Electronic structure blurring-mediated solid-state H2O2 electrosynthesis with high productivity.
Yuxiang Zhang, Jingjing Duan, Markus Antonietti, Sheng Chen
Abstract
Open AccessThe 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.