Acidity of Atmospheric Waters Induces Enhanced H2O2 Production through Photosensitized Chemistry of Phenolic Substances

IF 2.9 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

ACS Earth and Space Chemistry Pub Date : 2025-01-07 DOI:10.1021/acsearthspacechem.4c0031810.1021/acsearthspacechem.4c00318

Yingxin Xie, Qingxin Deng, Bowen He, Siyu Liu, Jiazhuo He, Yiqun Wang, Xue Li, Zhiqiang Yu, Hongwei Pang* and Sasho Gligorovski*,

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Abstract

Hydrogen peroxide (H₂O₂) is known to convert SO₂ to sulfuric acid and acts as a dominant reservoir of highly reactive hydroxyl radical (OH) in atmospheric waters (cloud, fog, rain, and aerosol liquid water). Here, we conclusively demonstrate that photosensitized oxidation of phenolic substances (catechol, o-cresol, and guaiacol) by the excited triplet state of nonphenolic compound (3,4-dimethoxybenzaldehyde, DMB) represents an unrecognized significant source of H₂O₂. Intriguingly, the highest H₂O₂ formation rate, (3.43 ± 0.14) × 10^–9 M s^–1, and H₂O₂ yield (Φ_H₂O₂), (7.68 ± 0.08) × 10^–1, were observed by photosensitized chemistry of catechol at low pH values (2.50) typical of cloud and aerosol water. The quantum chemical calculations revealed that the fraction of the protonated triplet state of DMB increases with a pH decrease, resulting in a faster formation of H₂O₂. A detailed mechanism was proposed describing the formation of H₂O₂ from the photosensitized reaction.

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来源期刊

ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology

CiteScore

5.30

自引率

11.80%

发文量

249

期刊介绍： The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.