Experimental Characterization and Model Verification of Thermal Conductivity from Mesoporous to Macroporous SiOC Ceramics

Abstract

Based on the chemical cross-linking method, this paper uses polydimethylsiloxane with various viscosities of 10 cSt, 20 cSt, 50 cSt, and 100 cSt to synthesize mesoporous and macroporous SiOC ceramics. Their thermal conductivities are measured by using 3ω method with high accuracy. Three typical models for their thermal conductivities, i.e., series model (SM), maxwell-Eucken 1 model (ME1), and effective medium theory (EMT) model, are utilized to derive the empirical formula through the multi-parameter linear optimization algorithm, which agrees well with the experimental results. The effects of pore size and specific surface area on the overall thermal conductivity of the porous structure are explored. Interestingly, it is found that the thermal conductivities of both gas phase and solid phase inside the porous structure increase with the increasing pore size at the nanometer scale, but the overall thermal conductivity of the porous structure decreases with the increasing pore size. Scanning electron microscopy graphs corroborate that the extension of the heat transfer route and the barrier of more pores between the solid phases together cause the reduction of the gas-solid coupling thermal conductivity of SiOC ceramics with larger pore size. On the contrary, the miniaturization of individual particles through modulating the synthesis parameters can increase the number of small pores in the sample itself to meet the pseudo-lattice vibration conditions, which results in the increment of the gas-solid coupling thermal conductivity and the overall thermal conductivity of the porous structure. These findings would provide meaningful guidance for designing SiOC porous ceramic super-insulation materials with extremely low thermal conductivity.

This is a preview of subscription content, access via your institution.

Abbreviations

A :

specific surface area of SiOC/m2·g−1

d por :

median pore diameter

k :

thermal conductivity/W·m−1·K−1

l :

the solid phonon mean free path/nm

p :

gas pressure/Pa

r :

the radius of the solid particle/nm

S s :

specific surface area of sample/m2·kg−1

T :

gas temperature/K

V :

freestanding sensor’s voltage signal

v :

volume fraction

α CR :

temperature coefficient of resistance

θ :

freestanding sensor’s temperature rise/K

ρ :

the density/kg·m−3

ϕ :

the porosity

cv:

convection

EMT:

effective medium theory

e:

experimental

fm:

fluid mass transfer

g:

gas-phase

L:

liquid phase

ME1:

maxwell-Eucken 1

ME2:

maxwell-Eucken 2

opt:

theoretical(optimized)

PM:

parallel model

rd:

radiation

SM:

series model

s:

solid-phase

th:

theoretically

1ω,rms:

real part of the first harmonic

3ω,rms:

real part of the third harmonic

References

  1. [1]

    Stabler C., Reitz A., Stein P., Albert B., Riedel R., Ionescu E., Thermal properties of SiOC glasses and glass ceramics at elevated temperatures. Materials, 2018, 11(2): 279.

    ADS  Article  Google Scholar 

  2. [2]

    Duan X., Jia D., Deng J., Yang Z., Zhou Y., Mechanical and dielectric properties of gel casted Si3N4 porous ceramic using CaHPO4 as an additive. Ceramics International, 2012, 38(5): 4363–4367.

    Article  Google Scholar 

  3. [3]

    Duan C., Cui G., Xu X., Liu P., Sound absorption characteristics of a high-temperature sintering porous ceramic material. Applied Acoustics, 2012, 73(9): 865–871.

    Article  Google Scholar 

  4. [4]

    Pia G., Casnedi L., Ionta M., Sanna U., On the elastic deformation properties of porous ceramic materials obtained by pore-forming agent method. Ceramics International, 2015, 41(9): 11097–11105.

    Article  Google Scholar 

  5. [5]

    Kita H., Ohsumi K., Yamada T., Influence of composition and oxidation temperature on thermal-conductivity of Si-Ti-O-N porous ceramics. Journal of the Ceramic Society of Japan, 1993, 101(1172): 389–393.

    Article  Google Scholar 

  6. [6]

    Hu L., Wang C., Hu Z., Lu S., Sun C., Huang Yong., Porous yttria-stabilized zirconia ceramics with ultra-low thermal conductivity. Part II: Temperature dependence of thermophysical properties. Journal of Materials Science, 2011, 46(3): 623–628.

    ADS  Article  Google Scholar 

  7. [7]

    Li S., Wang C., Hu L., Improved heat insulation and mechanical properties of highly porous YSZ ceramics after silica aerogels impregnation. Journal of the American Ceramic Society, 2013, 96(10): 3223–3227.

    Article  Google Scholar 

  8. [8]

    Zhou J., Wang C., Porous yttria — stabilized zirconia ceramics fabricated by nonaqueous — based gel casting process with PMMA microsphere as pore — forming agent. Journal of the American Ceramic Society, 2013, 96(1): 266–271.

    Article  Google Scholar 

  9. [9]

    Latournerie J., Dempsey P., Hourlier-Bahloul D., Bonnet J.P., Silicon oxycarbide glasses: Part 1-thermochemical stability. Journal of the American Ceramic Society, 2006, 89(5): 1485–1491.

    Article  Google Scholar 

  10. [10]

    Halasova M., Chlup Z., Strachota A., Cerny M., Dlouhy I., Mechanical response of novel SiOC glasses to high temperature exposition. Journal of the European Ceramic Society, 2012, 32(16): 4489–4495.

    Article  Google Scholar 

  11. [11]

    Alonso R.P., Mariotto G., Gervais C., Babonneau F., Soraru G.D., New insights on the high-temperature nanostructure evolution of SiOC and B-doped SiBOC polymer-derived glasses. Chemistry of Materials, 2007, 19: 5694–5702.

    Article  Google Scholar 

  12. [12]

    Cahill D.G., Pohl R.O., Thermal conductivity of amorphous solids above the plateau. Physical Review B, 1987, 35(8): 4067–4073.

    ADS  Article  Google Scholar 

  13. [13]

    Borca-Tascius T., Kumar A.R., Chen G., Data reduction in 3ω method for thin-film thermal conductivity determination. Review of Scientific Instruments, 2001, 72(4): 2139–2147.

    ADS  Article  Google Scholar 

  14. [14]

    Qiu L., Tang D., Zheng X., Su G., The freestanding sensor-based 3ω technique for measuring thermal conductivity of solids: Principle and examination. Review of Scientific Instruments, 2011, 82(4): 045106.

    ADS  Article  Google Scholar 

  15. [15]

    Qiu L., Li Y., Zheng X., Zhu J., Tang D., Wu J., Xu C., Thermal-conductivity studies of macro-porous polymer-derived SiOC ceramics. International Journal of Thermophysics, 2014, 35(1): 76–89.

    ADS  Article  Google Scholar 

  16. [16]

    Xie T., He Y., Hu Z., Theoretical study on thermal conductivities of silica aerogel composite insulating material. International Journal of Heat Mass Transfer, 2013, 58: 540–552.

    Article  Google Scholar 

  17. [17]

    Kaganer M.G., Thermal insulation in cryogenic engineering. Israel Program for Scientific Translations, 1969.

  18. [18]

    Zeng S.Q., Hunt A., Greif R., Mean free path and apparent thermal conductivity of a gas in a porous medium. Journal of Heat Transfer-Transactions of the ASME, 1995, 117: 758–761.

    Article  Google Scholar 

  19. [19]

    Chen G., Nonlocal and nonequilibrium heat conduction in the vicinity of nanoparticles. Journal of Heat Transfer-Transactions of the ASME, 1996, 118: 539–545.

    Article  Google Scholar 

  20. [20]

    Zhao J.J., Duan Y.Y., Wang X.D., Wang B.X., Effects of solid-gas coupling and pore and particle microstructures on the effective gaseous thermal conductivity in aerogels. Journal of Nanoparticle Research, 2012, 14: 1–15.

    Google Scholar 

  21. [21]

    Wei G.S., Liu Y.S., Du X.Z., Zhang X.X., Gaseous conductivity study on silica aerogel and its composite insulation materials. Journal of Heat Transfer, 2012, 134(4): 041301.

    Article  Google Scholar 

  22. [22]

    Zeng S.Q., Hunt A., Greif R., Mean free path and apparent thermal conductivity of a gas in a porous medium. Journal of Heat Transfer, 1995, 117(3): 758–761.

    Article  Google Scholar 

Download references

Acknowledgements

This work is financially supported by Beijing Natural Science Foundation (3202020), National Natural Science Foundation of China (No. 51876008), Beijing Nova Program (Z201100006820065) and Interdisciplinary Research Project for Young Teachers of USTB (Fundamental Research Funds for the Central Universities) (FRF-IDRY-19-004). WU Jin acknowledges financial support from Guangdong Natural Science Funds Grant (2018A030313400).

Author information

Affiliations

Authors

Corresponding authors

Correspondence to Yanhui Feng or Jin Wu.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Qiu, L., Du, Y., Bai, Y. et al. Experimental Characterization and Model Verification of Thermal Conductivity from Mesoporous to Macroporous SiOC Ceramics. J. Therm. Sci. (2021). https://doi.org/10.1007/s11630-021-1422-7

Download citation

Keywords

  • SiOC ceramics
  • macroporous media
  • 3ω method
  • thermal conductivity