Cold sintering with dimethyl sulfoxide solutions for metal oxides
Abstract
Cold sintering of ZnO and MnO with dimethyl sulfoxide (DMSO)-based solutions is demonstrated. For ZnO ceramics, density values approach 99% theoretical when cold-sintered at 180 °C with DMSO-HOAc and DMSO-Zn(OAc)2 solutions. MnO densified with aqueous HOAc solutions produces ceramics of 84% theoretical density that contain significant amounts of Mn(OH)2 secondary phases. In comparison, using DMSO-HOAc solutions produces density values of 94% theoretical at 250 °C with trace quantities of Mn3O4, verified via X-ray diffraction. Scanning electron microscope analysis of sample fracture surfaces containing Mn3O4 reveals numerous crystallites smaller than 100 nm that nucleate on or between the considerably larger starting MnO grains. With increasing temperature, these precipitates appear to coalesce and fill the porosity that remains after initial compaction. These results identify an avenue to cold sinter metal oxides that, in the presence of aqueous media, favor hydroxide formation which inhibits further densification.
Notes
Acknowledgements
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). 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 would like to acknowledge the use of the Huck Institutes of the Life Sciences’ Microscopy and Cytometry Facility. This material is based upon work supported by the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1746939. Any opinion, findings, and conclusions or recommendations expressed in this material are those of the authors(s) and do not necessarily reflect the views of the National Science Foundation.
Compliance with ethical standards
Conflict of interest
The authors are unaware of any conflicts of interest regarding the data and findings presented in this manuscript.
References
- 1.Herisson de Beauvoir T, Sangregorio A, Cornu I et al (2018) Cool-SPS: an opportunity for low temperature sintering of thermodynamically fragile materials. J Mater Chem C 6:2229–2233CrossRefGoogle Scholar
- 2.Dargatz B, Gonzalez-Julian J, Bram M et al (2016) 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 36:1207–1220CrossRefGoogle Scholar
- 3.Dargatz B, Gonzalez-Julian J, Bram M et al (2016) FAST/SPS sintering of nanocrystalline zinc oxide-Part II: abnormal grain growth, texture and grain anisotropy. J Eur Ceram Soc 36:1221–1232. https://doi.org/10.1016/j.jeurceramsoc.2015.12.008 CrossRefGoogle Scholar
- 4.Maria JP, Kang X, Floyd RD et al (2017) Cold sintering: current status and prospects. J Mater Res 32:3205–3218CrossRefGoogle Scholar
- 5.Guo J, Floyd R, Lowum S et al (2019) Cold sintering: progress, challenges and future opportunities. Annu Rev Mater Res 49Google Scholar
- 6.Yamasaki N, Yanagisawa K, Nishioka M, Kanahara S (1986) A hydrothermal hot-pressing method: apparatus and application. J Mater Sci Lett 5:355–356CrossRefGoogle Scholar
- 7.Yamasaki N, Weiping T, Jiajun K, Hosoi K (1995) Low-temperature sintering of calcium and magnesium carbonate by the hydrothermal hot-pressing technique. J Mater Sci Lett 14:1268–1270CrossRefGoogle Scholar
- 8.Goglio G, Ndayishimiye A, Largeteau A, Elissalde C (2019) View point on hydrothermal sintering: main features, today’s recent advances and tomorrow’s promises. Scr Mater 158:146–152CrossRefGoogle Scholar
- 9.Kähäri H, Teirikangas M, Juuti J, Jantunen H (2014) Dielectric properties of lithium molybdate ceramic fabricated at room temperature. J Am Ceram Soc 97:3378–3379CrossRefGoogle Scholar
- 10.Kähäri H, Teirikangas M, Juuti J, Jantunen H (2015) Improvements and modifications to room-temperature fabrication method for dielectric Li2MoO4 ceramics. J Am Ceram Soc 98:687–689CrossRefGoogle Scholar
- 11.Guo J, Guo H, Baker AL et al (2016) Cold sintering: a paradigm shift for processing and integration of ceramics. Angew Chem Int Ed 55:11457–11461CrossRefGoogle Scholar
- 12.Guo H, Baker A, Guo J, Randall CA (2016) Cold sintering process: a novel technique for low-temperature ceramic processing of ferroelectrics. J Am Ceram Soc 99:3489–3507CrossRefGoogle Scholar
- 13.Guo H, Baker A, Guo J, Randall CA (2016) Protocol for ultralow-temperature ceramic sintering: an integration of nanotechnology and the cold sintering process. ACS Nano 10:10606–10614CrossRefGoogle Scholar
- 14.Funahashi S, Guo J, Guo H et al (2017) Demonstration of the cold sintering process study for the densification and grain growth of ZnO ceramics. J Am Ceram Soc 100:546–553CrossRefGoogle Scholar
- 15.Guo H, Guo J, Baker A, Randall CA (2016) Hydrothermal-assisted cold sintering process: a new guidance for low-temperature ceramic sintering. ACS Appl Mater Interfaces 8:20909–20915CrossRefGoogle Scholar
- 16.Kang X, Floyd R, Lowum S et al (2019) Mechanism studies of hydrothermal cold sintering of zinc oxide at near room temperature. J Am Ceram Soc. https://doi.org/10.1111/jace.16340 Google Scholar
- 17.Kang X (2017) Hydrothermal cold sintering. Thesis. North Carolina State University RepositoryGoogle Scholar
- 18.Pourbaix M (1966) Atlas of electrochemical equilibria in aqueous solution, 1st edn. Pergamon Press, OxfordGoogle Scholar
- 19.Oswald HR, Asper R (1977) Bivalent metal hydroxides. In: Lieth RMA (ed) Preparation and crystal growth of materials with layered structures. D. Reidel Publishing Company, Dordrecht, pp 71–140CrossRefGoogle Scholar
- 20.Roy DM (1987) New strong cement materials: chemically bonded ceramics. Am Assoc Adv Sci 235:651–658Google Scholar
- 21.Mohamed MA, Halawy SA (1994) Kinetic and mechanistic study of the non-isothermal decomposition of manganese(II) acetate tetrahydrate. Thermochim Acta 242:173–186CrossRefGoogle Scholar
- 22.Kanzaki M (1991) Dehydration of brucite (Mg(OH)2) at high pressures detected by differential thermal analysis. Geophys Res Lett 18:2189–2192CrossRefGoogle Scholar
- 23.Blank DA, North SW, Stranges D et al (1997) Unraveling the dissociation of dimethyl sulfoxide following absorption at 193 nm. J Chem Phys 106:539–550CrossRefGoogle Scholar
- 24.Head DL, McCarty CG (1973) The thermal decomposition of DMSO. Tetrahedron Lett 16:1405–1408CrossRefGoogle Scholar
- 25.Hem JD (1963) Chemical equilibria and rates of manganese oxidation. United States Department of the Interior, Washington, DCGoogle Scholar
- 26.Kingery WD, Woulbroun JM, Charvat FR (1963) Effects of applied pressure on densification during sintering in the presence of a liquid phase. J Am Ceram Soc 46:391–395CrossRefGoogle Scholar
- 27.Coble RL (1970) Diffusion models for hot pressing with surface energy and pressure effects as driving forces. J Appl Phys 41:4798–4807CrossRefGoogle Scholar
- 28.Martens WN, Frost RL, Kristof J, Theo Kloprogge J (2002) Raman spectroscopy of dimethyl sulphoxide and deuterated dimethyl sulphoxide at 298 and 77 K. J Raman Spectrosc 33:84–91CrossRefGoogle Scholar