Measured concentrations of relatively nonreactive, anthropogenic halocarbon tracers (CFC-11, CFC-12, CFC-113)
were used to infer the time since recharge, or age, of
groundwater collected from the Upper Glacial and Magothy
Aquifers underlying Brookhaven National Laboratory on
Long Island, NY. On the basis of the reconstructed
historical
atmospheric concentrations of CCl4, the initial
CCl4
concentration for the precipitation that recharged the
aquifer
was estimated as a function of age. Correlation of
measured and estimated initial CCl4 concentrations
within
the aquifer, over inferred ages of 0−50 yr, suggested
that
CCl4 was being removed in situ with a half-life of 14 ± 4
yr.
Groundwater samples collected at the water table had
CCl4 concentrations that were ≤50% of equilibrium
with
contemporary atmospheric concentrations, suggesting
that removal was also significant in the unsaturated zone.
Soil gas profiles confirmed that atmospheric CCl4
was
being removed from the unsaturated zone, with only ∼25%
of the initial CCl4 being present in the gas phase at a
depth
of 30 cm, and with no evidence for removal of CFC-11,
CFC-12, or CFC-113. A time−series of soil gas profiles
col
lected before and after a major rainfall event indicated
that most removal occurred in the top 15 cm of soil.
The
flux of CCl4 into the soil was estimated to be ∼8600
±
5100 pmol m-2 d-1,
and removal of CCl4 in soils therefore
has the potential to significantly affect the global
atmospheric lifetime of this compound. The observed
degradation in bulk aerobic environments raises
questions concerning the conventional wisdom that
CCl4
is degraded significantly only within reducing environ
ments.