Large Area Millisecond Preparation of High-Quality, Few-Layer Graphene Films on Arbitrary Substrates via Xenon Flash Lamp Photothermal Pyrolysis and Their Application for High-Performance Micro-supercapacitors

We report a method for fast, efficient, and scalable preparation of high-quality, large area, few-layer graphene films on arbitrary substrates via high-intensity pulsed xenon flash lamp photothermal pyrolysis of thin precursor films at ambient conditions in millisecond time frames. The precursors comprised poly(2,2-bis(3,4-dihydro-3-phenyl-1,3-benzoxazine)), and cyclized polyacrylonitrile and possess significant absorption cross section within the bandwidth of the emission spectrum of a xenon flash lamp. By localizing light absorption to the precursor films, the process enabled the preparation of few-layer graphene films on any substrate, including thermally sensitive substrates without the need for any catalytic substrate as in chemical vapor deposition-based approaches or conductive electrodes as in electrochemical method-based approaches. The extent of conversion of the precursor films to graphene was strongly dependent on pulse energy and the local temperature achieved due to photothermal effect, which were controlled via pulse power modulation; it also depended on structural properties of the precursor and to a lesser extent on the substrate. The cPAN showed a higher efficiency for conversion to graphene, as confirmed by Raman spectra (I_D/I_G ∼ 0.3), and sheet resistance of 0.1 Ω cm. To demonstrate the utility of the process, graphene film electrodes prepared photothermally on carbon fiber current collector were used for the fabrication of micro-supercapacitors with a very high areal supercapacitance of 3.5 mF/cm². Subsequent deposition of manganese oxide onto the fabricated electrodes significantly increased the energy storage capability of the supercapacitor, yielding a device with exceptionally high capacitance of 80 F/g at 1 mA current, good rate capability, and long cycle life.