Laser solid-phase synthesis of graphene shell-encapsulated high-entropy alloy nanoparticles

Rapid synthesis of high-entropy alloy nanoparticles (HEA NPs) offers new opportunities to develop functional materials in widespread applications. Although some methods have successfully produced HEA NPs, these methods generally require rigorous conditions such as high pressure, high temperature, restricted atmosphere, and limited substrates, which impede practical viability. In this work, we report laser solid-phase synthesis of CrMnFeCoNi nanoparticles by laser irradiation of mixed metal precursors on a laser-induced graphene (LIG) support with a 3D porous structure. The CrMnFeCoNi nanoparticles are embraced by several graphene layers, forming graphene shell-encapsulated HEA nanoparticles. The mechanisms of the laser solid-phase synthesis of HEA NPs on LIG supports are investigated through theoretical simulation and experimental observations, in consideration of mixed metal precursor adsorption, thermal decomposition, reduction through electrons from laser-induced thermionic emission, and liquid beads splitting. The production rate reaches up to 30 g/h under the current laser setup. The laser-synthesized graphene shell-encapsulated CrMnFeCoNi NPs loaded on LIG-coated carbon paper are used directly as 3D binder-free integrated electrodes and exhibited excellent electrocatalytic activity towards oxygen evolution reaction with an overpotential of 293 mV at the current density of 10 mA/cm² and exceptional stability over 428 h in alkaline media, outperforming the commercial RuO₂ catalyst and the relevant catalysts reported by other methods. This work also demonstrates the versatility of this technique through the successful synthesis of CrMnFeCoNi oxide, sulfide, and phosphide nanoparticles.