Reassessing the Quantum Yield and Reactivity of Triplet-State Dissolved Organic Matter via Global Kinetic Modeling

Du, Penghui1,2; Tang, Kexin4; Yang, Biwei1,2; Mo, Xiaohan1,2,3; Wang, Junjian1,2

2024-03-22

10.1021/acs.est.4c00214

ENVIRONMENTAL SCIENCE & TECHNOLOGY   影响因子和分区

0013-936X

1520-5851

Measuring the quantum yield and reactivity of triplet-state dissolved organic matter ((DOM)-D-3*) is essential for assessing the impact of DOM on aquatic photochemical processes. However, current (DOM)-D-3* quantification methods require multiple fitting steps and rely on steady-state approximations under stringent application criteria, which may introduce certain inaccuracies in the estimation of DOM photoreactivity parameters. Here, we developed a global kinetic model to simulate the reaction kinetics of the hv/DOM system using four DOM types and 2,4,6-trimethylphenol as the probe for (DOM)-D-3*. Analyses of residuals and the root-mean-square error validated the exceptional precision of the new model compared to conventional methods. (DOM)-D-3* in the global kinetic model consistently displayed a lower quantum yield and higher reactivity than those in local regression models, indicating that the generation and reactivity of (DOM)-D-3* have often been overestimated and underestimated, respectively. The global kinetic model derives parameters by simultaneously fitting probe degradation kinetics under different conditions and considers the temporally increasing concentrations of the involved reactive species. It minimizes error propagation and offers insights into the interactions of different species, thereby providing advantages in accuracy, robustness, and interpretability. This study significantly advances the understanding of (DOM)-D-3* behavior and provides a valuable kinetic model for aquatic photochemistry research.

dissolvedorganic matter environmental photochemistry tripletexcited state quantum yield globalkinetic model

SCI ; EI

英语

第一 ; 通讯

National Natural Science Foundation of China["22206070","42122054","42192513","22206211","42321004"] ; National Natural Science Foundation of China[JCYJ20220818100403007] ; Shenzhen Science and Technology Innovation Commission["2021A1515110153","2021B1515020082"] ; Guangdong Basic and Applied Basic Research Foundation[2020KCXTD006] ; Key Platform and Scientific Research Projects of Guangdong Provincial Education Department[2023B1212060002]

Engineering ; Environmental Sciences & Ecology

Engineering, Environmental ; Environmental Sciences

WOS:001189946600001

AMER CHEMICAL SOC

ENVIRONMENT/ECOLOGY

Web of Science

1.Southern Univ Sci & Technol, Sch Environm Sci & Engn, State Environm Protect Key Lab Integrated Surface, Shenzhen 518055, Guangdong, Peoples R China
2.Southern Univ Sci & Technol, Sch Environm Sci & Engn, Guangdong Key Lab Soil & Groundwater Pollut Contr, Shenzhen 518055, Guangdong, Peoples R China
3.Peking Univ, Sch Urban Planning & Design, Shenzhen Grad Sch, Shenzhen 518055, Guangdong, Peoples R China
4.Sun Yat Sen Univ, Sch Civil Engn, Ctr Water Resources & Environm, Guangzhou 510275, Guangdong, Peoples R China

Du, Penghui,Tang, Kexin,Yang, Biwei,et al. Reassessing the Quantum Yield and Reactivity of Triplet-State Dissolved Organic Matter via Global Kinetic Modeling[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY,2024,58(13).

Du, Penghui,Tang, Kexin,Yang, Biwei,Mo, Xiaohan,&Wang, Junjian.(2024).Reassessing the Quantum Yield and Reactivity of Triplet-State Dissolved Organic Matter via Global Kinetic Modeling.ENVIRONMENTAL SCIENCE & TECHNOLOGY,58(13).

Du, Penghui,et al."Reassessing the Quantum Yield and Reactivity of Triplet-State Dissolved Organic Matter via Global Kinetic Modeling".ENVIRONMENTAL SCIENCE & TECHNOLOGY 58.13(2024).