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Title: Spatially resolved chemical imaging of individual atmospheric particles using nanoscale imaging mass spectrometry: insight into particle origin and chemistry

Journal Article · · Analytical Methods
DOI:https://doi.org/10.1039/C3AY42012D· OSTI ID:1321443
 [1];  [2];  [3]
  1. California Dept. of Public Health, Richmond, CA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Knowledge of the spatially resolved composition of atmospheric particles is essential for differentiating between their surface versus bulk chemistry and understanding particle reactivity and the potential environmental impact. Here, we demonstrate the application of nanometer-scale secondary ion mass spectrometry (CAMECA NanoSIMS 50 ion probe) for 3D chemical imaging of individual atmospheric particles without any sample pre-treatment, such as sectioning of particles. Use of NanoSIMS depth profile analysis enables elemental mapping of particles with nanometer spatial resolution over a broad range of particle sizes. We have used this technique to probe the spatially resolved composition of ambient particles collected during a field campaign in Mexico City. Particles collected during this campaign have been extensively characterized in the past using other particle analysis techniques and hence offer a unique opportunity for exploring the utility of depth-resolved chemical imaging in ambient particle research. The particles that we examined in our study include those collected during a pollution episode related to urban waste incineration as well as background particles from the same location before the episode. Particles from the pollution episode show substantial intra-particle compositional variability typical of particles resulting from multiple emission sources. In contrast, the background particles have relatively homogeneous compositions with enhanced presence of nitrogen, oxygen, and chlorine at the particle surface. We also observed the surface enhancement of nitrogen and oxygen species is consistent with the presence of surface nitrates resulting from gas–particle heterogeneous interactions and is indicative of atmospheric ageing of the particles. The results presented here illustrate 3D characterization of ambient particles for insight into their chemical history.

Research Organization:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC52-07NA27344
OSTI ID:
1321443
Report Number(s):
LLNL-JRNL-650135; AMNECT
Journal Information:
Analytical Methods, Vol. 6, Issue 8; ISSN 1759-9660
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 20 works
Citation information provided by
Web of Science

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Air pollution–aerosol interactions produce more bioavailable iron for ocean ecosystems journal March 2017
Physicochemical Characteristics of Individual Aerosol Particles during the 2015 China Victory Day Parade in Beijing journal January 2018
Direct observations of organic aerosols in common wintertime hazes in North China: insights into direct emissions from Chinese residential stoves journal January 2017
Organic coating on sulfate and soot particles during late summer in the Svalbard Archipelago journal January 2019
Quantitative capabilities of STXM to measure spatially resolved organic volume fractions of mixed organic ∕ inorganic particles journal January 2019