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Molecularly Engineered Covalent Organic Frameworks for Hydrogen Peroxide Photosynthesis
Summary
Researchers developed a covalent organic framework photocatalyst for producing hydrogen peroxide from water and air using solar energy, achieving a solar-to-chemical conversion efficiency of up to 1.08%. The resulting hydrogen peroxide solution was capable of degrading pollutants. While not directly about microplastics, this research presents a potentially useful technology for environmental remediation including pollutant degradation in water systems.
Synthesizing H<sub>2</sub> O<sub>2</sub> from water and air via a photocatalytic approach is ideal for efficient production of this chemical at small-scale. However, the poor activity and selectivity of the 2 e<sup>-</sup> water oxidation reaction (WOR) greatly restricts the efficiency of photocatalytic H<sub>2</sub> O<sub>2</sub> production. Herein we prepare a bipyridine-based covalent organic framework photocatalyst (denoted as COF-TfpBpy) for H<sub>2</sub> O<sub>2</sub> production from water and air. The solar-to-chemical conversion (SCC) efficiency at 298 K and 333 K is 0.57 % and 1.08 %, respectively, which are higher than the current reported highest value. The resulting H<sub>2</sub> O<sub>2</sub> solution is capable of degrading pollutants. A mechanistic study revealed that the excellent photocatalytic activity of COF-TfpBpy is due to the protonation of bipyridine monomer, which promotes the rate-determining reaction (2 e<sup>-</sup> WOR) and then enhances Yeager-type oxygen adsorption to accelerate 2 e<sup>-</sup> one-step oxygen reduction. This work demonstrates, for the first time, the COF-catalyzed photosynthesis of H<sub>2</sub> O<sub>2</sub> from water and air; and paves the way for wastewater treatment using photocatalytic H<sub>2</sub> O<sub>2</sub> solution.
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