As a representative transition metal, iron plays a key
role in
chemical activities of atmospheric particulate matter (PM), being
involved in particle-related free radical generation and adverse health
effects. However, limited understanding of the structure and properties
of individual micrometer-sized particulates obscures investigating
the contributions of iron toward chemical activities. Here, we describe
multidimensional analytical strategies to characterize the mass, spatial
distribution, and chemical forms of iron in single haze particles
using synchrotron radiation techniques. We first used X-ray fluorescence
imaging to quantify the masses of multiple metals and yielded distribution
maps of transition metals, which revealed the types of elements that
tend to occur together. Additionally, we employed nanocomputed tomography
to assess the spatial distribution of iron and observed that iron
exists as small aggregates and is concentrated primarily in subsurface
regions. We also combined X-ray absorption near structures with scanning
transmission X-ray microscopy to quantify the ferrous and ferric forms
and mapped their distributions in individual particles, which probably
attribute chemical activity of iron. In conclusion, we demonstrated
the power of synchrotron radiation-based techniques to study heretofore
inaccessible chemical information in single haze particles, which
may provide important clues about iron chemistry as a source of Fenton
reactions and health effects. The multifaceted analytical approaches
exhibit high sensitivity (subfemtogram per particle or ∼0.2
fg/μm2) toward multiple elements and are promising
to be used for studying other concepts such as the solubility of aerosol
iron, the heterogeneous oxidation of organic matters and SO2, and the formation and the aging of haze particles.