Journal
ACS CATALYSIS
Volume 12, Issue 24, Pages 14911-14917Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c03878
Keywords
covalent organic frameworks; photocatalysis; water oxidation; hydration
Categories
Funding
- National Key Research and Development Program of China
- National Natural Science Foundation of China
- [2020YFA0710303]
- [52172188]
- [U1905215]
- [52072076]
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A hydration-initiated pathway of photocatalytic water oxidation over covalent organic frameworks (COFs) is proposed, where the hydration of water addition to the hydrazone unit efficiently induces the initial step of photocatalytic water oxidation. The subsequent oxidative deprotonation and the coupling of the bonded hydroxyl radicals selectively yield H2O2. This study provides a mechanistic insight into water oxidation over COFs.
A hydration-initiated pathway of photocatalytic water oxidation over covalent organic frameworks (COFs) is proposed. The hydration of water addition to the hydrazone unit of hydrophilic COF efficiently induces the initial step of photocatalytic water oxidation. The subsequent oxidative deprotonation and the coupling of the bonded hydroxyl radicals selectively yield H2O2. Oxidative deprotonation is identified as the rate-determining step, which can be facilitated by electron and proton capture. An excellent H2O2 production rate of 1.0 mmol g-1 h-1 was achieved in pure water under atmospheric conditions. This study provides a mechanistic insight into water oxidation over COFs.
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