Abstract
The scalable synthesis of high-quality graphite materials remains a formidable challenge due to the inherent trade-off between crystalline perfection and manufacturing efficiency. Existing forms of graphite, such as highly oriented pyrolytic graphite (HOPG) and Kish graphite, suffer from sluggish pyrolytic processes, limited carbon diffusion rates and energy-intensive protocols, often requiring several days for production. Here, we report a pulsed Joule heating-induced carburization (PJHIC) strategy that exploits transient non-equilibrium states to enable rapid carbon diffusion and segregation in metal substrates. By applying instantaneous thermal shocks ( > 1300 °C, > 300 °C/s heating rate) to solid carbon precursor-coated nickel and cobalt foils, we demonstrate the rapid carbon transport in bulk metals and achieve a vertical graphite growth rate of 730 nm/min, which is an order of magnitude faster than conventional methods. Cyclic temperature pulses further enable the synthesis of 1–5 μm-thick ABA-stacked graphite films with millimeter-scale grain sizes. The resulting rapid epitaxially grown graphite films exhibit a highly ordered crystalline structure and exceptional thermal conductivity (1314 W m–1 K–1), comparable to high-quality HOPG and Kish graphite. This work establishes a non-equilibrium synthesis paradigm for high-quality layered materials, bridging atomic-scale precision with industrial-scale manufacturing.
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Acknowledgements
This work was supported by the National Natural Science Foundation of China (No. T2188101 to Z.F. Liu and L.S.), Beijing Natural Science Foundation (No. 2264127 to L.S.), Shenzhen Science and Technology Program (Nos. RCYX20200714114643187 and WDZC20200821100123001 to B.S.), Guangdong Special Support Program (No. 2023TQ07A273 to B.S.), the CAS Project for Young Scientists in Basic Research (No. YSBR-003 to W.Z.), the Electron Microscopy Center at the University of Chinese Academy of Sciences (to W.Z.), and the Youth Innovation Promotion Association of CAS (No. 2022038 to M.X. Liu) and the CAS Project for Young Scientists in Basic Research (No. YSBR-054 to M.X. Liu).
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Z.F.Liu and L.S. supervised and convinced the project. L.S., H.L., and Z.W. designed the experiments and constructed the fast segregation model. H.L., Z.W., X.W., and J.C. carried out the synthesis and characterization of samples. H.L., Z.W., X.W., and L.S. analyzed the data and plotted the figures. X.H. and B.S. performed the TDTR thermal-conductivity experiments and the data analysis. L.L. and W.Z. conducted the ADF-STEM characterization and data analysis. Mengyuan Liu and Mengxi Liu conducted STM characterization and data analysis. X.Z. and Z.Y. Li helped with the two-stage model for the non-equilibrium segregation process. Q.C., Q.Z., J.D., C.W., and S.Z. helped with the figure plot, carbon diffusion model analysis and data statistics. X.W. and L.S. wrote the paper. All authors discussed the results and commented on the manuscript.
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Liu, H., Wang, Z., Wang, X. et al. Rapid synthesis of micron-thick flexible graphite films via non-equilibrium carbon flux engineering. Nat Commun (2026). https://doi.org/10.1038/s41467-026-70028-8
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DOI: https://doi.org/10.1038/s41467-026-70028-8
