Comprehensive measurement of carbonyls in Lhasa, Tibetan Plateau: Implications for strong atmospheric oxidation capacity.

ABSTRACT

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.