International Journal of Pressure Vessels and Piping 83 (2006) 336342

www.elsevier.com/locate/ijpvp

The interaction of mercury and aluminium in heat

exchangers in a natural gas plants
R. Coade *, D. Coldham
HRL Technology Pty Ltd, 677 Springvale Road, Mulgrave, Vic. 3170, Australia

Abstract
This paper reviews current understanding of mercury induced liquid metal embrittlement (LME) and the mechanism of failure in aluminium
heat exchangers. Natural gas can be contaminated with low levels of mercury, which can concentrate in cryogenic heat exchangers. There have
been several instances where LME has led to major failures and gas leakage in gas processing plant.
q 2006 Elsevier Ltd. All rights reserved.
Keywords: Liquid metal embrittlement; Mercury; Aluminium heat exchangers; Natural gas

1. Introduction

2. Natural gas processing to produce liquids

Liquid metal embrittlement (LME) is a complex metal

fracture mechanism that occurs without warning. Liquid
mercury has been known to have a potentially devastating
effect on aluminium for several decades [14], and the
accumulation of mercury in parts of natural gas plants has
led to failures. In the 1970s, LME and corrosion of aluminium
alloys by mercury in liquid natural gas (LNG) industry became
a cause for concern. A paper published in 1980 entitled
MercuryLNGS Problem [5] focussed on the potential risk
of failures and papers published in Proceedings of GPA Annual
Conventions and elsewhere in 1990s discussed failures of
components due to LME by mercury and on methods to combat
this [68].
The conditions required for LME to occur are:

The natural gas purchased by consumers consists almost

entirely of methane, the simplest hydrocarbon. In gas
reservoirs, however, methane is typically found with heavier
hydrocarbonssuch as ethane, propane, butane and pentane.
The raw gas also contains water vapour, hydrogen sulphide,
carbon dioxide, nitrogen and other gases that are removed from
the gas stream at processing plants.
In gas processing plants, hydrocarbons are separated
through fractionationbased on the different boiling points
of the hydrocarbons in the natural gas liquids (NGL) stream.
The liquids are cooled to temperatures around K50 8C and the
various fractions are separated as they boil off as the liquids
temperature is increased in stages in various heat exchangers.
This cryogenic distillation, separating ethane and heavier
hydrocarbons from sales gas (methane) occurs within cold
boxes, typically made from aluminium. An example of such a
coldbox is shown in Fig. 1.

(1) the presence of an embrittling liquid metalwith mercury

being a well-known, severe embrittling agent for
aluminium alloys,
(2) the presence of a stress above a threshold value, which can
be as low as 5% of the yield stress under some conditions
for aluminium alloys in mercury, and
(3) wetting of the substrate by the liquid metal, which in the
case of aluminium alloys requires rupture of the oxide film
between the substrate and liquid metal.
* Corresponding author.
E-mail address: rcoade@hrl.com.au (R. Coade).

0308-0161/$ - see front matter q 2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ijpvp.2006.02.022

3. Forms of Hg attack in aluminium heat exchangers

Mercury can occur in natural gas feed stock, often at very
low levels, and can sometimes accumulate in quantities
sufficient to cause severe attack and failure of cryogenic
aluminium heat exchangers. The cooling equipment in a gas
separation process is typically an aluminium plate-fin heat
exchanger, the construction of which is often an Al 3003 core
with Al 5083 or 6061 headers, nozzles and piping. The mercury
in the natural gas can degrade the aluminium coldbox materials
by three basic mechanisms [6]:

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337

Gordon [9] citing the early work of Pinnel and Bennett

[10,11] and Bruce and Wise [12] described the amalgamate of
Al and Hg as a white fibrous corrosion product identified as
either an amorphous form of g-Al2O3 or a form of hydrated
Al2O3 (alumina) or alumina hydroxide. Phannensteil et al. [13]
concluded that it was necessary for ions to be present in the
water for amalgam corrosion to occur. It is probable that these
ions destabilised the protective oxide layer allowing the
mercury to come in contact with the base metal.
Nelson [8] acknowledges that mercury can cause catastrophic attack of aluminium in the presence of free water,
however, suggests that in cryogenic heat exchangers the
presence of water is extremely unusual, and has not been a
factor in any reported leak occurrence.

(7)

(6)

3.3. Liquid metal embrittlement (LME)

Fig. 1. Schematic view of cryogenic heat exchanger showing the manifolds (6)
and nozzles (7).

3.1. Amalgamation
Amalgamation is the process by which mercury forms liquid
solutions with various metals, primarily Al, Au, Ag and Zn. In
the case of aluminium, the concentration of aluminium in the
amalgam is low and thus the depth of attack is limited.
Furthermore, aluminium is generally prevented from contact
with mercury by the Al2O3 protective surface oxidefor the
amalgam reaction the mercury must wet the aluminium metal
surface. The oxide on aluminium is not homogeneous and
contains numerous defects, but in general mercury will not
migrate through these microscopic cracks and defects to reach
the underlying metal. However, if the extent or severity of such
defects is increased by thermal or mechanical stresses, abrasion
or some chemical environments there is increased risk of
mercury damage.
3.2. Amalgam corrosion
Amalgam corrosion is the combined action of mercury and
moisture producing a corrosion process that propagates with
miniscule amounts of mercury. The reaction is:
Hg C Al/ HgAl amalgam

(1)

HgAl C 6H2 O/ Al2 O3 $3H2 O C 3H2 C Hg

(2)

Small amounts of aluminium can dissolve in liquid mercury,

diffuse to the mercurymoist air interface, and then rapidly
oxidize. Since, oxidation removes aluminium from the
mercury, further aluminium can dissolve, and the process can
continue until the aluminium is completely converted to oxide.
In practice, voluminous oxide whiskers and deep pits are
observed. Rapid oxidation requires the presence of moisture,
and reaction rates are slow in its absence.

LME of Al alloys by mercury is one example of a generic

phenomenon in which many (but not all) metals are embrittled
by certain liquid metals [14]. For example, mercury embrittles
not only Al alloys but also Cu, Ti, Ni, Fe, and Zn alloys, but
does not embrittle Mg alloys [15]. Al alloys are also embrittled
by, for example, liquid Ga, In, Pb, Sn, Cd, and Na. There are
several types of LME (with different mechanisms), but most
cases involve only adsorption of embrittling atoms at stressed
surfaces and crack tips, i.e. no diffusion of embrittling atoms
into the material or ahead of crack tips is involved [16,17]. The
Al:Hg system falls into this category and, hence, other types of
LME are not considered here.
LME is generally much more severe than other embrittling
processes, such as hydrogen-embrittlement or stress-corrosion
cracking, and once cracks have initiated, very rapid sub-critical
cracking can occur even at low stresses (stress-intensity
factors) [18]. Cracking occurs preferentially along grain
boundaries for the Al:Hg couple (and for many other couples),
but transgranular (cleavage-like) fractures can also occur.
Liquid metals are drawn into growing cracks so that the crack
tip is always in contact with embrittling metal atoms. (The ratecontrolling process for cracking is still being debated, but the
rate of flow of liquid within cracks may control the rate of
cracking in some circumstances.)
Adsorption of embrittling atoms at crack tips weakens
substrate interatomic bonds, and facilitates crack growth by
enabling interatomic bonds to break or shear more easily than
in inert environments. Preferential adsorption at grainboundary/surface intersections results in the preference for
intergranular fracture. Much less plasticity is associated with
fracture in liquid metal environments than in air, and fracture
surfaces can be featureless or can exhibit small, shallow
dimples, whereas large deep dimples are produced by fracture
in air. Thin films of liquid metal are left behind the advancing
crack tip and, hence, fracture surfaces are covered with a film
of liquid metal. For the Al:Hg system, de-wetting can occur
so that small globules of mercury are present on fracture
surfaces. The presence of mercury on fracture surfaces can also
result in the growth of oxide whiskers after fracturea

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phenomenon peculiar to aluminium and discussed in the

preceding section.
For LME cracks to initiate there must be intimate contact
between liquid and solid metals, with no intervening oxide
films to prevent wetting and adsorption. Al alloys are covered
by a thin, protective oxide film, and surfaces can be covered by
liquid mercury indefinitely without any reaction until the oxide
is damaged. Oxide films can be broken by mechanical
processes, e.g. by scribing or abrasion, by chemical processes,
e.g. corrosion, or by plastic deformation of the aluminium
resulting in slip steps at the surface. Slip processes can occur
locally in favourable oriented grains at stresses well below the
macroscopic yield stress, and slip steps can emerge at the
surface after long times under stress due to creep processes
(thermally activated dislocation re-arrangements) beneath the
surface.
The time required for slip-step/oxide-rupture events will, of
course, decrease with increasing stress and, hence, times to
LME initiation will also decrease with increasing stress. The
kinetics of LME crack initiation and growth depend not only on
stress (or stress-intensity factor) but also on many other
variables such as the composition of the liquid, the amount of
liquid, the composition, microstructure, and strength of the
substrate alloy and temperature [19].
The amount of liquid metal is important for several reasons.
Firstly, increasing surface coverage of the substrate by the
liquid metal could decrease the time to crack initiation, since
the probability of potentially weak sites in oxide films exposed
to the liquid would be increased. Secondly (and more
importantly), cracks can run out of liquid metal if there is
only a limited supply because films of liquid metal are left on
fracture surfaces behind crack tips. Crack-arrest can therefore
occur providing the stress-intensity factor, K, is below the
critical K for fast fracture in the absence of environmental
effects.
Cryogenic heat exchangers are often manufactured from
aluminium alloy 5083, an aluminiummagnesium alloy.
Magnesium silicide can contribute to age-hardening in these
alloys. At room temperature, aluminium can hold w1% Mg in
solution although heat exchanger alloys typically contain 4.5%
Mg. The aluminium rolling mills anneal this material at
w455 8C to dissolve all the Mg. Then the rolled stock is
quenched to room temperature to hold the magnesium in solid
solution. This results in a metastable solid solution that wants
to precipitate Al3Mg2. The kinetics of precipitation is so slow
at room and cryogenic temperatures, that for all practical
purposes, the alloy is stable.
However, when the alloy is welded, the temperature of the
heat affected zone can facilitate the precipitation of Al3Mg2.
This can result in a continuous or semicontinuous film of
Al3Mg2 being precipitated at the grain boundaries. The weld
structure is also subject to grain boundary precipitation because
of the solidification pattern and reheat from multi-pass welds.
Alloy composition and temper can affect LME through
effects on strength, and grain-boundary microstructure (and
grain-boundary composition if segregation occurs), which can
affect creep rates and strain localization (hence, oxide-rupture),

and adsorption kinetics. Alloy strength is particularly

important, and increasing strength can either decrease or
increase susceptibility to LME depending on the circumstances. Crack growth rates generally increase, and threshold K
values for cracking generally decrease, with increasing
strength [20].
Specific data for welded 5083-0 alloy in liquid mercury at
20 8C show that threshold K values are somewhat lower for
5183 weld material with an equiaxed microstructure than for
the 5083 plate (in the T-L orientation), although the crack
growth rate was somewhat higher for the latter for some K
values [21,22]. Limited data on the times to failure for the
welded 5083-0 alloy stressed in mercury at 20 8C show that
failure can occur in less than 1 h at high stresses (70% of yield),
and that there is considerable scatter with other similarly
stressed specimens lasting for w20 h. Failures occurred after
hundreds of hours at low stresses, with the threshold stress for
cracking being perhaps only w10% of the yield stress.
4. Breaching the aluminium protective oxide
For LME cracks to initiate there must be intimate contact
between liquid and solid metals, with no intervening oxide
films to prevent wetting and adsorption. Al alloys are covered
by a thin, protective oxide film, and surfaces can be covered by
liquid mercury indefinitely without any reaction until the oxide
is damaged. Oxide films can be broken by mechanical
processes, e.g. by scribing or abrasion, by chemical processes,
e.g. corrosion, or by deformation of the aluminium resulting in
slip steps at the surface.
In LNG plant, Gordon [9] favours the abrasion on the
surface by hard particles in the gas or liquid streams as the key
oxide breaching mechanism. He suggests that as the gas
entering cryogenic equipment usually consists of mainly
methane, CO2 and hydrogen, it is oxygen-free. Hence, the
reducing atmosphere of the gas stream may prevent any
reformation of the protective oxide layer once damaged from
hard particles in the gas stream has occurred.
Others suggest that the differential thermal expansion
between the aluminium substrate and the alumina oxide
being a factor of around 3 could cause the oxide to crack
when the heat exchangers is warmed.
It is known that slip processes can occur locally in
favourably oriented grains at stresses well below the
macroscopic yield stress, and slip steps can emerge at the
surface after long times under stress due to creep processes
(thermally activated dislocation re-arrangements) beneath the
surface. It is possible that such activity could lead to breaks in
the oxide film. The time required for slip-step/oxide-rupture
events will, of course, decrease with increasing stress and,
hence, times to LME initiation will also decrease with
increasing stress.
5. Metallography of LME cracking in heat exchangers
The coldbox on a cryogenic heat exchanger typically
includes a distribution manifold with several nozzles from

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339

the inlet manifold connected via headers to the heat exchanger

core. The manifolds are manufactured from seam welded pipe
and circumferential welds attach flanges. LME can lead to
extensive delamination cracking in the manifold itself, and also
cause extensive intergranular cracking in the field circumferential welds [23]. Some typical examples of such damage are
considered in the following paragraphs.
In one case, LME led to cracking and failure in the manifold
just downstream from the flange, and involved cracking along
the longitudinal axis of the pipe at about the 6 oclock position
for about 300 mm. There was an exceptional amount of
secondary cracking in many directions leading to the
detachment of substantial pieces of material and to major
delaminations parallel to the surface of the pipe. LME cracking
also ran around the circumferential weld area.
Examination of fracture surfaces showed that (i) there were
no shear lips or other macroscopic signs of ductility for any of
the cracks, (ii) all fracture surfaces were intergranular, and (iii)
all fracture surfaces were contaminated with small globules of
liquid mercury and oxide whiskers characteristic of mercurywetted aluminium surfaces.
The longitudinal fracture surface was textured and directional,
with numerous delamination cracks running normal to the
fracture surface, as shown in Fig. 2. This cracking extended for
Fig. 3. Section showing multiple cracking near the surface of the longitudinal
fracture and near the end of the delamination crack. 165!.

some distance, in some areas greater than 50 mm deep, and the

cracking became branched, as shown in the micrographs in Fig. 3.
The length of the delamination cracking varied with
position. The cracks could deviate from the delamination

Fig. 2. Photograph showing the surface of the longitudinal crack and the
delamination cracks, which are more visible in the macroscopic view of a
section through the primary crack after polishing showing the nature and length
of cracking.

Fig. 4. Examples of delamination cracking that has deviated and intersected the
internal surface, with alumina whiskers clearly exposing the cracks.

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Fig. 5. Macroscopic view of a section through the circumferential weld

showing extensive branched intergranular cracking.

plane and intersect the internal surface of the vessel. In this

case, as the cracks were exposed to moist air they become
delineated with aluminium oxide whiskers, as can be seen in
Fig. 4
All cracks and fracture surfaces were found to be
contaminated with mercury and/or oxide whiskers consistent
with mercury induced corrosion. The presence of mercury on
the fracture surfaces, the intergranular nature of cracking and
the multiplicity of the cracking suggested a liquid metal
embrittlement phenomenon.
The circumferential weld metal is equiaxed and appears to
be more susceptible to intergranular cracking than does the
parent material in the manifold. This could be accentuated by

Fig. 6. Cracks at the outer surface of the circumferential weld and within the
weld showing extensive branched intergranular cracking. 100!95/141!.

the presence of grain boundary precipitation although it is more

likely to be a result of a structure that presents fewer barriers to
crack movement than the heavily textured manifold. Secondary
cracking within the circumferential weld is typically branched,
following the equiaxed grain boundaries. An example of cracks
within the circumferential weld is shown macroscopically in
Fig. 5.
The very branched nature of the cracking associated with
the circumferential weld is shown in Fig. 6, indicating the
equiaxed grain structure of the weld. The section through the
weld perpendicular to the longitudinal crack path shows
the growth of secondary cracks from the primary crack face
extending towards the outer surface, indicating a growth of the
primary fracture from the inner to the outer surface.
6. Fractography
Aluminium fracture surfaces can be cleaned in concentrated
nitric acid to remove corrosion product, contaminant and
mercury without damaging the surface. After cleaning the
surfaces could be examined in the scanning electron
microscope. Although traces of corrosion product remained,
key features of the fracture could be resolved.
The surface of the fracture through the circumferential weld
revealed a grain structure and some intergranular cracking as
can be seen in Fig. 7. It can be seen that although there is no
indication of extensive deformation, as would be expected in
intergranular LME cracking, there is micro-ductility as
indicated by the localised dimpled appearance across the

Fig. 7. Fracture surface of cracking in the circumferential weld showing the

intergranular and branched nature of cracks.

R. Coade, D. Coldham / International Journal of Pressure Vessels and Piping 83 (2006) 336342

Fig. 8. Longitudinal fracture surface at the top of one of the ridges showing
lamellar cracking and a more detailed views of the substructure of the fracture
showing additional cracking across the lamellar cracking and tearing with some
boundaries visible and possible sites where second phase particles have been
removed.

grain face. The cracking had a similar intergranular appearance

at the outer surface in this region also but this was perhaps not
as pronounced as indicated in the photographs at the ID
surface.
The longitudinal crack in the manifold extended for nearly
300 mm from the circumferential weld, and various sections of
the longitudinal fracture surface were examined to identify any
differences in the fracture mode along the failure path.
Fig. 8 shows the appearance at the top of one of the ridges
mid-way through the thickness. The higher magnification
views show some micro-ductility across the grain faces.

7. Discussion
Liquid metal embrittlement and cracking of aluminium
alloys by mercury requires the presence of mercury in the
liquid state, tensile stress above a threshold value, which can be
as low as 5% of the yield stress under some conditions for
5083-0 aluminium alloys in mercury, and wetting of the
aluminium substrate by the liquid metal, which requires rupture
of oxide films between the substrate and liquid metal. The
fracture surfaces exhibited droplets of mercury throughout, and
these occur after superficial oxidation leads to de-wetting of the
surface. Associated with this is the formation of alumina
whiskers. Both these features when observed on fracture
surfaces provide strong support for LME as the failure
mechanism.

341

In natural gas processing plants considerable quantities of

mercury can collect in the cryogenic heat exchangers. The
substantial amounts of mercury are derived from traces of
mercury present in natural gas and this can condense and
collect in cold parts of the system if it is not removed in
upstream filters. Typically the mercury would condense onto
surfaces in the solid form (i.e. at temperatures less than
K39 8C) and would only melt during shut down periods when
it would be expected to collect in low points in the manifolds
and pipework in the heat exchanger system.
The key issue for LME is the simultaneous breaching of the
protective alumina layer in the presence of liquid mercury.
Stresses due to internal pressure alone would generally be
above the threshold values for LME. In addition, there are
significant bolting stresses near the flange of the distribution
manifold and residual stresses from welding, resulting in
stresses that could approach the yield stress in this area. Weld
material (with equiaxed grains) is more susceptible to LME
than the pipe material (with elongated grains and a lessfavourable intergranular crack path for the relevant crack-plane
orientation). Thus, the high stresses near the weld, more
susceptible weld material, and the potential for mercury to pool
in this region if it is a low spot indicates that LME crack
initiation could occur at the weld.
Rupture of the protective aluminium oxide film, allowing
intimate contact between mercury and aluminium, is most
likely to be caused by slip-bands intersecting the surface due to
micro-yielding and creep processes. This might occur under the
high, sustained pressure and residual stresses but in most
instances is probably accentuated by superimposed thermalstress from transient operations and potentially from piping
induced loads.
At high stresses, the oxide-rupture process can sometimes
occur rapidly (!1 h) and can sometimes take considerable
time (O100 h) under nominally the same conditions, for
reasons that are not well understood.
Once cracks have initiated, crack growth in 5083-0 in liquid
mercury can occur very rapidly (up to tens of millimetres per
second)the time to failure is therefore determined by the
time for cracking to initiate. The variability in crack initiation
times can explain why in some LNG processing plant one
manifold might be extensively cracked, whereas a parallel
manifold might not exhibit any cracking (despite containing
mercury and being subject to similar stresses).
It is the largely varying times to crack initiation and the
potentially rapid growth of these cracks once initiated, that
makes the non-destructive inspection for Hg induced LME
problematical. For example, ultrasonic crack detection requires
the plant to be off-line and the cladding removed, and only then
can find cracks once initiated and before they have grown to a
critical size. Radiography can locate areas where Hg is
accumulating providing an opportunity to locally remove the
Hg or to inspect these regions, but while radiography will
clearly show cracks infiltrated with Hg, where such infiltration
occurs, failure is imminent. Hence the non-destructive
inspection for Hg induced LME is quite difficult, suggesting

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that the less well known techniques such as acoustic emission

may be worthy of further investigation for such plant.
The extent of cracking is known to depend, inter alia, on the
amount of mercury present, and cracks can run out of
mercury and arrest when only small quantities are present.
Large quantities of mercury known to be present in some gas
fields increase the likelihood of failures if there is no mercury
removal process upstream of the cryogenic heat exchangers.
Most reported instances of mercury induced cracking have
apparently involved relatively small amounts of cracking,
resulting in leaks rather than bursts, probably because there
were only small amounts of mercury present.
Modern LNG plant incorporates various mercury removal
systems, upstream from the cold boxes of the cryogenic
distillation plant to minimise the risk of LME. Cold box
manifolds can be manufactured from aluminium alloys and
tempers that are less susceptible to LME.
8. Conclusion
Liquid mercury in contact with aluminium can induce
serious and rapid failures. Mercury at relatively low
concentrations in natural gas can concentrate in the cryogenic
distillation process. If mercury is present in the liquid form
(e.g. during process interruptions or plant shut down) it can
cause catastrophic damage in aluminium heat exchangers in
LNG plant. The cracking can occur without warning, and
because of the rapid rates of LME crack growth there is no
adequate non-destructive testing techniques to safely monitor
and protect plant.
Mercury induced LME in aluminium alloys leads to
intergranular cracking and potentially very widespread damage
in heat exchange manifolds. Cracking surfaces are characteristically covered with droplets of mercury and in most cases
alumina whiskers are found to grow from cracks.
Acknowledgements
The author wishes to thank Mr Stan Lynch from DSTO for
his assistance in the preparation of this paper.
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