The overlooked carbonate radical in micropollutant degradation: An insight into hydration interaction

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F46747885%3A24620%2F23%3A00011236" target="_blank" >RIV/46747885:24620/23:00011236 - isvavai.cz</a>

Výsledek na webu

<a href="https://www.sciencedirect.com/science/article/pii/S1385894723039761" target="_blank" >https://www.sciencedirect.com/science/article/pii/S1385894723039761</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.cej.2023.145245" target="_blank" >10.1016/j.cej.2023.145245</a>

Jazyk výsledku

angličtina

Název v původním jazyce

The overlooked carbonate radical in micropollutant degradation: An insight into hydration interaction

Popis výsledku v původním jazyce

Carbonate radical (CO3∙-) is an abundant reactive oxygen species in sunlit surface waters and radical-based treatment systems. The roles of this kosmotropic radical in these aquatic systems have been often overlooked presumably due to its low redox potential and ambiguous solvation mechanism. In this study, CO3∙--mediated oxidation of a frequently detected micropollutant, ibuprofen, was investigated. The results showed that the H-atom abstraction (HAA) pathway dominated the degradation processes regardless of the protonation state. However, without explicitly considering the solvent molecules, the calculated reaction rate constant (k, 1.09 × 107 M−1 s−1) was overestimated by an order of magnitude. With the explicit inclusion of the hydration shell, the calculated k value (5.26 × 105 M−1 s−1) agreed well with the measured one (7.89 × 105 M−1 s−1). Considerable charge transfer was found from the CO3 center to the solvation shells. In addition, the contour plot of CO3∙- contribution to overall elimination of various micropollutants was also constructed. The surface with the contribution greater than 10% includes many micropollutants with electron-rich groups such as thioethers, anilines and phenolates, demonstrating that the role of CO3∙- cannot be overlooked in most sunlit surface waters. These results yield mechanistic insights to the CO3∙--mediated degradation of micropollutants, providing practical guidance for their removal in both natural water systems and engineered water treatment processes.

Název v anglickém jazyce

The overlooked carbonate radical in micropollutant degradation: An insight into hydration interaction

Popis výsledku anglicky

Carbonate radical (CO3∙-) is an abundant reactive oxygen species in sunlit surface waters and radical-based treatment systems. The roles of this kosmotropic radical in these aquatic systems have been often overlooked presumably due to its low redox potential and ambiguous solvation mechanism. In this study, CO3∙--mediated oxidation of a frequently detected micropollutant, ibuprofen, was investigated. The results showed that the H-atom abstraction (HAA) pathway dominated the degradation processes regardless of the protonation state. However, without explicitly considering the solvent molecules, the calculated reaction rate constant (k, 1.09 × 107 M−1 s−1) was overestimated by an order of magnitude. With the explicit inclusion of the hydration shell, the calculated k value (5.26 × 105 M−1 s−1) agreed well with the measured one (7.89 × 105 M−1 s−1). Considerable charge transfer was found from the CO3 center to the solvation shells. In addition, the contour plot of CO3∙- contribution to overall elimination of various micropollutants was also constructed. The surface with the contribution greater than 10% includes many micropollutants with electron-rich groups such as thioethers, anilines and phenolates, demonstrating that the role of CO3∙- cannot be overlooked in most sunlit surface waters. These results yield mechanistic insights to the CO3∙--mediated degradation of micropollutants, providing practical guidance for their removal in both natural water systems and engineered water treatment processes.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

20701 - Environmental and geological engineering, geotechnics

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2023

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Chemical Engineering Journal

ISSN

1385-8947

e-ISSN

—

Svazek periodika

474

Číslo periodika v rámci svazku

OCT 15

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

9

Strana od-do

—

Kód UT WoS článku

001066190800001

EID výsledku v databázi Scopus

2-s2.0-85170252457