Atmospheric
iodine cycling is of significance in climate change
and environmental and health impacts. To better explore speciation
transformation of atmospheric stable and radioactive iodine, an ultra-sensitive
analytical method was established for determination of 129I and 127I in particulate, gaseous inorganic, and gaseous
organic species, which was conducted with a self-designed cascade
sampling apparatus, followed by their separation with a pyrolysis
system and accelerator mass spectrometry and ICP–MS measurements.
Combustion protocols for three sampling matrices and NaOH concentration
for iodine trapping were optimized to achieve a safe analytical procedure
with a high chemical yield of iodine. Based on the lowest concentrations
of 129I and 127I, a suitable activated carbon
product for adsorption of gaseous organic iodine was carefully selected.
The detection limits of the three species were 0.30–2.21 ng
m–3 for 127I and 0.05–0.22 ×
105 atoms m–3 for 129I. This
newly established method was successfully applied to analyze the levels
and species of 129I and 127I in ambinet air
from Xi’an, China, from May to August, 2020. Gaseous organic
iodine was found to be the dominant species of 127I and 129I, accounting for about half of total iodine, and gaseous
inorganic iodine and particulate iodine accounted for one-quarter
each during the whole sampling period. Speciation variation of 129I and 127I indicates that speciation transformation
apparently occurred at the turn of spring and summer, mainly between
particulate and gaseous organic iodine. This study has implications
on delicate tracing of the atmospheric behavior of iodine with long-lived
anthropogenic 129I.