Abstract
The large class of layered ceramics encompasses both van der Waals (vdW) and non-vdW solids. While intercalation of noble metals in vdW solids is known, formation of compounds by incorporation of noble-metal layers in non-vdW layered solids is largely unexplored. Here, we show formation of Ti3AuC2 and Ti3Au2C2 phases with up to 31% lattice swelling by a substitutional solid-state reaction of Au into Ti3SiC2 single-crystal thin films with simultaneous out-diffusion of Si. Ti3IrC2 is subsequently produced by a substitution reaction of Ir for Au in Ti3Au2C2. These phases form Ohmic electrical contacts to SiC and remain stable after 1,000 h of ageing at 600 °C in air. The present results, by combined analytical electron microscopy and ab initio calculations, open avenues for processing of noble-metal-containing layered ceramics that have not been synthesized from elemental sources, along with tunable properties such as stable electrical contacts for high-temperature power electronics or gas sensors.
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Acknowledgements
We acknowledge H. Pedersen for useful discussions about the results. We acknowledge the support from the VINN Excellence Center in research and innovation on Functional Nanoscale Materials (FunMat) by the Swedish Governmental Agency for Innovation Systems (VINNOVA) and the Swedish Government Strategic Research Areas in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU No. 2009 00971). P.E., J.L., M.D. and J.R. also acknowledge support from the Swedish Foundation for Strategic Research through the Future Research Leaders 5 Program and the Synergy Grant FUNCASE, Functional Carbides and Advanced Surface Engineering. I.A.A. is grateful for support provided by the e-Science Research Centre (SeRC). S.I.S. acknowledges Swedish Research Council (VR) Project No. 2014-4750. P.E. also acknowledges support from the European Research Council under the European Community’s Seventh Framework Programme (FP/2007-2013)/ERC grant agreement no. 335383. L.H. acknowledges the Knut and Alice Wallenberg Foundation for a Scholar Grant and support for the Linköping Ultra Electron Microscopy Laboratory. The calculations were performed on resources provided by the Swedish National Infrastructure for Computing (SNIC) at National Supercomputer Centre (NSC) and PDC.
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H.F., M.A., A.L.S. and P.E. conceived and initiated the work. H.F. conducted and analysed the growth, annealing, XRD and SEM. M.D. performed the ab initio studies with input from S.I.S., I.A.A., J.R., H.F. and P.E. J.L. conducted the STEM and EDX and analysed the results with contributions from H.F., L.H. and P.E. J.P. designed, executed, and interpreted the in situ annealing in TEM, and recorded the movie. H.F., M.D. and P.E. wrote the manuscript with contributions from the other coauthors. All coauthors read and commented on successive drafts of the manuscript. M.A., A.L.S. and P.E. supervised the work.
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Fashandi, H., Dahlqvist, M., Lu, J. et al. Synthesis of Ti3AuC2, Ti3Au2C2 and Ti3IrC2 by noble metal substitution reaction in Ti3SiC2 for high-temperature-stable Ohmic contacts to SiC. Nature Mater 16, 814–818 (2017). https://doi.org/10.1038/nmat4896
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DOI: https://doi.org/10.1038/nmat4896
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