TY - JOUR
T1 - Impact of reversible and irreversible gas-particle partitioning of atmospheric carbonyl compounds on oxalic acid formation and δ¹ ³C distribution in Northwest China
AU - Qi, Weining
AU - Han, Yongming
AU - Liu, Yali
AU - Zhang, Yifan
AU - Dai, Wenting
AU - Teng, Teng
AU - Shen, Minxia
AU - Li, Lu
AU - Guo, Xiao
AU - Cao, Yue
AU - Jiang, Yingkun
AU - Wang, Qian
AU - Li, Shicong
AU - Li, Jianjun
N1 - Publisher Copyright:
© 2025 Elsevier B.V.
PY - 2025/12/5
Y1 - 2025/12/5
N2 - The gas-particle partitioning of carbonyl compounds through reversible and irreversible pathways constitutes a critical route for secondary organic aerosol formation. This study simultaneously observed distribution of formaldehyde (FA), acetaldehyde (AA), glyoxal (GLY), and methylglyoxal (MGLY) in both gas and particle phases, as well as concentration and stable carbon isotope (δ¹³C) of oxalic acid. The results show that in the reversible partitioning process, the carbonyl compounds during clean period are mainly partitioned into organic phase, and the salt-in effect exhibits kinetic limitations. However, they are mainly partitioned into aerosol liquid water during haze periods with lower partitioning coefficients, and there is a significant salt-in effect. The carbonyls present different irreversible partitioning pathways to contribute oxalic acid formation in haze periods. In Haze I (O3: 24 ± 11 ppb), the carbonyl compounds are mainly partitioned into aqueous phase and reacted with water to form polymers or undergoing self-polymerization. The large multifunctional compounds decomposed to yield oxalic acid, leading to progressive enrichment of δ¹ ³C. In Haze II (O3: 41 ± 13 ppb), the elevated atmospheric oxidation capacity promoted aqueous-phase oxidation of the carbonyls to generate intermediate products and ultimately forming oxalic acid. Under these conditions, oxalic acid-C exhibited a depleted δ¹ ³C signal.
AB - The gas-particle partitioning of carbonyl compounds through reversible and irreversible pathways constitutes a critical route for secondary organic aerosol formation. This study simultaneously observed distribution of formaldehyde (FA), acetaldehyde (AA), glyoxal (GLY), and methylglyoxal (MGLY) in both gas and particle phases, as well as concentration and stable carbon isotope (δ¹³C) of oxalic acid. The results show that in the reversible partitioning process, the carbonyl compounds during clean period are mainly partitioned into organic phase, and the salt-in effect exhibits kinetic limitations. However, they are mainly partitioned into aerosol liquid water during haze periods with lower partitioning coefficients, and there is a significant salt-in effect. The carbonyls present different irreversible partitioning pathways to contribute oxalic acid formation in haze periods. In Haze I (O3: 24 ± 11 ppb), the carbonyl compounds are mainly partitioned into aqueous phase and reacted with water to form polymers or undergoing self-polymerization. The large multifunctional compounds decomposed to yield oxalic acid, leading to progressive enrichment of δ¹ ³C. In Haze II (O3: 41 ± 13 ppb), the elevated atmospheric oxidation capacity promoted aqueous-phase oxidation of the carbonyls to generate intermediate products and ultimately forming oxalic acid. Under these conditions, oxalic acid-C exhibited a depleted δ¹ ³C signal.
KW - Carbonyl compounds
KW - Gas-particle partitioning
KW - Oxalic acid
KW - Reversible and irreversible uptake
KW - δ¹ ³C
UR - https://www.scopus.com/pages/publications/105021575388
U2 - 10.1016/j.jhazmat.2025.140496
DO - 10.1016/j.jhazmat.2025.140496
M3 - 文章
C2 - 41252988
AN - SCOPUS:105021575388
SN - 0304-3894
VL - 500
JO - Journal of Hazardous Materials
JF - Journal of Hazardous Materials
M1 - 140496
ER -