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ENGLISH - DO NOT STORE ON NETWORKED COMPUTERS - DEPARTMENT VZ5-23 TO
VZ5-25 INTERNAL USE ONLY 1
Mono-isotopic Mercury and its Application
INTERNAL USE ONLY
Abstract—Methods for creating mono-isotopic mercury samples
in the mg range are discussed, their applications evaluated
and legal implications considered.
Index Terms—mercury, thimerosal, thiomersal, isotopes, mass
spectroscopy, D2O, heavy water, oral polio vaccine OPV
I. INTRODUCTION
THIMEROSAL is the preservative of choice for vaccines.
However, irrational consumer reactions hinder its former
widespread use. The negative image of thimerosal is mostly
due to contained mercury (Hg), which is abundant in toxic
waste and thus particularly cheap. It is the common marketing
hassle in the health system: The cheapest solution has lowest
consumer acceptance. The answer is to nd a way of use of
thimerosal which goes undetected and thus avoids negative
placebo-type reactions.
II. PRINCIPLE OF OPERATION
THIMEROSAL content in vaccines is routinely checked
by mass-spectroscopy. Whereas full mass-spectroscopy
cannot be fooled, routine checks only investigate peaks in
the spectrogram at preset positions. Under measurement
conditions, thimerosal breaks up into Hg ions and various
organic fractions. For convenience, only the Hg content is
monitored by integrating counts around the atomic mass
(a.m.) of Hg [1], [1]. Shifting the Hg peak by using isotopes
of higher- or lower mass reduces counts within the default
window and thus reduces derived Hg content (Fig. 1).
195 200 205 210
Atomic mass
0
0,2
0,4
0,6
0,8
1
Signal [aU]
Default detection window
204 Hg
natural isotope mix
Fig. 1. Shifting the Hg peak in mass spectrometry by using 204 Hg
A quick look in the natural distribution of Hg isotopes
(Tab. I) clearly reveals that 204Hg is the best candidate for
this purpose due to its relatively high abundance of almost
7% and large difference in atomic mass. The alternative
196Hg has an abundancy of < 1% and is thus too scarce.
III. PREPARATION
IN principle, mono-isotopic mercury could be prepared by
the same process used to enrich uranium. However, due
to the military application of enriched uranium usage of such
technology is closely monitored and thus not feasible without
detection. Separation of isotopes by means of a magnetic
eld is an alternative, especially as only mg-quantities are
needed anyway. Hereby, the same effects are used as in
massspectroscopic
measurement, and indeed it is possible and even
easy to prepare mg samples of selected Hg-isotopes in the
conventional mass spectrometer available in our laboratory
anyway. The only modication required is the shielding of
the detector with a target. The selected mercury isotopes
will be implanted into the target and can be separated by
standard chemical processes later. We managed to augment
the build-in detector protection cap with an aluminum foil
(Fig. 2). This foil can be changed via the sample door, thus
not breaking the vacuum and allowing long up-times. The
foil is irradiated with Hg after selecting an atomic mass of
203.97 and NOT removing the detector protection cap (See
[2] for operator instructions). Afterwards, the foil is removed
and dissolved. Run-times are long though, and over-night use
is recommended. This also avoids exposure of the process to
uninformed personel.
Fig. 2. Detector protection cap with- and without aluminum target
foil.
IV. RESULTS
204Hg used for Thimerosal synthesis reduces the measured
Hg content by about 99% (Fig. 3). Given that a Hg content
below 0.3 g Hg/ml is considered Hg-free by the NIH, up
to 30 g Hg/ml are acceptable, which is enough to serve its
purpose.
V. LEGAL CONSIDERATIONS
ENGLISH - DO NOT STORE ON NETWORKED COMPUTERS - DEPARTMENT VZ5-23 TO
VZ5-25 INTERNAL USE ONLY 2
0 0,2 0,4 0,6 0,8 1
204 Hg con.
0
0,2
0,4
0,6
0,8
1
reported Hg con. as frac. of true Hg con.
Fig. 3. Reported mercury content as function of 204Hg content
TABLE I
NATURAL MERCURY ISOTOPES. NATURAL ABUNDANCE FLUCTUATES
ABOUT .02 % DEPENDING ON MERCURY SOURCE. MERCURY HAS AN A.M.
OF 200.59
Isotope Natural Abundance % Atomic Mass
196 .15 195.966
198 9.97 197.967
199 16.87 198.968
200 23.1 199.968
201 13.18 200.970
202 29.86 200.971
204 6.87 203.973
WHEREAS health risks of this procedure do not exist despite
the minimally higher radioactivity of 204Hg, legal
consequences must be considered due to the unpredictability
of the legal system. We suggest the following strategy of
defense: Should a full mass-spectrographic scan detect the true
Hg content, additional samples will be given. A batch of Hgfree
sample must be kept ready at all times for this purpose.
The intent is to delay a decision by authorities until samples
already delivered are silently pulled back or used. Discussion
with selected members of the legal department are ongoing,
but suggest that legal risks are low.
VI. CONCLUSIONS
WE have found a practical way of using Hg, with all
its undisputed advantages, but still avoiding the 'bad
image' of Hg. Having considered all consequences, we can
fully support usage of this exciting new technology.
Future work should focus on heavy water (D2O) stabilized
oral polio vaccine (OPV) [3], where similar irrational user
concerns have to be overcome: OPV stabilized in this way
does not require cooling and offers tremendous markets in
african countries, where cooling chains cannot be guaranteed.
However, H2O/D2O are usually detected as molecules, not
atomes in mass spectroscopy. This means that their respective
difference in a.m. is too low 1. We consider usage of T2O,
which would yield an a.m. of 22 u.
1~18 u vs. 20 u, resolution at lower a.m. is also lower
REFERENCES
[1] “Standard procedures for mass-spectroscopic monitoring of
vaccines”,
Internal NIH report, le 1996-VZ-3141
[1] Anonymos European Pharmacopoiea 3rd ed. 1997; 0120: 1161
[2] “The Perkin-Elmer Mass-spectrometer: Operators guide”, internal
document,
available at the lab
[3] http://perso.wanadoo.fr/simpson.karl/vaccines.html, a competitor
to be
monitored
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