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

Abstract

Abstract The development of H 2 O 2 economy is hampered by the instability of liquid-state bulk H 2 O 2 solutions (2H 2 O 2  → 2H 2 O + O 2 ; ΔG° = −117 kJ mol −1 ). Comparatively, dispersing H 2 O 2 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 H 2 O 2 with productivity up to 0.943 mol L −1 h −1 . Notably, the as-fabricated solid-state H 2 O 2 features not only high H 2 O 2 gravimetric densities ( > 30 wt%) but also good stability for repeated H 2 O 2 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 H 2 O 2 molecules. The revelation that “stabilized H 2 O 2 ” can be manufactured under industrial conditions offers a path towards a sustainable H 2 O 2 production.