A Covalent Organic Framework for Cooperative Water Oxidation

• DOI: 10.1021/jacs.2c07282
• Publication Date: 2022-09-15T23:58:28Z
• Authors: Suvendu Karak; Vladimir Stepanenko; Matthew A. Addicoat; Philipp Keßler; Simon Moser; Florian Beuerle; Frank Würthner
• Keywords: Covalent organic framework

The future of water-derived hydrogen as the "sustainable energy source" straightaway bets on success sluggish oxygen-generating half-reaction. endeavor to emulate natural photosystem II for efficient water oxidation has been extended across spectrum organic and inorganic combinations. However, achievement so far restricted homogeneous catalysts rather than their pristine heterogeneous forms. poor structural understanding control over mechanistic pathway often impede overall development. Herein, we have synthesized a highly crystalline covalent framework (COF) chemical photochemical oxidation. interpenetrated structure assures catalyst stability, catalyst's performance remains unaltered after several cycles. This COF exhibits highest ever accomplished catalytic activity such an organometallic solid-state material where rate oxygen evolution is high ∼26,000 μmol L–1 s–1 (second-order constant k ≈ 1650 L g–2). also proves its exceptional (k 1600 g–2) during light-driven under very dilute conditions. cooperative interaction between metal centers in network offers 20–30-fold superior well photocatalytic compared amorphous polymeric counterpart.