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- ItemEvolution of Ozone Pollution in China: What Track Will It Follow?(Columbus, Ohio : American Chemical Society, 2022) Guo, Jia; Zhang, Xiaoshan; Gao, Yi; Wang, Zhangwei; Zhang, Meigen; Xue, Wenbo; Herrmann, Hartmut; Brasseur, Guy Pierre; Wang, Tao; Wang, ZheIncreasing surface ozone (O3) concentrations has emerged as a key air pollution problem in many urban regions worldwide in the last decade. A longstanding major issue in tackling ozone pollution is the identification of the O3 formation regime and its sensitivity to precursor emissions. In this work, we propose a new transformed empirical kinetic modeling approach (EKMA) to diagnose the O3 formation regime using regulatory O3 and NO2 observation datasets, which are easily accessible. We demonstrate that mapping of monitored O3 and NO2 data on the modeled regional O3-NO2 relationship diagram can illustrate the ozone formation regime and historical evolution of O3 precursors of the region. By applying this new approach, we show that for most urban regions of China, the O3 formation is currently associated with a volatile organic compound (VOC)-limited regime, which is located within the zone of daytime-produced O3 (DPO3) to an 8h-NO2 concentration ratio below 8.3 ([DPO3]/[8h-NO2] ≤ 8.3). The ozone production and controlling effects of VOCs and NOx in different cities of China were compared according to their historical O3-NO2 evolution routes. The approach developed herein may have broad application potential for evaluating the efficiency of precursor controls and further mitigating O3 pollution, in particular, for regions where comprehensive photochemical studies are unavailable.
- ItemHumic Substance Photosensitized Degradation of Phthalate Esters Characterized by 2H and 13C Isotope Fractionation(Columbus, Ohio : American Chemical Society, 2023) Min, Ning; Yao, Jun; Li, Hao; Chen, Zhihui; Pang, Wancheng; Zhu, Junjie; Kümmel, Steffen; Schaefer, Thomas; Herrmann, Hartmut; Richnow, Hans HermannThe photosensitized transformation of organic chemicals is an important degradation mechanism in natural surface waters, aerosols, and water films on surfaces. Dissolved organic matter including humic-like substances (HS), acting as photosensitizers that participate in electron transfer reactions, can generate a variety of reactive species, such as OH radicals and excited triplet-state HS (3HS*), which promote the degradation of organic compounds. We use phthalate esters, which are important contaminants found in wastewaters, landfills, soils, rivers, lakes, groundwaters, and mine tailings. We use phthalate esters as probes to study the reactivity of HS irradiated with artificial sunlight. Phthalate esters with different side-chain lengths were used as probes for elucidation of reaction mechanisms using 2H and 13C isotope fractionation. Reference experiments with the artificial photosensitizers 4,5,6,7-tetrachloro-2′,4′,5′,7′-tetraiodofluorescein (Rose Bengal), 3-methoxy-acetophenone (3-MAP), and 4-methoxybenzaldehyde (4-MBA) yielded characteristic fractionation factors (−4 ± 1, −4 ± 2, and −4 ± 1‰ for 2H; 0.7 ± 0.2, 1.0 ± 0.4, and 0.8 ± 0.2‰ for 13C), allowing interpretation of reaction mechanisms of humic substances with phthalate esters. The correlation of 2H and 13C fractions can be used diagnostically to determine photosensitized reactions in the environment and to differentiate among biodegradation, hydrolysis, and photosensitized HS reaction.