Size-dependent Molecular Characteristics and Possible Sources of Organic
Aerosols at a Coastal New Particle Formation Hotspot of East China
Abstract
We investigated size-dependent molecular characteristics of coastal
organic aerosols from < 0.032 μm to 3.2 μm at a new particle
formation (NPF) hotspot of east China by using Fourier transform-ion
cyclotron resonance mass spectrometry (FT-ICR-MS). Strong connection
between
C20-33HhOo/C18,30HhOoNn
compounds in particles smaller than 0.10 μm and the VOCs emitted from
local intertidal macroalgae suggests that the organic compounds (OC) in
ultrafine particles are formed probably via the gas-phase oxidation of
long-chain fatty aldehydes or acids, followed by particle-phase
accretion reactions or imine formation during the coastal NPF events. In
0.18-0.56 μm particles, dominant C8-C20
CHO, CHON, CHOS and CHONS compounds (maximum: C10 or
C15) are suggested most likely to be terpene oxidation
products. Highly oxygenated compounds with 0.6 ≤ H/C ≤ 1.5 and 0.67 ≤
O/C ≤ 1.2 reside mostly in 0.18-0.56 μm particles, accounting for 5% of
the OC formulas in this size range. Iodinated OC are subsequently formed
via electrophilic substitution of non-iodinated OC by iodine cations in
iodine-rich particles. CHN and Cl/Br-containing OC account altogether
for only 1-4% of total OC intensity. As a result of the above compound
distribution, the intensity weighted unsaturation degree and carbon
oxidation state of OC increase with particle size. The distribution of
aromatic compounds (i.e. Aromaticity Index > 0.5) is
bimodal with peaks in 0.056-0.18 μm and 1.0-3.2 μm. In addition, our
study observed higher unsaturation degree, carbon oxidation state and
aromaticity of OC in coastal PM2.5 than inland urban
PM2.5 in the same region.