Unique production strategy of Pt/C electrocatalysts via pulsed laser for hydrogen generation: Insights screening by DFT calculations

Design and optimizing the components and structure of highly-active electrocatalysts is a prevalent approach for reducing the input electrical energy consumption and concurrently H2 fuel production. An efficient and sustainable method is a water-electrolyzer for H2 generation, but still restricted by the stable electrode materials. In this study, a green chemistry approach for one-pot production of Pt/C nanospherical with controllable ratios of Pt and C was demonstrated using simple pulsed laser ablation in liquid (PLAL) process, during which Pt target ablation in diverse solvents (water, methanol, ethanol, and 1-propanol) without external carbon source and reducing/capping agents. The carbon-rich solvents are acted as both C-source and solvent, which are decomposed during the PLA process, producing C, H, and OH ions inside the cavitation bubble which condenses as C-shells on the Pt surface. The optimal Pt/C proportions have the highest electrochemical H2-evolution in acidic media with an overpotential of 59 mV at 10 mA/cm2, Tafel slope of 41 mV/dec, and j0 of 0.686 mA/cm2. The exceptional electrocatalytic concert of optimal Pt/C was further supported by the density functional theory. Optimized C-content in Pt/C reveals good dispersion and strong interaction of C with Pt can make efficient electron transfer, structural stability, and electrochemical durability, resulting in superior electrocatalytic performance in electrolyzer devices.