Abstract
This manuscript describes, defines, and discusses the process of cold sintering, which can consolidate a broad set of inorganic powders between room temperature and 300 °C using a standard uniaxial press and die. This temperature range is well below that needed for appreciable bulk diffusion, indicating immediately the distinction from the well-known and thermally driven analogue, allowing for an unconventional method for densifying these inorganic powders. Sections of this report highlight the general background and history of cold sintering, the current set of known compositions that exhibit compatibility with this process, the basic experimental techniques, the current understanding of physical mechanisms necessary for densification, and finally opportunities and challenges to expand the method more generically to other systems. The newness of this approach and the potential for revolutionary impact on traditional methods of powder-based processing warrants this discussion despite a nascent understanding of the operative mechanisms.
Similar content being viewed by others
References
M.N. Rahaman: Sintering of Ceramics (CRC Press, Baca Raton, 2008).
R.M. German: Sintering Theory and Practice (Wiley, New York City, 1996).
S-J.L. Kang: Sintering: Densification, Grain Growth, and Microstructure (Butterworth-Heinemann, Oxford, 2005).
M. Cologna, B. Rashkova, and R. Raj: Flash sintering of nanograin zirconia in <5 s at 850 °C. J. Am. Ceram. Soc. 93(11), 3556 (2010).
Z. Shen, Z. Zhao, H. Peng, and M. Nygren: Formation of tough interlocking microstructures in silicon nitride ceramics by dynamic ripening. Nature 417, 266 (2002).
R. Chaim, A. Shlayer, and C. Estournes: Densification of nanocrystalline Y2O3 ceramic powder by spark plasma sintering. J. Eur. Ceram. Soc. 29(1), 91 (2009).
Z. Valdez-Nava, S. Guillemet-Fritsch, C. Tenailleau, T. Lebey, B. Durand, and J.Y. Chane-Ching: Colossal dielectric permittivity of BaTiO3-based nanocrystalline ceramics sintered by spark plasma sintering. J. Electroceram. 22(1–3), 238 (2009).
C. Elissalde, M. Maglione, and C. Estournes: Tailoring dielectric properties of multilayer composites using spark plasma sintering. J. Am. Ceram. Soc. 90(3), 973 (2007).
N. Shomrat, S. Baltianski, C.A. Randall, and Y. Tsur: Flash sintering of potassium-niobate. J. Eur. Ceram. Soc. 35(7), 2209 (2015).
Z. Zhao, V. Buscaglia, P. Bowen, and M. Nygren: Spark plasma sintering of nano-crystalline ceramics. Key Eng. Mater. 264–268, 2297 (2004).
N. Yamasaki, K. Yanagisawa, M. Nishioka, and S. Kanahara: A hydrothermal hot-pressing method: Apparatus and application. J. Mater. Sci. Lett. 5, 355 (1986).
J. Guo, H. Guo, A.L. Baker, M.T. Lanagan, E.R. Kupp, G.L. Messing, and C.A. Randall: Cold sintering: A paradigm shift for processing and integration of ceramics. Angew. Chem., Int. Ed. 55(38), 11457 (2016).
H. Guo, A. Baker, J. Guo, C.A. Randall, and D. Johnson: Cold sintering process: A novel technique for low-temperature ceramic processing of ferroelectrics. J. Am. Ceram. Soc. 99(11), 3489 (2016).
H. Guo, A. Baker, J. Guo, and C.A. Randall: Protocol for ultralow-temperature ceramic sintering: An integration of nanotechnology and the cold sintering process. ACS Nano 10(11), 10606 (2016).
H. Guo, J. Guo, A. Baker, and C.A. Randall: Hydrothermal-assisted cold sintering process: A new guidance for low-temperature ceramic sintering. ACS Appl. Mater. Interfaces 8(32), 20909 (2016).
A. Baker, H. Guo, J. Guo, and C. Randall: Utilizing the cold sintering process for flexible-printable electroceramic device fabrication. J. Am. Ceram. Soc. 99(10), 3202 (2016).
J. Guo, A.L. Baker, H. Guo, M. Lanagan, and C.A. Randall: Cold sintering process: A new era for ceramic packaging and microwave device development. J. Am. Ceram. Soc. 7, 1 (2016).
J. Guo, H. Guo, D.S.B. Heidary, S. Funahashi, and C.A. Randall: Semiconducting properties of cold sintered V2O5 ceramics and Co-sintered V2O5-PEDOT: PSS composites. J. Eur. Ceram. Soc. 37(4), 1529 (2016).
J. Guo, S.S. Berbano, H. Guo, A.L. Baker, M.T. Lanagan, and C.A. Randall: Cold sintering process of composites: Bridging the processing temperature gap of ceramic and polymer materials. Adv. Funct. Mater. 26(39), 7115 (2016).
H. Guo, J. Guo, A. Baker, and C.A. Randall: Cold sintering process for ZrO2-based ceramics: Significantly enhanced densification evolution in yttria-doped ZrO2. J. Am. Ceram. Soc. 100(2), 491 (2016).
H. Guo, T.J.M. Bayer, J. Guo, A. Baker, and C.A. Randall: Cold sintering process for 8 mol% Y2O3-stabilized ZrO2 ceramics. J. Eur. Ceram. Soc. 37(5), 2303 (2017).
H. Kähäri, M. Teirikangas, J. Juuti, and H. Jantunen: Dielectric properties of lithium molybdate ceramic fabricated at room temperature. J. Am. Ceram. Soc. 97(11), 3378 (2014).
H. Kähäri, M. Teirikangas, J. Juuti, and H. Jantunen: Improvements and modifications to room-temperature fabrication method for dielectric Li2MoO4 ceramics. J. Am. Ceram. Soc. 98(3), 687 (2015).
H. Kähäri, M. Teirikangas, J. Juuti, and H. Jantunen: Room-temperature fabrication of microwave dielectric Li2MoO4–TiO2 composite ceramics. Ceram. Int. 42(9), 11442 (2016).
C.A. Randall, J. Guo, H. Guo, A. Baker, and M.T. Lanagan (The Penn State Research Foundation, assignee): Cold Sintering Ceramics and Composites. U.S. Provisional Patent Service Number 62/234 (2015).
S. Funahashi, J. Guo, H. Guo, K. Wang, A.L. Baker, K. Shiratsuyu, and C.A. Randall: Demonstration of the cold sintering process study for the densification and grain growth of ZnO ceramics. J. Am. Ceram. Soc. 100(2), 546 (2017).
S.S. Berbano, J. Guo, H. Guo, M.T. Lanagan, and C.A. Randall: Cold sintering process of Li1.5Al0.5Ge1.5(PO4)3 solid electrolyte. J. Am. Ceram. Soc., 100(5), 2123 (2017).
I.J. Induja and M.T. Sebastian: Microwave dielectric properties of mineral sillimanite obtained by conventional and cold sintering process. J. Eur. Ceram. Soc. 37(5), 2143 (2017).
P. De Silva, L. Bucea, V. Sirivivatnanon, and D.R. Moorehead: Carbonate binders by “cold sintering” of calcium carbonate. J. Mater. Sci. 42(16), 6792 (2007).
N. Yamasaki, W. Tang, and J. Ke: Low-temperature sintering of calcium carbonate by a hydrothermal hot-pressing technique. J. Mater. Sci. Lett. 11(13), 934 (1992).
K. Yanagisawa, K. Ioku, and N. Yamasaki: Formation of anatase porous ceramics by hydrothermal hot-pressing of amorphous titania spheres. J. Am. Ceram. Soc. 80(5), 1303 (1997).
K. Yanagisawa, K. Ioku, and N. Yamasaki: Pore size control of porous silica ceramics by hydrothermal hot-pressing. J. Ceram. Soc. Jpn. 102(1190), 966 (1994).
Y. Xie, S. Yin, H. Yamane, T. Hashimoto, and T. Sato: Low temperature sintering and color of a new compound Sn1.24Ti1.94O3.66(OH)1.50F1.42. Solid State Sci. 11(9), 1703 (2009).
F. Bouville and A.R. Studart: Geologically-inspired strong bulk ceramics made with water at room temperature. Nat. Commun. 8, 14655 (2017).
I.J. Clark, T. Takeuchi, N. Ohtori, and D.C. Sinclair: Hydrothermal synthesis and characterisation of perovskite. J. Mater. Chem. 9(1), 83 (1999).
M.Z.C. Hu, V. Kurian, E.A. Payzant, C.J. Rawn, and R.D. Hunt: Wet-chemical synthesis of monodispersed barium titanate particles—Hydrothermal conversion of TiO2 microspheres to nanocrystalline BaTiO3. Powder Technol. 110(1–2), 2 (2000).
P.K. Dutta, R. Asiaie, S.A. Akbar, and W. Zhu: Hydrothermal synthesis and dielectric properties of tetragonal BaTiO3. Chem. Mater. 6(9), 1542 (1994).
M. Yoshimura, S-E. Yoo, M. Hayashi, and N. Ishizawa: Preparation of BaTiO3 thin film by hydrothermal electrochemical method. Jpn. J. Appl. Phys. 28(11), 2007 (1989).
H. Akyıldız, M. Casper, S. Aygün, P. Lam, and J. Maria: Hydrothermal BaTiO3 thin films from nanostructure Ti templates. J. Mater. Res. 26(4), 592 (2011).
C. Vakifahmetoglu, J.F. Anger, V. Atakan, S. Quinn, S. Gupta, Q. Li, L. Tang, and R.E. Riman: Reactive hydrothermal liquid-phase densification (rHLPD) of ceramics—A study of the BaTiO3[TiO2] composite system. J. Am. Ceram. Soc. 99, 3893 (2016).
S-I. Hirano and S. Somiya: Hydrothermal reaction sintering of pure Cr2O3. J. Am. Ceram. Soc. 59(11–12), 534 (1976).
K. Anagisawa, M. Sasaki, M. Nishioka, K. Ioku, and N. Yamasaki: Preparation of sintered compacts of anatase by hydrothermal hot-pressing. J. Mater. Sci. Lett. 13, 765 (1994).
B. Dargatz, J. Gonzalez-Julian, M. Bram, P. Jakes, A. Besmehn, L. Schade, R. Röder, C. Ronning, and O. Guillon: FAST/SPS sintering of nanocrystalline zinc oxide-part I: Enhanced densification and formation of hydrogen-related defects in presence of adsorbed water. J. Eur. Ceram. Soc. 36(5), 1207 (2016).
W.M. Haynes: CRC Handbook of Chemistry and Physics, 97th ed. (CRC Press, Boca Raton, 2016).
R.A. Van Santen: The Ostwald step rule. J. Phys. Chem. 88(6), 5768 (1984).
D. Velegol, A. Garg, R. Guha, A. Kar, and M. Kumar: Origins of concentration gradients for diffusiophoresis. Soft Matter 12(21), 4686 (2016).
T. Senda and R.C. Bradt. Grain growth in sintered ZnO and ZnO–Bi2O3 ceramics. J. Am. Ceram. Soc. 1, 106 (1990).
P.B. Vandiver, O. Soffer, B. Klima, J. Svoboda, P.B. Vandiver, O. Soffer, B. Klima, and J. Svoboda: The origins of ceramic technology at dolni věstonice, czechoslovakia. Science 246(4933), 1002 (2017).
ACKNOWLEDGMENTS
The authors acknowledge support from The Center for Dielectrics and Piezoelectrics, a national research center and consortium under the auspices of the Industry/University Cooperative Research Centers program at the National Science Foundation under Grant Nos. IIP-1361571 and 1361503. The authors thank Professor James LeBeau and Matt Cabral for TEM imaging of cold sintered ceramics. This work was performed in part at the Analytical Instrumentation Facility (AIF) at North Carolina State University, which is supported by the State of North Carolina and the National Science Foundation (award number ECCS-1542015). The AIF is a member of the North Carolina Research Triangle Nanotechnology Network (RTNN), a site in the National Nanotechnology Coordinated Infrastructure (NNCI). We also thank the visiting scientist support from Murata Electronics, and also the Materials Characterization Laboratory, at the Materials Research Institute at PSU. This material is based upon work supported by the National Science Foundation Graduate Research Fellowship Program under Grant No. DGE-1252376. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Maria, JP., Kang, X., Floyd, R.D. et al. Cold sintering: Current status and prospects. Journal of Materials Research 32, 3205–3218 (2017). https://doi.org/10.1557/jmr.2017.262
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1557/jmr.2017.262