Cooperative Repair for Laser-Induced Graphene via Modified Poly-phenylamine and Fe²⁺ for Thermal-Conductive Gels

Laser-induced graphene (LIG) has great potential for multiple applications because of its large specific surface area, facile fabrication process, and tunable properties. However, abundant lattice defects severely degrade its conductivity. Herein, from an innovative perspective of precursor design, the poly-phenylamines (P-PAs) with improved solubility and strong light absorption were synthesized, which act as an intercalated polymer for graphene oxide (GO) nanosheets. On this basis, the composite precursors show remarkably enhanced photothermal conversion capability and a compact stacked structure. These bring a 60% reduction in I_D/I_G in LIG after laser irradiation. To explain the above phenomenon, an isolation effect induced by the compact stacking precursor is proposed based on experimental results. Furthermore, the cooperative effect between P-PAs and Fe²⁺ is introduced, and a fluffy LIG aerogel with the lowest I_D/I_G ratio of 0.17 is prepared, which is barely achievable in conventional LIGs. When the obtained graphene aerogel is compounded with PDMS, the as-prepared thermal-conductive composite gel reaches a thermal conductivity of 1.05 W·m^-1·K^-1 and an ultralow interfacial thermal resistance of 37.2 mm²·K·W^-1 under a low graphene loading of 3.3 wt%. This intercalation strategy in GO precursor supplies a new route for preparing high-quality LIGs and thermal-conductive gels, which show great application prospects in thermal management devices.