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A Detailed Reaction Mechanism for Thiosulfate Oxidation by Ozone in Aqueous Environments. | LitMetric

A Detailed Reaction Mechanism for Thiosulfate Oxidation by Ozone in Aqueous Environments.

Environ Sci Technol

Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.

Published: October 2024

AI Article Synopsis

Article Abstract

The ozone oxidation, or ozonation, of thiosulfate is an important reaction for wastewater processing, where it is used for remediation of mining effluents, and for studying aerosol chemistry, where its fast reaction rate makes it an excellent model reaction. Although thiosulfate ozonation has been studied since the 1950s, challenges remain in developing a realistic reaction mechanism that can satisfactorily account for all observed products with a sequence of elementary reaction steps. Here, we present novel measurements using trapped microdroplets to study the pH-dependent thiosulfate ozonation kinetics. We detect known products and intermediates, including SO, SO, SO, and SO, establishing agreement with the literature. However, we identify SO as a new reaction intermediate and find that the currently accepted mechanism does not directly explain observed pH effects. Thus, we develop a new mechanism, which incorporates SO as an intermediate and uses elementary steps to explain the pH dependence of thiosulfate ozonation. The proposed mechanism is tested using a kinetic model benchmarked to the experiments presented here, then compared to literature data. We demonstrate good agreement between the proposed thiosulfate ozonation mechanism and experiments, suggesting that the insights in this paper can be leveraged in wastewater treatment and in understanding potential climate impacts.

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Source
http://dx.doi.org/10.1021/acs.est.4c06188DOI Listing

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