Rapid synthesis of micron-thick flexible graphite films via non-equilibrium carbon flux engineering

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.