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Journal of Alloys and Compounds 645 (2015) S51–S55

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Journal of Alloys and Compounds


journal homepage: www.elsevier.com/locate/jalcom

Hydrogen isotope separation for fusion power applications


R. Smith a,b,⇑, D.A.J. Whittaker a,b, B. Butler a,b, A. Hollingsworth a,b, R.E. Lawless a,b, X. Lefebvre a,b,
S.A. Medley a,b, A.I. Parracho a,b, B. Wakeling a,b, JET-EFDA Contributors b,1
a
EURATOM/CCFE Fusion Association, Culham Science Centre, Abingdon OX14 3DB, UK
b
JET-EFDA, Culham Science Centre, Abingdon OX14 3DB, UK

a r t i c l e i n f o a b s t r a c t

Article history: The invited talk given at MH2014 in Salford ranged over many issues associated with hydrogen isotope
Available online 9 February 2015 separation, fusion machines and the hydrogen/metal systems found in the Joint European Torus (JET)
machine located near Oxford. As this sort of talk does not lend itself well to a paper below I have
Keywords: attempted to highlight some of the more pertinent information. After a description of the Active Gas Han-
Fusion dling System (AGHS) a brief summary of isotope separation systems is described followed by descriptions
Tritium: isotope of three major projects currently being undertaken by the Tritium Engineering and Science Group (TESG),
the upgrade to the Analytical Systems (AN-GC) at the AGH, the construction of a Water Detritiation Sys-
tem (WDS) and a Material Detritiation Facility (MDF). Finally, a review of some of the challenges facing
fusion with respect to metal/hydrogen systems is presented.
Ó 2015 Elsevier B.V. All rights reserved.

1. Introduction various hydrogen isotopes and helium could have unforeseen


influences on the ‘ITER scenarios’ and an integration of DT H-mode
The Joint European Torus (JET) tokomak and the connected plasma operations with a Be/W first wall is required. Tritium
Active Gas Handling System (AGHS), operated by the Tritium Engi- inventory control is an area which requires improvement, as does
neering and Science Group (TESG), were built for the study of a a validation of wall conditioning techniques for tritium, and meth-
fusion reactor with operating conditions relevant to a potential ods for tritium removal. Possibly the most valuable area is that of
power plant. This required the use of deuterium–tritium gas mix- operational experience. The training of staff in DT operations, and
tures for plasma fuelling. This meant that the design of the JET the development of organisational competence, is an area that is
tokomak and its associated support systems had to make provision vital. The final details of DTE2 are to finalised but the planned
for processing of radioactive tritium gas mixtures and tritium con- throughput of tritium is to rise from 100 g in DTE1 to 1000 g in
taminated materials. DTE2 and the total inventory in the AGHS will increase from 20 g
JET is the only tritium compatible magnetic confinement fusion in DTE1 to 60 g in DTE2.
device currently active. Tritium was injected into a large tokomak As the operators of the world’s only fusion related tritium plant
for the first time during the Preliminary Tritium Experiment (PTE) the members of the TESG are uniquely placed to understand the
in 1991 and since then 2 follow up T2 experiments in 1997 and issues associated with tritium/fusion operations. As part of the
2003. The next tritium campaign, DTE2 (Deuterium Tritium Exper- new EuroFusion consortia the TESG has become involved in the
iment 2), is being planned for 2017 and lessons learned during this design of DEMO, the European Fusion device currently in the con-
campaign will provide further valuable information to ITER and ceptual design stage which is planned to provide >300 MW (elec-
DEMO. tric) to a national grid by 2050.
The main motivational factors for DTE2 focus on risk mitigation
for ITER (the next generation tokomak being constructed in Cadar- 2. Overview of the AGHS PLANT
ache, France, by an international consortium. The operation with
The Joint European Torus (JET) Active Gas Handling System
(AGHS) was designed and built for the purpose of safely storing,
⇑ Corresponding author at: EURATOM/CCFE Fusion Association, Culham Science
supplying and recycling the hydrogen isotopes of deuterium (D2)
Centre, Abingdon OX14 3DB, UK.
E-mail address: robert.smith@ccfe.ac.uk (R. Smith).
and tritium (T2) used in fusion experiments at JET [1]. The AGHS
1
See appendix of Romanelli F. at al Proc. 24th IAEA Fusion Energy Conf. (San Diego, consists of an interconnected series of subsystems (Fig. 1). The
CA, 2012). Torus contains the deuterium–tritium plasma during short (of

http://dx.doi.org/10.1016/j.jallcom.2015.01.231
0925-8388/Ó 2015 Elsevier B.V. All rights reserved.
S52 R. Smith et al. / Journal of Alloys and Compounds 645 (2015) S51–S55

the order of 10 s) pulsed fusion experiments. The adjacent Neutral It is likely that the methods used at the AGHS will not be fully
Injection Boxes (NIBs) are used for heating and fuelling the plasma suitable for larger reactors such as ITER and DEMO. This is because
through highly energetic neutral beams of deuterium and tritium. these methods are costly, complicated to operate, energy intensive,
The AGHS provides the tritium used in the plasma and subse- operator intensive and time consuming. Because of the require-
quently extracts the gas (a mixture of deuterium, tritium and ment for more efficient technologies in future reactors, a number
impurities) after each experiment. of different techniques (both established and new) will be assessed
Deuterium and tritium are stored in the Product Storage (PS) by the TESG, in order to determine their viability.
subsystem in the form of uranium hydride, using bespoke uranium All isotope separation systems work by exploiting the small dif-
beds (UBeds). The PS UBeds contain either 1 kg or 4 kg of depleted ferences in physiochemical behaviour deriving from their differ-
uranium allowing for storage of 7 or 27 mol of hydrogen, respec- ence in mass (isotope effects, see e.g. [4]). Examples of these
tively [2,3]. The UBed is heated to a temperature of 873 K to release effects include variations in vapour pressure, chemical bond
gaseous D2 and T2. The D2 and T2, is then expanded into the Gas strength, boiling and freezing points, viscosity, surface tension,
Introduction and Distribution (GI and GD) transfer lines for supply and variations in optical omission spectra. Chemical equilibrium
to the Torus, either directly via a Gas Introduction Module (GIM) or and reaction rates can also change between isotopes and be
from the NIBs. exploited. In the case of hydrogen, the large proportional mass dif-
Hydrogen isotopes and other impurity gases (predominately ference can prove beneficial for isotope separation as it enhances
helium and traces of nitrogen and hydrocarbons) resulting from the isotopic effects.
the JET plasma experiments are pumped back to the AGHS via In order to establish the most promising candidates for an iso-
ML1 and ML2 using the Mechanical Forevacuum (MF) subsystem tope separation system for future reactors, a review of current
or, when tritium is present, the Cryogenic Forevacuum (CF) subsys- and promising future technologies will be produced by TESG. The
tem, which provides cryogenic pumping at liquid helium tempera- use of metal hydrides as a separation tool will be a key area of
tures. CF separates the hydrogen isotopes from the other gases investigation, along with the use of nanoporous framework mate-
(impurities) using a mixture of activated charcoal trapping and rials and molecular sieves. Other areas of research will include:
rough cryogenic distillation. The impurities are then taken to the Atomic vapour laser isotope separation (ALVIS), catalytic exchange,
Impurity Processing (IP) subsystem. The hydrogen isotopologues gaseous diffusion, thermal cycling absorption, centrifugation, bio-
(a mixture of H2, D2, T2, HD, HT and DT) are sent to the Intermedi- logical techniques and continuous ion exchange alongside the
ate Storage (IS) subsystem, where the gas is temporarily stored on existing technologies used in the AGHS.
UBeds.
The IP gas processing loop consists of a 2 m3 reservoir, a cold 4. Outline of the AN-GC upgrade
trap cooled by gaseous nitrogen (to 160 K) for removal of water,
a nickel catalyst module for removal of hydrocarbons, a thin palla- The primary instrument for determining the hydrogen isotopo-
dium permeator membrane for removal of any remaining impuri- logue content of samples (including hydrogen in hydrocarbons) in
ties, four UBeds for hydrogen storage and a 150 m 3 h 1 pump AN is the Analytical Gas Chromatograph (AN-GC) instrument [5].
connected in series. The IP subsystem separates any remaining GC instruments separate the various molecular components of a
hydrogen isotopologues from the impurity gases. mixed gas by passing a sample through a series of separation col-
The Cryogenic Distillation (CD) subsystem is used to roughly umns, which separate the gases in space, followed by an appropri-
separate the deuterium and tritium isotopes and remove the hydro- ate detector which distinguishes the boundaries between the
gen isotope from the gas mixture. The deuterium and tritium can gaseous species (see [5] for a detailed description with diagrams).
then be separated using the Gas Chromatography (GC) subsystem Hydrogen isotopes are chemically very similar and there are diffi-
(note, the interconnections between the CD and GC systems are culties associated with handling tritium due to its radioactivity.
not shown in Fig. 1). The resulting D2 and T2 products are then sent Therefore, there are no commercially available GC solutions for a
to PS for long term storage ready for supply to the Torus. tritium processing plant.
Additional AGHS subsystems, which are not part of the main D2 A new customised GC is being constructed for use during
and T2 recycling process, are used to aid the gas processing and DTE2. In addition to several standard separation columns, a cus-
ensure safety. The Analytical Laboratory (AN) is capable of analys- tomised hydrogen isotope separation column containing palla-
ing gas samples from each subsystem, allowing the composition of dium will be included. For safety reasons, the entire assembly
the gas at every processing stage to be determined. The Exhaust is contained within a nitrogen filled glovebox, thus bespoke fur-
Detritiation (ED) system (EDS) removes the remaining traces of tri- naces and liquid nitrogen dewars are required for temperature
tium, by converting all free hydrogen and hydrogen containing control.
compounds to water, from any gases destined for discharge to The AN-GC assembly includes several detectors; Thermal Con-
the environment. ductivity Detectors (TCDs) for the detection of hydrogen isotopes,
a Methaniser and Flame Ionisation Detector (FID) combination
3. Hydrogen isotope separation for future fusion applications for hydrocarbons, and Ionisation Chambers (ICs) for tritium. The
ICs for this system are custom built low volume units, with 5 cc
The balance of deuterium and tritium in a deuterium–tritium chambers and flush gold plated outer chambers and zero dead vol-
plasma is crucial for fusion applications. Fusion reactions also have ume micrometering valves to ensure the separation within the AN-
a very low burn-up rate for the tritium. Therefore, large quantities GC is not affected. A Quadrupole Mass Spectrometry (QMS) will
of tritium must be separated from deuterium (after removal of also be connected to the system, which allows detailed analysis
other impurities) and re-cycled after extraction from the Torus. of small samples (pressures 10 12 < P < 10 5 hPa) through a Resid-
Some of the work currently being undertaken by TESG involves ual Gas Analyser (RGA) detector. The RGA allows species that the
looking into alternative isotope separation techniques that can be AN-GC cannot separate to be discriminated, as well as determining
utilised by future fusion reactors. At present, the only fusion reac- the isotopic content of overlaying non-radioactive species. The
tor capable of operating with tritium is the JET and the two meth- exhaust of the AN-GC will include a bypass containing a custom
ods used are Gas Chromatography (in the GC subsystem) and built, tritium compatible Laser Raman (LARA) gas cell for further
Cryogenic Distillation (in the CD subsystem) analysis of the gasses [6].
R. Smith et al. / Journal of Alloys and Compounds 645 (2015) S51–S55 S53

Fig. 1. Schematic flow diagram of the JET AGHS [1]. This shows the Torus, NIBs and the D2 and T2 supply systems (left) and the AGHS subsystems used for processing and
storing D2 and T2 (right). The AGHS is connected to the Torus via the D2 and T2 supply lines for supply and the matrix lines 1 and 2 (ML1 and ML2, respectively) for exhaust
extraction.

5. Water detritiation system cryogenic distillation system. The two columns can be used in par-
allel for low separation but high volume processing or series to
The EDS removes hydrogen species from the exhaust by con- achieve higher separation but low volume. Comparison of the
verting them to water and collecting the condensate. The average two column design and an equivalent single column has been con-
activity of this condensate tritiated water is 10 GBq/l, with a max- ducted through modelling with PROSIM software [7]. The two col-
imum activity of 180 GBq/l with 4–10 tonnes of water generated umn solution reduced the cooling requirement at 20 K by a factor
each year and stored. A new capability is being developed by TESG of three and allowed for a greater throughput by reducing the
to process this water (Fig. 2). This reduces the waste disposal costs reflux ratio by two (the reflux ration being a measure of recycling
and demonstrates a more enclosed tritium cycle during the next of the distillation top product by the column).
fusion tritium campaign.
The purpose of the Water Detritiation System (WDS) is to crack
water into hydrogen isotopologues and oxygen, then concentrate 6. New materials detritiation facility
the tritium ready for processing by the existing AGHS instruments.
The non tritiated gas is released direct to the atmosphere. There is around 30 tonnes of intermediate level tritiated waste
Water is first purified using a bespoke series of tritium compat- (specific activity above 12 kBq/g of T) expected to be produced dur-
ible water filters. Then, the hydrogen isotopologues are separated ing JET operations up to the end of DTE2. The waste consists of var-
from oxygen using an electrolyser unit. A palladium permeation ious steels (70%), carbon fibre composite tiles (20%), beryllium
membrane is used to remove any impurities and the resultant Q2 (3%), and other metals (7%). The specific activity of the waste
(where Q is any hydrogen species) is separated in a two column is up to 100 kBq/g. It is necessary to re-classify this waste as
low level waste (between 0.1 kBq/g and 12 kBq/g tritium) before
the end of the JET operating contract in 2018 for disposal. The
materials detritiation facility (MDF) has been designed to meet this
requirement through processing two batches of 35 kg of waste per
day during 400 days of operation between early 2015 and the end
of 2018.
Depth profiling studies [8–12] show that between 18% and
62% of the tritium activity for this waste is on the surface, thus
more easily removed than bulk contamination. A study was
made by the JET waste management group and Inutec to deter-
mine the viability of bakeout at 1000 °C under air flow as a tech-
nique for detritiation of carbon fibre composite divertor tiles
Fig. 2. The process cycle of the AGHS, including the capability being developed to (summary available on request) to compliment similar studies
process the tritiated water. on other fusion related materials [9,12,13–14]. The results of
S54 R. Smith et al. / Journal of Alloys and Compounds 645 (2015) S51–S55

Fig. 3. Schematic representation of one material detritiation process.

these studies indicate that a bakeout under air flow technique is material, results in regulatory constraints. Alternative materials
successful. Other requirements of the MDF are the ability to with improved performance are of interest as storage media.
track the ILW and LLW waste, sample the waste, break up larger The long term effects of hydrogen diffusion into structural
components and to cycle the process if the LLW limit is not materials are of interest, including embrittlement and effects on
reached for a given batch. other material parameters. Relevant materials include stainless
A commercially available furnace with a 600 L volume that can steels, Eurofer, oxide dispersion steels, tungsten and beryllium.
reach 1600 °C will be used for the main detritiation stage of the Tritium containment is very important. Hydrogen easily dif-
process. The process is outlined in Fig. 3. After receipt, waste is fuses through many materials, so techniques to form permeation
sorted, sampled and analysed for tritium content. The waste is then barriers are required to improve safety, reduce complexity and
separated into 40 kg batches placed in barcoded boxes and vented increase the lifetime of a plant.
through the tritium recovery system. The boxes are placed into the Separation of hydrogen and hydrogen compounds from other
furnace for the main detritiation stage where tritiated water is off- gasses is a key requirement both for low concentrations (such as
gassed. A pumping system moves air (to provide the oxygen for diffusion into coolants) and high concentrations (in the tritium fuel
combustion) through the furnace to a bubbler system consisting cycle). Novel separation techniques could contribute to fusion
of two 200 L water filled drums (where isotopic exchange with development.
water removes tritium from the air) and out to atmosphere. The It is more difficult to pump lighter gases such as hydrogen com-
bakeout temperature is chosen such that it is below the melting pared to gases such as nitrogen. Experiences with hydrogen pump-
point of the material. After bakeout, sampling is done and either ing technologies are of interest.
the process is repeated or waste is stored in an LLW rack for dis- Finally, it is worth mentioning that the availability, supply, stor-
posal. This process can be completed once per day with two fur- age and gas handling of deuterium will be important, and any
naces used in the facility and operator input only required during issues relating to this specific isotope of hydrogen would be of
working hours. A feasibility study [15] showed that the process interest.
is achievable, cost effective and safe for waste with the specific
activity in the ranges expected.
8. Conclusions

7. Challenges facing fusion development with relation to metal The TESG is currently engaged in a series of upgrades in prepa-
hydrides ration for DTE2 in 2017 as well as the construction of new facilities
to process waste generated. The experience gained both in this
Many of the challenges in dealing with metal hydrides are sim- preparation for, in the execution of DTE2 (Deuterium Tritium
ilar for dealing with hydrogen species in the fusion community. Experiment 2) will be an invaluable resource to the work to come
The additional hazard experienced in fusion relates to the radiolog- at ITER and DEMO.
ical effects of tritium, which readily exchanges with hydrogen in As fusion engineering matures, links with academia outside of
compounds such as water, so is easily assimilated into living the usual fusion field will become increasingly important. Applying
organisms. This results in a need to carefully monitor for and con- the knowledge and lessons learnt from relevant fields will benefit
tain tritium to ensure environmental releases are minimised. the practical application of fusion technology.
Challenges include:
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