Li Feifei, Lv Jitao, He Anen, Xu Jin, Zhao Lixia, Wang Xianwei, Mao Li, Li Shasha, Wang Hailin, Wang Yawei, Jiang Guibin
State Key Laboratory of Environmental Chemistry and Eco-toxicology, Research Center for Eco-environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
J Am Chem Soc. 2025 Aug 27;147(34):30574-30581. doi: 10.1021/jacs.5c02431. Epub 2025 Jul 10.
Singlet oxygen (O) is a classical nonradical reactive oxygen species (ROS), which is of great significance in both natural and engineering environments. Here, we found that O can be generated spontaneously at the air-water interface of microdroplets under dark conditions. O isotope labeled O (O) and water (HO) were used to identify the source and formation pathway of O and previously reported ROS produced in microdroplets. The results showed that O and superoxide anions (•O) were sourced from O, •OH was sourced from HO, while HO can be produced from both HO and O. Moreover, the excited hydrated electron (e(aq)) induced indirect energy transfer is responsible for exciting O from the ground state to the singlet state. The findings of this work provide an important complement to the construction of a complete ROS chemistry in microdroplets.
单线态氧（O）是一种典型的非自由基活性氧（ROS），在自然环境和工程环境中都具有重要意义。在此，我们发现O能够在黑暗条件下于微滴的气-水界面自发产生。使用O同位素标记的O（O）和水（HO）来确定O以及先前报道的微滴中产生的ROS的来源和形成途径。结果表明，O和超氧阴离子（•O）来源于O，•OH来源于HO，而HO可由HO和O两者产生。此外，激发态水合电子（e(aq)）诱导的间接能量转移负责将O从基态激发到单线态。这项工作的发现为构建微滴中完整的ROS化学体系提供了重要补充。
