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An extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) for online measurement of atmospheric aerosol particles
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An extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) for online measurement of atmospheric aerosol particles
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Journal Article
An extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) for online measurement of atmospheric aerosol particles
2019
Overview
Real-time, online measurements of atmospheric organic aerosol (OA)
composition are an essential tool for determining the emissions sources and
physicochemical processes governing aerosol effects on climate and health.
However, the reliance of current techniques on thermal desorption, hard
ionization, and/or separated collection/analysis stages introduces
significant uncertainties into OA composition measurements, hindering
progress towards these goals. To address this gap, we present a novel,
field-deployable extractive electrospray ionization time-of-flight mass
spectrometer (EESI-TOF), which provides online, near-molecular (i.e.,
molecular formula) OA measurements at atmospherically relevant
concentrations without analyte fragmentation or decomposition. Aerosol
particles are continuously sampled into the EESI-TOF, where they intersect a
spray of charged droplets generated by a conventional electrospray probe.
Soluble components are extracted and then ionized as the droplets are
evaporated. The EESI-TOF achieves a linear response to mass, with detection
limits on the order of 1 to 10 ng m−3 in 5 s for typical
atmospherically relevant compounds. In contrast to conventional electrospray systems, the EESI-TOF response is not significantly affected by a changing OA matrix for the systems investigated. A slight decrease in sensitivity in response to increasing absolute humidity is observed for some ions. Although the relative sensitivities to a variety of commercially available organic
standards vary by more than a factor of 30, the bulk sensitivity to secondary organic aerosol
generated from individual precursor gases varies by only a factor of 15.
Further, the ratio of compound-by-compound sensitivities between the
EESI-TOF and an iodide adduct FIGAERO-I-CIMS varies by only ±50 %,
suggesting that EESI-TOF mass spectra indeed reflect the actual distribution
of detectable compounds in the particle phase. Successful deployments of the
EESI-TOF for laboratory environmental chamber measurements, ground-based
ambient sampling, and proof-of-concept measurements aboard a research
aircraft highlight the versatility and potential of the EESI-TOF system.
