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 gcatalyst–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.