Nanoengineering of Porous 2D Structures with Tunable Fluid Transport Behavior for Exceptional H₂O₂ Electrosynthesis

Precision nanoengineering of porous two-dimensional structures has emerged as a promising avenue for finely tuning catalytic reactions. However, understanding the pore-structure-dependent catalytic performance remains challenging, given the lack of comprehensive guidelines, appropriate material models, and precise synthesis strategies. Here, we propose the optimization of two-dimensional carbon materials through the utilization of mesopores with 5-10 nm diameter to facilitate fluid acceleration, guided by finite element simulations. As proof of concept, the optimized mesoporous carbon nanosheet sample exhibited exceptional electrocatalytic performance, demonstrating high selectivity (>95%) and a notable diffusion-limiting disk current density of -3.1 mA cm^-2 for H₂O₂ production. Impressively, the electrolysis process in the flow cell achieved a production rate of 14.39 mol g_catalyst^-1 h^-1 to yield a medical-grade disinfectant-worthy H₂O₂ solution. Our pore engineering research focuses on modulating oxygen reduction reaction activity and selectivity by affecting local fluid transport behavior, providing insights into the mesoscale catalytic mechanism.