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A Cryogenic Machine for Selective Recovery of Xenon

from Breathing System Waste Gases


John Dingley, MD* BACKGROUND: Xenon has many characteristics that make it very attractive as an
anesthetic and therapeutic drug. Unfortunately, the supply of xenon is fixed, and
Rod S. Mason, PhD therefore reclamation and recovery from even the most efficient breathing circuits
is desirable. We built and evaluated a cryogenic device to recover xenon from
waste anesthetic gases.
METHODS: Xenon was selectively frozen to 139.2C from test gas mixtures at ambient
pressure (STP). The machine ran on standard 240 V 13 A electrical current without
refrigerants that required replenishing, e.g., liquid nitrogen. A wide range of
xenon/oxygen mixtures were processed over a range of freezing chamber tempera-
tures. Efflux gas and thawed reclaimed xenon were collected separately. Xenon purity
and yield (fraction recovered) were measured and calculated on each occasion.
RESULTS: Gas was processed at 300 mL/min, and the operating temperature was
139.2 (0.096)C [Mean (sd)]. Purity and yield were 90% and 70% for gas
mixtures containing 20% xenon, increasing to 95% and 85%, respectively,
with an input gas xenon fraction 40%. Efficiency improved linearly with reducing
temperature.
CONCLUSIONS: Xenon of high purity (90%) and yield (70%) for such a machine
was recovered from all gas mixtures containing 20% xenon. The operating
temperature of the freezing chamber is a major influence on the efficiency of
recovery.
(Anesth Analg 2007;105:13128)

X enon is a noble gas with many attractive anesthetic


properties such as favorable hemodynamics, minimal
used in medicine, this would still only be approxi-
mately 800,000 anesthetics/treatments, even if xe-
side effects, and fast onset/emergence (1 8). It has non availability per patient was severely restricted
been licensed as an anesthetic in Russia (2002) and to, for example, 15 L. The notion that the price of
Europe (2007). Xenon may also be a potent neuropro- xenon will decrease as demand increases cannot be
tectant against hypoxic/ischemic brain injury (9 15). assumed, as liquefying additional air purely to
Proposed therapeutic uses include perinatal asphyxia extract xenon would be prohibitively expensive in
(15), cognitive deficit reduction after cardiac surgery energy terms. Given this fixed supply, recovery
(16,17), and stroke (18). methods could help to conserve xenon. The blood
If xenon does find a clinical role as an anesthetic solubility of xenon is much lower than that of other
or therapeutic agent, practical methods must be anesthetics (blood/gas solubility ratio 0.0115) and
found to minimize xenon consumption per patient uptake from the lungs is also very low (19). Conse-
episode because of its scarcity (approximate cost quently, although conventional circle anesthesia
US$10 per liter). Xenon is a by-product of industrial systems are usually considered to be gas-efficient,
oxygen production from the liquefaction of air. when used with xenon most of the xenon is still lost
Annual global production is therefore relatively as waste gas. Even with a fresh gas flow (FGF) as
fixed at approximately 9 12 million liters. If solely low as 500 mL/min, 80% of the supplied xenon is
lost as waste and if higher initial flows are used to
From the *Clinical School, and Department of Chemistry,
enhance wash-in; the waste fraction is even larger
University of Wales Swansea, Singleton Park, Swansea, UK. (20 22). However, the low solubility and uptake
Accepted for publication June 4, 2007. properties suggest that closed circuit breathing sys-
Supported by Department of Health, London, UK; New and tems, where FGF matches patient uptake with no
Emerging Applications of Technology (NEAT) funded project spill, might prove unusually gas-efficient with
AO94.
xenon (19). This is borne out by the closed circuit in
Reprints will not be available from the author.
Address correspondence to John Dingley, MD, University of Wales
vivo xenon consumption data of Luttropp et al. (6.5
Swansea, The Grove Building, Singleton Park, Swansea SA2 OUL, UK. L for initial 15 min and 2.5 L/h thereafter) and
Address e-mail to john.dingley@morrnhst-tr.wales.nhs.uk. Ferrari et al. (13 L for initial 30 min then 3.69 L/h
Copyright 2007 International Anesthesia Research Society thereafter) (23,24). Other groups have also success-
DOI: 10.1213/01.ane.0000278148.56305.72
fully used closed circuit xenon delivery systems

1312 Vol. 105, No. 5, November 2007


(24 29). Therefore, by optimizing breathing sys-
tems, this scarce resource can be used both respon-
sibly and at acceptable cost. Clearly, because of
limited supply, methods that could produce further
efficiency gains are worthy of investigation, and
xenon recovery is the next logical step.
There are two general approaches to xenon
recycling/recovery.
1. Collection of all waste gases by compression into
cylinders for reprocessing by the gas manufac- Figure 1. Cutaway view of the freezing chamber. This is
turer: As much as 60% of the xenon used has inserted into the refrigeration unit via one end of a thermally
insulated housing, seen on the right of the figure, permitting
been recovered in this way (24).
removal for sterilization. Being tapered, the distal end is
2. Selective recovery of xenon from waste gas mixtures. slightly smaller in diameter than the proximal end. On
One method used in Russia is to selectively insertion into a socket of equivalent shape within the
adsorb xenon onto molecular sieve material, refrigeration unit the tapers lock against each other creating
returning the saturated canisters to the gas manu- a good thermal connection with the cooling mechanism
inside.
facturer (20). Xenon liquefies at 108C, whereas
oxygen and nitrogen liquefy at 182.9C and
195.79C, respectively. At or below its freezing
point (111.7C), xenon should selectively freeze design modifications, as pilot studies had demon-
from such a gas mixture, and this has been strated that temperatures well below the freezing
achieved using liquid nitrogen coolant (20). In a point of xenon were needed to maximize yield. The
variation of this method, waste gases have been first stage dissipated the heat energy via an air-cooled
compressed to increase the freezing point of each radiator. Each stage was thermally insulated. The
gas, so that more modest cooling could then be refrigerants were: Stage 1, R404A (150 g); Stage 2,
used to freeze out the xenon. However, under R508B (110 g); and Stage 3, R14 (86 g) R290 (8 g). The
pressure, the other gases present tend to dissolve in design included an ultrasonic (1 MHz) xenon analyzer
the liquefying/solidifying xenon, reducing its final (Minison, Thomas Swan and Co. Ltd., Cambridge,
purity (30). UK) (29,31,32). All gas storage bags were metallic to
reduce xenon losses by diffusion (Hans Rudolph, Inc.,
The advantages of cryogenic approaches over KS City, MO).
adsorption methods include no gas contamination A control unit was built and programmed by one of
by the process itself and a more easily sterilized gas the authors (JD) (Fig. 3).
pathway.
Our first objective was to design and construct an Experimental Evaluation
automated ambient pressure cryogenic machine Pilot Experiments
with a removable sterilizable freezing chamber that Operating temperature. In one pilot experiment, a 50%
did not rely on cryogenic liquids, which evaporate xenon/50% oxygen mixture was pumped through a
and need replenishing as the cooling method. The freezing chamber being slowly cooled in 1 increments,
second objective was to experimentally evaluate the while the xenon content of the unfrozen efflux gas was
design. measured. We found that to maximize yield we needed
to operate the machine at temperatures substantially
lower than the freezing point of pure xenon, to maxi-
METHODS
mally skew the xenonsolid equilibrium by sublimation
Description of Apparatus with xenongas towards the solid form. For example, the
The final freezing chamber design consisted of an xenon concentration in the unfrozen efflux gas was
elongated tapered cylinder with proximal inlet and almost 15% at a temperature of 115C, but this could be
distal outlet ports (Fig. 1). This fitted into a corre- reduced to less than half this value at 139.2C.
sponding port in the refrigeration system, permitting Gas flow rate. At 500 mL/min efficiency decreased
easy removal for cleaning/sterilization. This chamber due to heating of the chamber by the incoming bulk
contained copper rings to present a large surface area gas flow. Later evaluations were performed at 300
for xenon to freeze onto and to allow even heat mL/min processing flow to allow a safety margin.
transfer throughout its interior.
The refrigeration unit comprised three stages, one Main Experiments
precooling the refrigerant circulating in the next stage Purity and yield for different input gas mixtures.
until a final working temperature in the freezing Gas storage bags were connected to the two outlets to
chamber of 139.2C was attained (NBS Cryoresearch collect unfrozen efflux gas and the xenon produced
Ltd., Tollesbury, UK) (Fig. 2). This was the lowest during the thaw cycle. Input gas for processing was
temperature the machine could achieve after several contained in a similar bag on the machine gas inlet.
Vol. 105, No. 5, November 2007 2007 International Anesthesia Research Society 1313
gold standard laser refractometer method (mean
difference of 0.74% and 2 standard deviation limits
of agreement of 1.08% to 2.56%) (33). We applied a
slight correction factor (multiply ultrasonic reading by
0.9835) derived from this previous work to improve
accuracy.
The above-mentioned procedure was repeated with
a series of five different oxygen/xenon input gas
mixtures. Three complete series of measurements
were made.
Relationship between efflux xenon concentration
and freezing chamber temperature. In pilot studies,
we observed that even when the chamber was sub-
stantially below the freezing point of xenon, some
xenon always remained unfrozen. To further investi-
gate the impact of freezing chamber temperature on
xenon recovery, a 50% xenon/50% oxygen input gas
mixture was passed through the chamber at a series of
sequentially decreasing and then increasing tempera-
tures with the percentage xenon in the efflux gas
noted at each step.

RESULTS
Figure 2. Freeze cycle: Gas to be processed is contained in Results are shown in Table 1. The mean freezing
bag (A). This is pumped via an inlet port (B) through the chamber temperature was 139.2 (0.1), at an ambi-
freezing chamber at 139.2C (C) where the xenon selec- ent temperature of 19.5 (1.7)C mean (sd). It was
tively solidifies. The remaining gases (efflux gas) emerge noted that xenon always started to thaw at a chamber
from the distal end of the chamber, pass through the xenon temperature of between 107C and 108C, in-
analyzer (D) and are directed by the outlet valve (E) to
atmosphere via hose (F). The xenon analyzer displays the keeping with the quoted boiling point of 107C
xenon content of the efflux gas which should be low. Thaw 3C (32). Purity and yield are shown graphically in
cycle: The gas pump stops, inlet port (B) automatically (Fig. 4).
closes, the chamber temperature increases to 100C where- The volume of gas processed was measured by
upon the xenon in the freezing chamber (C) thaws, becomes summation of the gas volume in the xenon and waste
gaseous and expands out via analyzer (D) to the outlet valve
(E), which now directs the xenon via hose (G) to a collection gas collection bags after each run (Table 1, columns 3
bag. The valves are all oxygen compatible (Model E3A. ACL and 5). There was a small difference between the
srl. Caponago, Italy). The microprocessor system (H) con- calculated total xenon content of the gas being pro-
trols the valves, gas pump, and the temperature of the cessed and that of the same gas once processed. This
chamber during each freeze/thaw cycle. The refrigeration could result, for example, from under-measurement of
unit forms the base of the machine (I).
the xenon collection bag or over-measurement of the
waste gas bag volumes. The opposite measurement
error could cause a slight apparent xenon gain.
The machine functioned automatically under com-
Yield calculations could therefore be performed in two
puter control. Once the chamber had cooled to
different ways. Although there is very little practical
139.2C, the inlet valve opened and a gas pump
difference between the results of either calculation, for
propelled the gas to be processed through the freezing
the purpose of Figure 4, we have erred on the side of
chamber. The xenon froze, forming xenon ice,
caution and presented the lowest, most conservative
whereas the unfrozen efflux waste gas from the cham-
yield values.
ber outlet was directed to a gas collection bag. After 5
The xenon concentration in the efflux gas was
L of gas had been processed, the pump stopped, the
rather independent of the concentration in the input
inlet valve closed and the chamber warmed to
gas (Fig. 5). The freezing chamber temperature influ-
100C, allowing frozen xenon to thaw to gas. The
enced the efficiency of recovery, as evidenced by the
chamber outlet valve changed, to direct the expanding
percentage of xenon present in the efflux gas, which
xenon gas to a xenon collection bag. After each run,
increased as temperature increased (Fig. 6).
the volume of gas in the efflux waste and xenon
storage bags (V1) and (V2) was measured by emptying
each bag in aliquots with a calibrated 200-mL syringe. DISCUSSION
The purity of recovered xenon was measured using This study demonstrated that the device developed
the xenon analyzer. This analyzer has been extensively for cryogenic recovery of xenon from waste anesthetic
evaluated and found to be very accurate relative to a gases was able to extract xenon reliably, and that the
1314 Selective Xenon Recovery System ANESTHESIA & ANALGESIA
Figure 3. Control algorithm for the machine.

Table 1. Performance of Machine with a Series of Test Gas Mixtures of Varying Xenon Content
Efflux waste Xenon recovery Xenon recovery
Input gas Input gas xenon Efflux waste gas gas xenon bag volume bag xenon
volume (mL) concentration (%) volume (mL) concentration (%) (mL) concentration (%)
5100 48.9 2950 7.5 2150 96.1
5650 39.0 3650 7.0 2000 98.2
4610 27.9 3400 6.8 1210 94.1
4730 20.4 3950 6.8 780 90.4
4560 10.6 4300 6.8 260 72.5
5940 48.2 3350 7.2 2590 95.8
6160 40.0 3900 7.1 2260 96.1
5560 29.8 4150 7.0 1410 94.8
5890 20.8 4900 6.8 990 92.2
5600 10.7 5300 6.8 300 73.4
6600 49.2 3620 7.3 2980 97.7
6360 39.7 4040 7.4 2320 96.5
6290 30.0 4700 7.1 1590 95.3
5545 20.1 4690 7.1 855 92.4
5610 10.5 5330 7.1 280 76.7
All gas processed at 300 mL/min. Ambient temperature 19.5 (1.7)C. Cooling chamber temperature 139.2 (0.1)C Mean (SD).

Vol. 105, No. 5, November 2007 2007 International Anesthesia Research Society 1315
gas as it passes through the freezing chamber can be
estimated, from the heat capacities of oxygen and
xenon, to be approximately 52 J/min. Improving heat
transfer properties where the chamber and its outer
cooling sleeve are in contact would permit both
faster gas flows and more rapid freeze/thaw cycling
times.
For a 70% xenon, 30% O2 inhaled gas mixture
(approximately 1 MAC), collection of useful gas for
recovery could include: gas flushed from a closed
breathing system to counteract N2 build up, xenon-
rich gas remaining in the circle and that eliminated
from the body in the first few exhaled breaths at the
end of an anesthetic. This would likely produce sev-
eral liters of gas with 20% xenon content, from
which our machine should be able to recover 70% of
the xenon.
For xenon, very low-flow circuits are not as efficient
as one might assume and it is clear that xenon
Figure 4. Purity and yield of recovered xenon relative to the recovery in this situation would greatly reduce overall
xenon content of the input gas (flow, 300 mL/min; tempera- xenon use. For example, Burov et al. (20,35) described
ture, 139.2C).
a very-low flow protocol in which anesthesia is main-
tained with FGFs of 300 mL/min xenon and 300
purity of the extracted xenon exceeded 90%. The mL/min oxygen. If, during maintenance, we assume
percentage unfrozen xenon in the efflux gas is mainly typical uptake values of 60 mL/min xenon and 250
determined by the temperature of the freezing cham- mL/min oxygen (metabolic), this would still generate
ber and independent of the input gas xenon fraction. an overspill or wastage rate of 240 mL/min (14.4 L/h)
Since the experiments were performed at atmospheric xenon (i.e., 80% of the xenon FGF) and 3 L/h oxygen.
pressure, the expected percentage of unfrozen xenon A closed-circuit breathing system would be a better
can be derived from the vapor pressure. At 139.2C, choice of breathing system as it would minimize the
the machine operated exactly as predicted from pub- volume of gas to be processed (36).
lished physical chemistry data; however, at tempera- From these closed-circuit breathing systems, the
tures close to its freezing point, the efficiency of xenon waste gas collected would mainly be produced by
recovery appeared to be much better than predicted denitrogenation circle flushes with fresh gas, re-
(Fig. 6) (32). This requires some consideration. sidual xenon purged from the circle, and the initial
The published vapor data in the 139 to 112 exhaled gas collected during emergence from anesthe-
temperature range are for xenon gas in equilibrium sia. This gas would again be rich in xenon. By extrapo-
(by sublimation) with frozen solid xenon. However, lation of data from Luttropp et al. and Ferrari et al. (in
before multiple layers of solid xenon can form, gas which a denitrogenation flush was included) a 2-h
will first be adsorbed onto the surfaces of the copper closed circle anesthetic would consume 10.9 L ($109)
rings in the freezing chamber. Xenon adsorbs much and 18.6 L ($186) of xenon, respectively (23,24). Fur-
more readily to copper than to its own solidified thermore, by returning all waste gas collected in this
molecules (i.e., xenon ice); therefore, the intense way to the xenon manufacturer, Ferrari et al. (24)
cooling we used may not be required if the copper managed to recover 60% of the total xenon used. The
surface area can be increased (34). cost of industrially reprocessed xenon has been
Also, the xenon content decreases as the gas moves estimated at $3 per liter, and thus if 60% could be
along the chamber. Further xenon can only reach the recycled, this would reduce the above estimates for a
distal chamber by diffusion from the proximal section 2-h anesthetic from $109 $186 to $63$108. It is likely,
(diffusion limited transport). therefore, that even with closed-circuit breathing sys-
It is clear that we observed the mixed effects of tems, a recovery device could still usefully reduce
several processes. Potential improvements to the de- overall xenon consumption per anesthetic, a 50%
sign would include the use of a honeycomb structure reduction perhaps being a realistic target. By combin-
within the freezing chamber to increase the copper ing xenon recovery with closed circuit use, it is
surface area (for which xenon has a high affinity) and conceivable that a 2-h administration for anesthesia or
a further reduce operating temperature. neuroprotection could be achieved using less than 10
The gas processing rate could also be improved. L xenon overall.
Currently, every 5 L of gas processed takes 53 min, There are a number of issues that would have to be
mostly due to the pauses in processing during cooling addressed before a cryogenic machine of this type could
and thawing. The heat transfer (removal) rate from the be used in a clinical setting. Waste gas from a circle
1316 Selective Xenon Recovery System ANESTHESIA & ANALGESIA
Figure 5. Xenon content of efflux gas from
freezing chamber is not materially affected by
xenon content of the input gas being processed
(flow, 300 mL/min; temperature, 139.2C).

Figure 6. Relationship between the xenon con-


tent of the unfrozen efflux gas and the chamber
temperature. Input gas was a 50% oxygen/50%
xenon mixture. Measurements were taken in
decreasing and then increasing temperature
steps. Predicted values derived from vapor pres-
sure data (xenongas over xenonsolid) taken from
published literature are also shown (32).

system might be very humid, containing carbon dioxide pathways could be sterilized between patients, the
and possibly volatile anesthetic vapors. These could be sterility of the gas itself would be less of an issue than
removed by removing gas for processing from a point if recovered xenon were intended for other patients.
distal to the circle soda lime canister to ensure carbon Although the removable chamber can be sterilized
dioxide removal, by using a dehumidification chamber more readily than, for example, membrane or zeolite-
containing silica gel beads for example or by using a based devices, sterility concerns over the gas itself
volatile vapor adsorbent, such as activated charcoal, as mean that, realistically, recycling would need to be
seen in the Physioflex closed circuit machine (37). Alter- restricted to the same patient episode only. It is more
natively, a precooling chamber at approximately likely that such a device might form part of a theater
50C could selectively freeze water vapor, volatiles, complex central xenon recovery facility, from which
and any residual carbon dioxide. the relatively pure xenon could be returned at inter-
From a legal perspective, the recovery process vals to a gas manufacturer for final purification,
could be considered the manufacture of a medical gas sterilization, and recertification as a medical gas.
and the operator to be a medical gas manufacturer, In conclusion, we have demonstrated that an auto-
responsible for its medical purity (typically 99.9% or mated xenon recovery machine running on 240 V AC,
above) and freedom from microbial contamination. If 13 A standard electrical current with autoclavable
recovered xenon were only to be reused during the components is technically feasible. It functioned, as
same patient anesthetic then, so long as the gas intended, without the use of refrigerants (e.g., liquid

Vol. 105, No. 5, November 2007 2007 International Anesthesia Research Society 1317
nitrogen) that require replenishment. Within-patient 13. Homi HM, Yokoo N, Ma D, Warner DS, Franks NP, Maze M,
Grocott HP. The neuroprotective effect of xenon administration
xenon recycling and reuse might prove feasible, but during transient middle cerebral artery occlusion in mice.
concerns over purity, gas sterility, and legal issues Anesthesiology 2003;99:876 81
preclude interpatient xenon reuse. A machine such as 14. Ma D, Yang H, Lynch J, Franks NP, Maze M, Grocott HP. Xenon
this might be best suited for use in a central xenon attenuates cardiopulmonary bypass-induced neurologic and
neurocognitive dysfunction in the rat. Anesthesiology 2003;
recovery facility. Even with the most efficient breath- 98:690 8
ing systems, this recovery method could still usefully 15. Dingley J, Tooley J, Porter H, Thoresen M. Xenon provides
reduce overall xenon consumption. Such unusual at- short-term neuroprotection in neonatal rats when administered
after hypoxia-ischemia. Stroke 2006;37:501 6
tention to detail may be necessary if xenon finds a 16. Arrowsmith JE, Grocott HP, Reves JG, Newman MF. Central
clinical role as a neuroprotective drug, since demand nervous system complications of cardiac surgery. Br J Anaesth
could easily outstrip a fixed supply. Regardless of the 2000;84:378 93
purchase price, medical xenon will always be a scarce 17. Grocott HP. Cerebral injury during cardiac surgery: under-
standing the need for a neuroprotective strategy. J Anasth
commodity. Ten liters of xenon per 2 h delivery period Intensivbehandl 2002;2:45 6
may be a realistic overall target using closed circuit 18. Altschuler EL. Xenon as neuroprotectant in acute stroke? Med
breathing systems in combination with a xenon recov- Hypotheses 2001;56:227 8
19. Goto T, Suwa K, Uezono S, Ichinose F, Uchiyama M, Morita S.
ery device of this type. The blood-gas partition coefficient of xenon may be lower than
generally accepted. Br J Anaesth 1998;80:255 6
ACKNOWLEDGMENTS 20. Burov NE, Makeev GN, Potanov VN, Kornienko L. Alternative
The authors thank Dr. Alexei Moozyckine, Swansea, UK, means for reducing the cost of xenon anesthesia. Anesteziol
for technical assistance; Mr. John Minister, NBS Cryore- Reanimatol 1997:71 4
21. Lynch C III, Baum J, Tenbrinck R. Xenon anesthesia. Anesthe-
search, Tollesbury, UK, for advice and construction of part of siology 2000;92:865 8
the machine; Dr. Per Blom and Wolfgang Shmehl of Linde 22. Nalos M, Wachter U, Pittner A, Georgieff M, Radermacher P,
Gas therapeutics, Lidingo, Sweden for donation of xenon gas. Froeba G. Arterial and mixed venous xenon blood concentra-
tions in pigs during wash-in of inhalational anaesthesia. Br J
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1318 Selective Xenon Recovery System ANESTHESIA & ANALGESIA

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