/10.1016/j.jallcom.2019.06.272

    Article  CAS  Google Scholar 

  4. Roy D, Das S, Nandy P (2012) Possibility of decreasing the activation energy of resistivity of mullite by do** with nickel ion. Mater Sci-Pol. 30:406–413. https://doi.org/10.2478/s13536-012-0049-5

    Article  CAS  Google Scholar 

  5. Schneider H, Fischer RX, Schreuer J (2015) Mullite: crystal structure and related properties. J Am Ceram Soc 98:2948–2967. https://doi.org/10.1111/jace.13817

    Article  CAS  Google Scholar 

  6. Cameron WE (1977) Mullite: a substituted alumina. Am Miner 62:747–755

    CAS  Google Scholar 

  7. Chen CY, Lan GS, Tuan WH (2000) Preparation of mullite by the reaction sintering of kaolinite and alumina. J Eur Ceram Soc 20:2519–2525. https://doi.org/10.1016/S0955-2219(00)00125-4

    Article  CAS  Google Scholar 

  8. Schneider H, Komarneni S (eds) (2006) Mullite. Wiley, Weinheim

    Google Scholar 

  9. Kanzaki S, Tabata H, Kumazawa T, Oht S (1985) Sintering and mechanical properties of stoichiometric Mullite. J Am Ceram Soc 68:C-6-C-7. https://doi.org/10.1111/j.1151-2916.1985.tb15252.x

    Article  Google Scholar 

  10. Montanaro L, Tulliani JM, Perrot C, Negro A (1997) Sintering of industrial mullites. J Eur Ceram Soc 17:1715–1723. https://doi.org/10.1016/S0955-2219(97)00043-5

    Article  CAS  Google Scholar 

  11. Cichy P (1967) Electrothermally Fused Mullite. America Ceramic Society Bulletin vol 46(9):735 Ceramic Place, Po Box 6136, Westerville, OH 43081-6136: Am Ceram Soc

  12. Cividanes LS, Campos TMB, Rodrigues LA, Brunelli DD, Thim GP (2010) Review of mullite synthesis routes by sol–gel method. J Sol-Gel Sci Technol 55:111–125. https://doi.org/10.1007/s10971-010-2222-9

    Article  CAS  Google Scholar 

  13. Mulpuri RP, Sarin VK (1996) Synthesis of mullite coatings by chemical vapor deposition. J Mater Res 11:1315–1324. https://doi.org/10.1557/JMR.1996.0166

    Article  CAS  Google Scholar 

  14. Guse W, Mateika D (1974) Growth of mullite single crystals (2Al2O3·SiO2) by the Czochralski method. J Cryst Growth 22:237–240. https://doi.org/10.1016/0022-0248(74)90101-8

    Article  CAS  Google Scholar 

  15. Carvalho RG, Fernandes AJS, Oliveira FJ, Alves E, Franco N, Louro C, Silva RF, Costa FM (2010) Single and polycrystalline mullite fibres grown by laser floating zone technique. J Eur Ceram Soc 30:3311–3318. https://doi.org/10.1016/j.jeurceramsoc.2010.07.033

    Article  CAS  Google Scholar 

  16. Buljan I, Kosanovic C, Kralj D (2011) A novel synthesis of nano-sized mullite from aluminosilicate precursors. J Alloy Compd 509:8256–8261. https://doi.org/10.1016/j.jallcom.2011.05.099

    Article  CAS  Google Scholar 

  17. Balla VK, Bose S, Bandyopadhyay A (2008) Processing of bulk alumina ceramics using laser engineered net sha**. Int J Appl Ceram Technol 5:234–242. https://doi.org/10.1111/j.1744-7402.2008.02202.x

    Article  CAS  Google Scholar 

  18. Yan S, Huang YF, Zhao DK, Niu FY, Ma GY, Wu DJ (2019) 3D printing of nano-scale Al2O3–ZrO2 eutectic ceramic: principle analysis and process optimization of pores. Addit Manuf 28:120–126. https://doi.org/10.1016/j.addma.2019.04.024

    Article  CAS  Google Scholar 

  19. Bernard SA, Balla VK, Bose S, Bandyopadhyay A (2010) Direct laser processing of bulk lead zirconate titanate ceramics. Mater Sci Eng B 172:85–88. https://doi.org/10.1016/j.mseb.2010.04.022

    Article  CAS  Google Scholar 

  20. Ouabbas Y, Chamayou A, Galet L, Baron M, Thomas G, Grosseau P, Guilhot B (2009) Surface modification of silica particles by dry coating: characterization and powder ageing. Powder Technol 190:200–209. https://doi.org/10.1016/j.powtec.2008.04.092

    Article  CAS  Google Scholar 

  21. Niihara K (1983) A fracture mechanics analysis of indentation-induced Palmqvist crack in ceramics. J Mater Sci Lett 2:221–223. https://doi.org/10.1007/BF00725625

    Article  CAS  Google Scholar 

  22. Niu FY, Wu DJ, Lu F, Liu G, Ma GY, Jia ZY (2018) Microstructure and macro properties of Al2O3 ceramics prepared by laser engineered net sha**. Ceram Int 44:14303–14310. https://doi.org/10.1016/j.ceramint.2018.05.036

    Article  CAS  Google Scholar 

  23. McMillan P, Piriou B (1982) The structures and vibrational spectra of crystals and glasses in the silica-alumina system. J Non-Cryst Solids 53:279–298. https://doi.org/10.1016/0022-3093(82)90086-2

    Article  CAS  Google Scholar 

  24. Rüscher CH (1996) Phonon spectra of 2:1 mullite in infrared and Raman experiments. Phys Chem Miner 23:50–55. https://doi.org/10.1007/BF00202993

    Article  Google Scholar 

  25. Regiani I, Magalhaes WLE, de Souza DPF, Paiva-Santos CO, de Souza MF (2002) Nucleation and growth of mullite whiskers from lanthanum-doped aluminosilicate melts. J Am Ceram Soc 85:232–238. https://doi.org/10.1111/j.1151-2916.2002.tb00071.x

    Article  CAS  Google Scholar 

  26. Fan ZQ, Zhao YT, Tan QY, Mo N, Zhang MX, Lu MY, Huang H (2019) Nanostructured Al2O3–YAG–ZrO2 ternary eutectic components prepared by laser engineered net sha**. Acta Mater 170:24–37. https://doi.org/10.1016/j.actamat.2019.03.020

    Article  CAS  Google Scholar 

  27. Klug FJ, Prochazka S, Doremus RH (1987) Alumina-silica phase diagram in the mullite region. J Am Ceram Soc 70:750–759. https://doi.org/10.1111/j.1151-2916.1987.tb04875.x

    Article  CAS  Google Scholar 

  28. He X, Li C, Liu JL, Huang QX, Shen XF, Liu TY, Lu AX (2020) Glass forming ability, structure and properties of Cr2O3–Fe2O3 co-doped MgO–Al2O3–SiO2–B2O3 glasses and glass-ceramics. J Non-Cryst Solids 529:119779. https://doi.org/10.1016/j.jnoncrysol.2019.119779

    Article  CAS  Google Scholar 

  29. Baer A (1998) Microstructural development of melt-grown mullite fibrils. PhD Dissertation, University of California Santa Barbara

  30. Zhao YZ, Yin HR (2006) Glass. Chemical Industry Press, Bei**g

    Google Scholar 

  31. Sung YM (2000) Kinetics analysis of mullite formation reaction at high temperatures. Acta Mater 48:2157–2162. https://doi.org/10.1016/S1359-6454(00)00032-X

    Article  CAS  Google Scholar 

  32. Jian Z, Kuribayashi K, Jie W (2004) Critical undercoolings for the transition from the lateral to continuous growth in undercooled silicon and germanium. Acta Mater 52:3323–3333. https://doi.org/10.1016/j.actamat.2004.03.027

    Article  CAS  Google Scholar 

  33. Li MJ, Nagashio K, Kuribayashi K (2001) On occurrence of multiple-site crystallization in undercooled mullite melts. Scr Mater 45:1431–1437. https://doi.org/10.1016/S1359-6462(01)01180-0

    Article  CAS  Google Scholar 

  34. Sing SL, Yeong WY, Wiria FE, Tay BY, Zhao ZQ, Zhao L, Tian ZL, Yang SF (2017) Direct selective laser sintering and melting of ceramics: a review. Rapid Prototyp J 23:611–623. https://doi.org/10.1108/RPJ-11-2015-0178

    Article  Google Scholar 

  35. Knudsen FP (1959) Dependence of mechanical strength of brittle polycrystalline specimens on porosity and grain size. J Am Ceram Soc 42:376–387. https://doi.org/10.1111/j.1151-2916.1959.tb13596.x

    Article  CAS  Google Scholar 

  36. Griffith AA (1921) VI. The phenomena of rupture and flow in solids. Philos Trans R Soc A-Math Phys Eng Sci 221:582–593. https://doi.org/10.1098/rsta.1921.0006

    Article  Google Scholar 

  37. Kriven WM, Siah LF, Schmücker M, Schneider H (2004) High temperature microhardness of single crystal Mullite. J Am Ceram Soc 87:970–972. https://doi.org/10.1111/j.1551-2916.2004.00970.x

    Article  CAS  Google Scholar 

Download references

Acknowledgements

The authors would like to acknowledge the financial support from the National Natural Science Foundation of China (No. 51805070, No. 51790172), the Fundamental Research Funds for the Central Universities (DUT19RC(3)060) and the Liaoning Province Natural Science Foundation Guidance Program (2019-ZD-0010).

Author information

Authors and Affiliations

  1. Key Laboratory for Precision and Non-traditional Machining Technology of Ministry of Education, Dalian University of Technology, Dalian, 116024, Liaoning Province, People’s Republic of China

    Dongjiang Wu, Dake Zhao, Fangyong Niu, Yunfei Huang, Jia Zhu & Guangyi Ma

Authors
  1. Dongjiang Wu
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Dake Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Fangyong Niu
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Yunfei Huang
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Jia Zhu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Guangyi Ma
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

Fangyong Niu helped in conceptualization, methodology, formal analysis, investigation, writing—review and editing, funding acquisition. Dongjiang Wu contributed to investigation, experiments, writing—review and editing, project administration, funding acquisition, supervision. Dake Zhao contributed to conceptualization, methodology, investigation, visualization, formal analysis, writing—original draft. Yunfei Huang helped in writing—review and editing. Jia Zhu helped in investigation, experiments, writing—review and editing. Guangyi Ma helped in writing—review and editing. All authors read and approved the manuscript.

Corresponding author

Correspondence to Fangyong Niu.

Ethics declarations

Conflict of interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Ethical approval

The authors declare under the ethical responsibility that the submitted paper is original and has not been or is not being submitted to the peer review process to any other journal, and that all the authors have read the paper and agree with its submission to Journal of Materials Science.

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

Wu, D., Zhao, D., Niu, F. et al. In situ synthesis of melt-grown mullite ceramics using directed laser deposition. J Mater Sci 55, 12761–12775 (2020). https://doi.org/10.1007/s10853-020-04938-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10853-020-04938-3

Search

Navigation