RESUMEN
Carbonyls are ubiquitous in the troposphere and play a crucial role in atmospheric oxidation capacity (AOC), particularly in photochemistry-active regions such as the Tibetan Plateau (TP). However, the composition and evolution of carbonyls over the TP is still poorly understood due to a lack of comprehensive observations and modelling. Here, we conducted an intensive field measurement of 37 carbonyls and their precursors at a suburban site in Lhasa during summer 2022. Markedly higher levels of carbonyls (7.24 ± 3.83 ppbv) were found during ozone pollution episodes, with 36 % higher than those during non-episodes. Formaldehyde was the most abundant carbonyl (38 %), which primarily originating from photochemical secondary formations. Simulations using the Rapid adaptive Optimization Model for Atmospheric Chemistry (ROMAC) indicated strong AOC in Lhasa, with the daytime maximum of ·OH and ·HO2 of 9.8 × 106 and 4.2 × 108 molecules cm-3, respectively, which were even higher than that in most of the megacities in China. Notably, AOC significantly enhanced with the increasing carbonyls during the episodes, with the concentrations of ·OH and ·HO2 were boosted 21 % and 67 % than those during non-episodes, respectively. Budget analysis revealed that the ·HO2 + NO (88 %) and ·OH + VOC (74 %) pathways dominated the generation and loss of ·OH, respectively. And for ·HO2, they were ·RO2 + NO (67 %) and ·HO2 + NO (83 %). This study provides valuable insights into the strong AOC in the ecologically-fragile and climate-sensitive TP region, and highlighted the crucial role of anthropogenic-biogenic interactions in the active photochemistry of TP.
RESUMEN
Anthropogenic aromatics play a key role in photochemical pollution and pose a serious threat to human health. Current knowledge on source characteristics of aromatics in the urban region of the Tibetan Plateau (TP), the "Third Pole" and ecologically sensitive area, remains limited. In this study, an intensive observation of 17 aromatic hydrocarbons was conducted in Lhasa, the cultural and economic center of TP, during the second Tibetan Plateau Scientific Expedition and Research in summer 2020. The results showed that the average concentration of aromatics in Lhasa (7.6 ± 7.4 ppbv) was unexpectedly higher than those in megacities such as Beijing, Shanghai, and Guangzhou. Tripled concentrations and corresponding ozone formation potential during pollution episodes were recorded. Further source apportionment using positive matrix factorization revealed that solvent usage (60.0 %) was the dominant source, which may be due to the extremely low atmospheric pressure. Vehicle exhaust (15.4 %), industrial emissions (12.8 %), fuel evaporation (6.2 %), and burning emissions (5.7 %) were also important sources. The concentration weighted trajectory analysis revealed that the observed high levels of aromatics were mainly driven by local anthropogenic emissions, rather than the regional transport by the Indian summer monsoon. Long-term exposure to aromatics in Lhasa was assessed to pose carcinogenic risks to the population, with the risks of benzene and ethylbenzene 5 times the criteria. Our results suggest that, given the magnified emissions of aromatics in this extreme environment (low atmospheric pressure and strong solar radiation), the implementation of targeted pollution controls is urgently needed to mitigate the aromatic-related photochemical pollution and health threats in TP.