工業用H₂O₂電解合成のための界面制御と勾配濡れ性工学によって実現された自己呼吸電極

High-performance gas diffusion electrodes (GDEs) are essential for electrochemical H₂O₂ production, yet conventional catalyst layers (CLs) suffer from PTFE-fused encapsulation and disordered pores that create mass-transport bottlenecks and suppress three-phase interface (TPI) formation. Here, we introduce a non-fused particulate-packed catalyst/binder interface and elucidate the mechanisms governing TPI formation through 3D reconstruction and mesoscale LBM analyses. Guided by these insights, we construct a hierarchical gradient CL with ordered porosity and tunable wettability contrast, and multiscale simulations together with in-situ breakthrough and microfluidic experiments confirm capillarity-driven electrolyte displacement and directional self-transport of H₂O₂, enabling stable Faradaic efficiencies >85% at 300 mA cm^-2 for 300 h. We further develop a 400 cm² four-unit self-breathing flow-through stack integrating thermal, fluidic, and electronic systems for continuous, oxygen-free, low-cost H₂O₂ generation. This work offers a fundamental design framework for advanced GDEs and demonstrates a milestone integrated self-breathing H₂O₂ electrosynthesis system with commercial viability.