Appendix: "Differential Helium Retention in Zircons"
Geophysical Research Letters, Vol. 9, No. 10, Pages 1129-1130, October 1982
Differential Helium Retention in Zircons: Implications for Nuclear Waste Containment
Robert V. Gentry,1* Gary L. Glish,2 and Eddy H. McBay2
1Physics Department, Columbia Union College, Takoma Park, MD 20012
2Analytical Chemistry Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830
Abstract. A very sensitive helium leak detector
was utilized to measure the helium liberated from
groups of zircons extracted from six deep granite
cores. The observed low differential loss of
gaseous helium down to 2900 m (197°C) in these
ancient Precambrian rocks is easily attributable
to the greater diffusion of He at higher
temperatures rather than losses due to corrosion
of the zircons. This fact strongly suggests that
deep granite burial should be a very safe
corrosion-resistant containment procedure for
long-term waste encapsulation.
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*Also: Research Assistant Professor, Physics
Department, University of Tennessee, Knoxville,
TN 37916.
Copyright 1982 by the American Geophysical Union.
Paper number 2L1385.
0094-8276/82/002L-1385 $3.00
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Recent mass spectrometric studies (Gentry, et
al. 1982) have revealed that lead has been retained
in zircons extracted from deep (960 m to
4310 m) granite cores where the ambient temperature
increases from 105°C to 313°C at the
greatest depth. As a follow-up to those experiments
we now report the results of differential
helium retention in similar zircons extracted
from the same granite core samples which were
used in the lead analyses (Laney and Laughlin,
1981).
The procedure for separating the zircons from
the six different granite cores (from depths of
960, 2170, 2900, 3502, 3930, and 4310 m) was the
same as that used in the previous experiments.
The high-density fractions, obtained by passing
the crushed core samples through different methylene iodide separating funnels, were thoroughly
washed with acetone before being placed on a
standard microscope slide. A fine-tipped needle
was used to pick out the individual zircons with
the aid of a polarizing microscope. Groups of
these separated zircons, usually about 10 in
number, were then loaded onto the platinum
filament of the thermal inlet probe of the mass
spectrometer for differential helium analysis.
The helium measurements were performed on a
Leybold-Heraeus model F helium leak detector that
had a Chemical Data Systems Pyrolysis unit
interfaced to the test port. The leak detector
has a detection limit of less than 10−10 cm3/sec
when operating in the dynamic mode. (The
instrument could have been operated in a near-static mode with increased sensitivity down to
~l0−11 cm3/sec of He, but our experiments did not
necessitate this increased sensitivity.)
In our initial series of measurements our
spectrometer was calibrated against a 5 (±0.5)
× 10−8 cm3/sec standard He leak. A subsequent
recalibration with a more precise 5 (±0.5) × 10−10
cm3/sec standard He leak revealed the total helium
liberated during these initial measurements was
slightly underestimated. The general procedure was
to measure helium evolution from a group of
zircons at progressively higher temperatures of
400°C, 600°C, and 1000°C for 20 sec intervals.
(Previous studies of helium diffusion (Magomedov,
1970) from zircons indicated 1000°C was sufficient
to liberate the helium with an activation energy
of 15 kcal/mol.) We did not include the small
amount of He observed at 1100°C in the total He
summation because of possible atmospheric
contamination. Between six and eight groups of
zircons were analyzed at each depth. Runs were
repeated at a given temperature until background
helium levels were observed. Data recordings and
integration under the peaks were done with a
Nicolet 1170 signal averager.
The third column in Table 1 shows, as a function
of depth, the total amount of He liberated
per μg of zircon for zircon groups comprised of
approximately equal-size (~50-75 μm) zircons. The
fourth column in Table 1 shows the ratio of the
amount of He actually measured in zircons from any
particular depth to the estimated amount of He
which should have accumulated in those same
zircons assuming negligible diffusion loss. For
the zircons taken from a surface outcrop we assumed
this ratio was one because the specimens we
used were small fragments from the interior of
larger zircon crystals.
For the other zircons from the granite and
gneiss cores, we made the assumption that the
radiogenic Pb concentration in zircons from all
depths was, on the average, the same as that
measured (Zartman, 1979) at 2900 m, i.e., ~80 ppm
with 206Pb/207Pb and 206Pb/208Pb ratios of ten
(Gentry, et al., 1982; Zartman, 1979). Since every
U and Th derived atom of 206Pb, 207Pb, and 208Pb
represents 8, 7, and 6 α-decays respectively, this
means there should be ~7.7 atoms of He generated
for every Pb atom in these zircons.
Table 1: The values listed below show first,
as a function of depth and temperature, the
amount of helium liberated from various groups
of zircons in units of 10−8 cc per μg and
second, the ratio of the amount of helium
liberated to the theoretical amount which would
have been retained assuming no diffusion loss.
The near equality of the He concentrations in
the surface and 960 m depth zircons is not
particularly meaningful because the surface
zircons were from an entirely different
geological unit and doubtless have different U-Th-Pb concentrations than the zircons from the
core samples.
Sample Depth (m) |
Sample Temp. (°C) |
He (10−8 cc/μg) |
He(measured) He(theoret.) |
Surface |
20 |
8.2 |
1 |
960 |
105 |
8.6 |
0.58 |
2170 |
151 |
3.6 |
0.27 |
2900 |
197 |
2.8 |
0.17 |
3502 |
239 |
7.6 × 10−2 |
1.2 × 10−2 |
3930 |
277 |
~2 × 10−2 |
~10−3 |
4310 |
313 |
~2 × 10−2 |
~10−3 |
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