State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, 5 Yiheyuan Road, Beijing 100871, P. R. China.
Environ Sci Technol. 2022 Jun 21;56(12):7668-7678. doi: 10.1021/acs.est.2c00420. Epub 2022 May 10.
It is known that there are semiconductor oxides involved in mineral dust, which have photocatalytic properties. However, soot particles contained in carbonaceous aerosol and their photoactivity under sunlight are rarely realized. In this study, reactive oxygen species (ROS) such as superoxide anions and hydroxyl radicals were generated upon visible-light irradiation of soot particles, and the production activity was consistent with the carbonaceous core content, indicating that the atmospheric soot particles can serve as a potential photocatalyst. The increase of oxygen-containing functional groups, environmentally persistent free radicals, oxygenated polycyclic aromatic hydrocarbons, and the oxidative potential (OP) of soot after irradiation confirmed the occurrence of visible-light-triggered photocatalytic oxidation of the soot itself. The mechanism analyses suggested that the carbonaceous core caused the production of ROS, which subsequently oxidize the extractable organic species on the soot surface. It is oxidized organic extracts that are responsible for the enhancements of the OP, cell mortality, and intracellular ROS generation. These new findings shed light on both the photocatalytic role of the soot and the importance of ROS during the photochemical self-oxidation of soot triggered by visible light and will promote a more comprehensive understanding of both the atmospheric chemical behavior and health effects of soot particles.
已知矿物粉尘中存在半导体氧化物,具有光催化性能。然而,碳质气溶胶中所含的烟尘颗粒及其在阳光照射下的光活性很少被认识到。在这项研究中,在可见光照耀下,烟尘颗粒会产生活性氧物质(ROS),如超氧阴离子和羟基自由基,其产生活性与碳质核心含量一致,表明大气中的烟尘颗粒可以作为一种潜在的光催化剂。照射后烟尘中含氧官能团、环境持久性自由基、含氧多环芳烃和氧化势(OP)的增加证实了烟尘本身在可见光触发下发生了光催化氧化。机理分析表明,碳质核心导致了 ROS 的产生,而 ROS 随后氧化了烟尘表面可提取的有机物质。正是这些被氧化的有机提取物导致了 OP、细胞死亡率和细胞内 ROS 生成的增强。这些新发现不仅揭示了烟尘的光催化作用,而且还强调了在可见光触发的烟尘光化学自氧化过程中 ROS 的重要性,将促进对烟尘颗粒的大气化学行为和健康影响的更全面理解。