Squaric acid-based zwitterionic covalent organic framework induces triple synergy for boosted hydrogen peroxide photosynthesis.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41062494.
- Also identified by DOI 10.1038/s41467-025-63997-9 and PMC identifier 12508133.
- Licence recorded as CC BY-NC-ND.
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Abstract
Photocatalytic oxygen reduction reaction offers a sustainable approach for hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) synthesis, while the efficiency is limited by the challenge of synergistically optimizing the supply of oxygen, protons, and electrons. Here, by elaborately developing squaric acid-based zwitterionic covalent organic framework (STT COF), we propose a triple synergy strategy for boosting H<sub>2</sub>O<sub>2</sub> photosynthesis. The as-prepared STT COF delivers a high H<sub>2</sub>O<sub>2</sub> yield of 14356.5 μmol g<sup>-1</sup> h<sup>-1</sup> in pure water, with a notable apparent quantum yield of 40.0% at 420 nm, roughly 7.9 times that of its charge-neutral counterpart and outperforming other documented systems. Under natural sunlight irradiation, a 5 L H<sub>2</sub>O<sub>2</sub> solution (~400 μM) is produced in a continuous flow membrane reactor equipped with STT COF and gas diffusion layers. Mechanism studies demonstrate that STT COF induces a strong donor-acceptor (D-A) interaction to promote electron transfer, undergoes spontaneous hydrogenation for continuous protons and facilitating oxygen uptake in a favorable configuration, collectively creating a triple synergy to boost H<sub>2</sub>O<sub>2</sub> photosynthesis.