Work

A self-breathing electrode enabled by interface regulation and gradient wettability engineering for industrial H2O2 electrosynthesis

Year: 2026

Type: article

Abstract: The development of high-performance gas diffusion electrodes (GDEs) is critical for scalable and sustainable electrochemical H 2 O 2 production. However, conventional catalyst layers (CLs) suffer from catalyst encapsulation by fused polytetrafluoroethylene (PTFE) and disordered pore structures, forming a mass transport maze that restricts species diffusion and degrades three-phase interface (TPI) formation. Here, we introduce a non-fused particulate-packed catalyst/binder interface that forms discrete hydrophilic–hydrophobic domains and eliminates the insulating “PTFE armor”. Through 3D reconstruction and high-resolution lattice Boltzmann simulations, we identify that localized variations in wettability and pore structure critically govern electrolyte intrusion and sustaining effective TPIs. Inspired by these insights, we construct a gradient CL featuring hierarchical porosity and precisely tune wettability gradients. Multiscale simulations, in-situ breakthrough pressure measurements, and microfluidic experiments reveal that this gradient design enables directional electrolyte transport and propels H 2 O 2 away from CL, maintaining stable Faradaic efficiency (> 85%) at 300 mA cm − 2 over 300 hours. Moreover, we develop a commercialized scale-up 400 cm 2 four-unit flow-through cell stack integrated with thermal, fluidic, and electronic systems, capable of continuously producing H 2 O 2 at a low cost ($0.381 kg − 1 ) without external oxygen. We demonstrate that catalyst/binder interfaces govern microscale mass transport and TPI formation, with ordered porosity and wettability gradients synergistically boosting electrode performance. This work provides a fundamental design framework for next-generation GDEs and showcases a milestone demonstration of a breakthrough integrated self-breathing H 2 O 2 electrosynthesis system with compelling commercial viability.

Source: Nature Communications

DOI: 10.1038/s41467-026-68436-x