Electronic structure blurring-mediated solid-state H₂O₂ electrosynthesis with high productivity.

Abstract

The development of H₂O₂ economy is hampered by the instability of liquid-state bulk H₂O₂ solutions (2H₂O₂ → 2H₂O + O₂; ΔG° = -117 kJ mol^-1). Comparatively, dispersing H₂O₂ molecules in solid-state materials would offer good physical stability with less of handling, leak and exposure risks, but suffers from fabrication schemes irrelevant to commercial applications. Mediated by the concept of electronic structure blurring, here we elaborate one-step electrosynthesis of solid-state H₂O₂ with productivity up to 0.943 mol L^-1 h^-1. Notably, the as-fabricated solid-state H₂O₂ features not only high H₂O₂ gravimetric densities ( > 30 wt%) but also good stability for repeated H₂O₂ loading/deloading over 100 cycles and shelf life over 160 days. Mechanism study underscores the electronic structure blurring formed at local catalytic environments that contributes to homogenizing charge distributions of H-O and O-O bondings (charge transfer of 0.67 and 0.22 e), and thereby inhibiting the break of these bonds inside H₂O₂ molecules. The revelation that "stabilized H₂O₂" can be manufactured under industrial conditions offers a path towards a sustainable H₂O₂ production.