Cement and Concrete Composites 122 (2021) 104111

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Cement and Concrete Composites

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

Visualization of mercury percolation in porous hardened cement paste by

means of X-ray computed tomography
Yuxuan Qi a , Kangxin Liu a , Yu Peng a , Jiyang Wang a , Chunsheng Zhou b , Dongming Yan a ,
Qiang Zeng a ,∗
a
College of Civil Engineering and Architecture, Zhejiang University, Hangzhou 310058, PR China
b School of Civil Engineering, Harbin Institute of Technology, Harbin 150090, PR China

ARTICLE INFO ABSTRACT

Keywords: Mercury intrusion porosimetry (MIP) has been extensively used for the pore structure characterization of
Mercury intrusion porosimetry porous materials, but the percolation of mercury in porous cement-based materials during MIP has never been
X-ray computed tomography comprehensively investigated before. Here we visually probe the mercury percolation in a porous hardened
Percolation
cement paste (HCP) using X-ray computed tomography (X-CT). Novel double surface coatings on the HCP
Hardened cement paste
samples before and after MIP tests by an epoxy resin are specifically designed. The first coating enables the
Pore structure
one-directional penetration of mercury in the HCP samples during MIP, while the second coating can partially
seal the release of the entrapped mercury. MIP tests are operated under different maximum applied pressures
(10,000 and 30,000 psi) and equilibrium time (5, 10, and 30 s). The high X-ray attenuation of mercury enables
the visual trace of the intrusion mercury percolation pathways and the entrapped mercury clusters in the
HCP samples by X-CT. The position-dependent entrapped mercury clusters in the pores account for the gray
value changes and gradients in the HCP samples after MIP. The MIP characteristics, such as, total intrusion
volume, volume size distribution and mercury entrapment, change with the maximum applied pressure and
equilibrium time, but the percolation pore size shows the consistent values. The findings of this work deepen
the understandings of MIP for the microstructure characterization of porous materials.

1. Introduction pore networks in porous materials. It is generally accepted that the

Mercury intrusion porosimetry (MIP) is a popular technique to
characterize the pore structure of cement-based materials (CBMs). Com-
pared with other porosimetries, like gas (nitrogen, argon, carbon diox-
ide and water) sorption and image analysis, MIP shows several ad-
vantages, such as, low cost, simple physical principle, fast operation,
relatively large sample size, and broadly accessible pore range (depend-
ing on the maximum pressures applied) [1–5]. However, debates on
MIP are always mentioned by scholars due to the possibly biased pore
results induced by several intrinsic and extrinsic factors, including: the
effects of sample size and surface roughness [2,6,7], the effect of sample
pretreatment (drying) [8,9], the oversimplifications of pore topology
(geometry and connectivity) and interpretation parameters [10–17],
the material deformations and damages under high pressures dur-
ing mercury intrusion [18–22], and the assumption of static testing
processes [23–25].
Almost all MIP tests in open literature are conducted under high
maximum pressures that allow the complete percolation of mercury
through some narrow throats that contribute to form the connected
pores at the greatest mercury rises are identical to the threshold size
for mercury percolation through which continual mercury flows oc-
cur [26]. In a previous study by Thompson et al. [27], significant
electric resistance shifts occur at the mercury injection (intrusion) shifts
for porous rocks, which indirectly evidences the mercury percolation
processes in porous media. The pore parameters determined by mer-
cury injection percolation are important for permeability prediction,
and the quantitative permeability-pore relationship is known as the
Katz–Thompson (KT) equation [28]. Over the past thirty four years,
the KT equation has been popularly used to predict the permeability
of different types of porous materials [29–33], and mercury intru-
sion might be one of the benchmark porosimetries for pore structure
characterization [34,35].
Researches on the percolation of mercury intrusion under pressure,
however, are rather limited. Some computer simulations may enable
the virtual injections of mercury in fixed lattices (representing pore
spaces in limited scales), which may facilitate to explore the percolation
process of mercury intrusion [23,24,36]. The relevant experimental

∗ Corresponding author.
E-mail address: cengq14@zju.edu.cn (Q. Zeng).

https://doi.org/10.1016/j.cemconcomp.2021.104111
Received 4 August 2020; Received in revised form 31 March 2021; Accepted 17 May 2021
Available online 25 May 2021
0958-9465/© 2021 Elsevier Ltd. All rights reserved.
Y. Qi et al.
work is rarely documented. This must come from the difficulties in
experiments for probing mercury intrusion in porous materials. An
obvious difficulty is that mercury can easily evaporate and is poi-
sonous to humans, so the mercury-intruded sample is not suitable for
microscopic observation. Alternatively, the intrusion of low melting-
point metal is often combined with scanning electron microscopy (SEM)
to measure the pore structure of CBMs [37–42]. This method, albeit
feasible, only acquires 2 dimensional intruded pores in CBMs that
are intrinsically different from the real pores with heterogeneously 3
dimensional spacial structure.
Driven by the continual developments of advanced experimen-
tal methodology, e.g., X-ray computed tomography (X-CT), the non-
destructive microstructure (and transport properties) characterization
of porous materials in multi scales is progressively realized [43–51].
X-CT and MIP tests are often combined in parallel to investigate
the microstructure of CBMs in different scales. For instance, Xue
et al. [52] used micro X-CT and MIP to jointly assess the degradation
of cement mortars under thermal actions. The coupled X-CT and MIP
tests, however, are rarely reported. Previous studies implied that the
combination of X-CT and MIP helps better understand the MIP testing
process [7,18,34,53–56]. This relies on the fact that mercury has
the dramatically higher X-ray attenuation than any phase in ordinary
porous materials [57]. The tracks of mercury entrapped in the pores of
a porous material not only visually testify porosity variation at different
material positions, but also provide information on transport pathways
that are hardly obtained by other means [53]. Within the same regime,
Rigby and coworkers has performed visual examinations on the entrap-
ment of mercury in porous silica [54] and directly detected the spatial
configurations of pore chambers with mercury entrapment connected
by percolation paths in macro porous alumina by micro-X-CT tests [55].
It was suggested that micro X-CT scanning, in association with MIP,
can detect pores and fractures two orders of magnitude smaller than
voxel resolution and will strongly improve 3D spatial analysis of low
porosity rock texture [56]. Our recent study proved that X-CT scans
can quantitatively assess the pore structure damages of CBMs during
the intrusion of mercury under high pressure [18]. The combination
of X-CT and the intrusion of low-melting point metals (e.g., Woods
metal [58] and other bismuth-based alloys [41,42]) was also applied
to characterize the pore structure of various porous materials.
While the combination of X-CT and MIP facilitates to unravel the
mercury entrapment in porous materials that indirectly reflects the
transport paths, difficulties in the controls of mercury intrusion patterns
always exist. For example, porous samples with and without surface
coating may show different mercury intrusion patterns and MIP pore
spectra [59]. Furthermore, the partial surface coatings on HCP samples
can depress the surface roughness (or surface conformance) effect
and decrease the threshold pore size (TSP) [7]. Therefore, elaborate
surface coatings on porous samples are expected to help manipulate
the direction and pattern of mercury intrusion. This would provide
a preferable way to possibly trace the mercury intrusion percolation
pathways in porous CBMs. Despite the percolation of pore networks and
the formation of mercury entrapments in ’ink-bottle’ pores have been
virtually studied with statistical and molecular simulations [23,24], the
directly experimental visuals, to the best of the authors’ knowledge, are
still absent.
This work aims to fill the blank of the visual reports of mercury
percolation in the interconnected pore system of a porous HCP. A new
testing scheme is proposed to control the intrusion directions and pat-
terns. Specifically, double coatings on HCP cylinders are applied before
MIP and X-CT tests. This is an improve experimental scheme based on
our previous studies [18,34], where the first coating step to control
the intrusion patterns of mercury during MIP tests was not considered.
Two maximum intrusion pressures (10,000 and 30,000 psi) and three
equilibrium time (5, 10 and 30 s) are adopted to control MIP tests. The
mercury clusters entrapped in the pores of the HCP are probed by X-CT
measurements. Profound discussions are then performed to deepen the
understandings of mercury intrusion in the pore system of HCP.
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Cement and Concrete Composites 122 (2021) 104111
2. Experiments
2.1. Material and specimen preparation
A white Portland cement (P. W. Grade 52.5) (Aalborg Portland
Group, Anqing, China) was adopted as the only binder to synthesize the
HCP specimens. The bulk oxide compositions, density, and the Blaine
fineness of the cement are listed in Table 1. A water-to-cement (w/c)
ratio of 0.35 was designed in the mix. A high-efficient water reducer
(MasterGlenium® , Basf, Shanghai, China) was mixed with the cement
by 3wt% to get the high fluidity of paste slurries. This water reducer
dosage is much higher than that used in practical concrete to grantee
the injection of paste slurries into thin tubes.
Manual mixing and stirring were operated in a beaker to prepare
the white cement paste slurries. A syringe was used to inject the
paste slurries into thin plastic tubes with the inner diameter of 3 mm
(Fig. 1a). The paste-filled plastic tubes in different lengths were then
fixed on a polystyrene foamed plastic board (Fig. 1b). Later, this board,
together with the plastic tubes, was stored in a vessel at the temperature
of 20 ± 2 ◦ C and relative humidity over 95% for continual curing. After
28 d, paste cylinders of 3 mm in diameter were demoulded from the
tubes.
Cylinders in length of 20 mm were selected and oven dried at 50
◦ C for 48 h for removing the physically absorbed and/or confined
water [60]. The oven-dried cylinders were then coated with a quick-
hardening epoxy resin (termed as the first coating) (Fig. 1c). MIP tests
on those epoxy-sealed paste cylinders cannot be conducted because
no open surfaces are available for mercury penetrations. Therefore an
Abrasi-Met 250 manual cutter was used to cut each long cylinder into
two half cylinders with equal length (10 mm) and one open end.
The HCP cylinders then experienced the first X-CT test (Fig. 1d).
Later, MIP tests were conducted (Fig. 1e). Once the MIP tests com-
pleted, the samples were immediately removed into plastic tubes (5 mm
of inner diameter). The pre-mixed quick-hardening epoxy resin was
then poured into the tubes to seal the samples as quickly as possible
(termed as the second coating). This step was to prevent the leakage of
mercury into the air, because mercury is highly evaporable at room
temperature and is toxic to humans. The coatings of samples after
MIP was recommended for the lab-safety based on our experimental
experiences [7,18,34]. After the epoxy resin in the tubes was hardened,
the paste cylinders with double coats were readily prepared for the
second X-CT tests to probe the spatial positions of the mercury intruded
in the samples (Fig. 1e).
2.2. Test procedure
2.2.1. MIP tests
A MIP device of Micromeritics AutoPore IV 9510 (Micromeritics
Instrument Corporation, USA) was used for MIP tests. Two different
maximum pressures, i.e., 10,000 and 30,000 psi (corresponding to 68.9
and 206.8 MPa, respectively) and three different equilibrium time,
i.e., 5, 10 and 30 s, were applied. Accordingly, samples were labeled
as MaxPressure-EquilTime-W/C (Table 2). By taking the Washburn
equation [25] and the commonly used physical parameters of mercury,
i.e., the contact angle of 130 degree and the surface tension of 485
mN/m [4], the minimum accessible pores under 10,000 and 30,000 psi
were estimated as 18 and 6 nm, respectively. The intruded pore volume
in terms of the equivalent pore size can be displayed in the cumulative
and differential PSD spectra.
2.2.2. X-CT tests
X-CT scans were conducted in an industry device of XTH255/320
LC (Nikon, Japan) with the X-ray source of 225 kV. Two X-CT tests to
each sample before and after MIP were performed. For the first X-CT
test before MIP, three HCP cylinders were bundled up to form a bigger
specimen (see the inset panel of Fig. 1d). This operation was designed
Y. Qi et al. Cement and Concrete Composites 122 (2021) 104111

Table 1
Chemical component and physical properties of the white cement.
Chemical composition Content Physical properties Value
Silica (SiO2 , %) 24.75 Density (kg∕m3 ) 3.10
Alumina (Al2 O3 , %) 1.91 Specific surface area (m2 ∕kg) 380
Calcium oxide (CaO, %) 69.21
Iron oxide(Fe2 O3 , %) 0.30
Magnesium oxide (MgO, %) 0.56
Sulfur trioxide (SO3 , %) 2.10
Sodium oxide (Na2 O(eq), %) 0.16
Others 0.30
Loss on ignition (LOI, %) 0.71

Table 2
Sample nomenclatures and MIP testing parameters.
Sample ID Maximum intrusion pressure Minimum accessible Equilibrium time (s)
(psi [MPa]) pore size (nm)
1-5–035 10,000 [68.9] 18 5
1-10–035 10,000 [68.9] 18 10
1-30–035 10,000 [68.9] 18 30
3-5–035 30,000 [206.8] 6 5
3-10–035 30,000 [206.8] 6 10
3-30–035 30,000 [206.8] 6 30

Fig. 1. Sample preparation and testing procedures: (a) injection of paste slurries into plastic tubes (inner diameter of 3 mm); (b) setting of the tubes on a polystyrene foamed
plastic board; (c) coating of paste cylinders (20 mm in length) after oven drying with a layer of quick-hardening epoxy resin; (d) the first X-CT test; (e) MIP test; and (f) the
second XCT test.

to save the machine time (i.e., one test for three samples) without (Fig. 1f). For both X-CT tests, a slow rotation rate of the platform (12
loss of resolution. For the second X-CT test after MIP, X-ray scans degree/min) was set to ensure the high quality of two-dimensional (2D)
were conducted on each individual HCP cylinder fixed on the platform phase contrast images. The exposure time for a single projection was

3
Y. Qi et al.
Fig. 2. X-ray projections of the HCP samples after MIP tests with different applied pressures and equilibrium time: (a) 1-5-035, (b) 1-10-035, (c) 1-30-035, (d) 3-5-035, (e)
3-10-035, and (f) 3-30-035. The panels of (d-1) and (f-1) display the local phase contrast tomographic images of the 1-30-35 and 3-30-35 samples, respectively.
1 s and, totally, 1800 projections were generated for completing the
scans by 360 degrees in 30 min. The acceleration voltages of 150 kV
and 155 kV were, respectively, applied to deliver the X-ray beams to
penetrate through the HCP samples before and after MIP test. To further
filter out low-energy X-rays and reduce the beam hardening artifacts,
a 0.5-mm-thick copper plate was positioned between the X-ray source
and the sample. The penetrated X-rays were probed by a high-sensitive
detector (DRZplus Scintillator with the pixels of 2000(h)×2000(v)) at
the back of the objects synchronously.
The collected data were first read by CTPro to primarily screen qual-
ity of the projections. The projections in high quality were imported
into an image-processing software (VGStudio, Version 3.1) for subse-
quent image processing and analysis. The typical 2D pixel resolution
was 7 μm. Region of interest (ROI) or volume of interest (VOI) would
be selected in necessary for microstructure analysis.
3. Results and discussion
3.1. X-ray projections
Fig. 2 shows the representative X-ray projections of the HCP samples
after MIP tests with different applied pressures and equilibrium time.
The dark color represents the mercury drops that are either entrapped
in the HCP samples or released to the epoxy coats. Directly and obvi-
ously, only part of the 1-5-035 sample has been intruded by mercury
under the maximum pressure of 10,000 psi and the equilibrium time of
5 s (Fig. 2a). The other samples, however, show the dark color nearly
over the entire areas, suggesting the relatively homogeneous mercury
distributions after MIP tests (Fig. 2b-f). The ganglia-like structures in
Fig. 2a represent the percolation paths in the HCP sample. The direct
visual examination of the mercury percolation paths is feasible for 1-
5-035, because the gray value differences between the intruded areas
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Cement and Concrete Composites 122 (2021) 104111
and the rest areas are significant (see the supplementary figure S1 for
the gray value distributions of a local area), However, for the other
samples, visual examination is not valid owing to the insufficient gray
value gradients (see the supplementary figure S2 for the gray value
distributions of a local area). The gradient distributions of the mercury
drops in 1-5-035 also directly provide the percolation directions. Rigby
et al. [55] reported the percolation pathways in macroporous alumina
materials after a complete MIP test under high pressure as well, but
failed to provide the percolation directions. Fig. 2a, to the best of the
authors, may provide the first visual demonstration of the percolation
paths of mercy intrusion in the pore network of HCP.
Fig. 2 also displays that part of the mercury has intruded into the
first epoxy coating layer. Indeed, the small dark circles (see for instance
Fig. 2c-1 and f-1) represent the tiny mercury drops entrapped in the first
epoxy layer around the side surface of each HCP body. By identifying
those mercury drops, one can separate the first coating layer from
the epoxy resins that show the light gray color in the images. For
example, the thickness of the first epoxy layer is estimated as 0.6 mm
for the 1-30-035 sample (Fig. 2c-1). A part of the mercury near sample
surfaces may release to the second epoxy layer before it is hardened.
The released mercury accumulates, forming big mercury drops; see the
big dark circles shown in Fig. 2.
3.2. Effect of mercury intrusion on gray value distributions
The voxel-gray value (VGV) distributions of the HCP samples are
used to measure the changes of X-CT images, because the voxel number
of an object is a scale to measure its size or volume (under a certain
voxel resolution), and the gray value reflects the X-ray attenuation
when X-ray beams penetrate through this object. Generally, a high
voxel number at low gray value represents a large phase with low X-ray
attenuation (e.g., the pores, cracks, lightweight phase in CBMs). This
Y. Qi et al.
Fig. 3. Voxel-gray value spectra of the HCP samples before and after the MIP tests with the maximum applied pressures of (a) 10,000 and (b) 30,000 psi and the equilibrium
time of 5, 10 and 30 s.
is the regime to quantitatively characterize different phases in CBMs
by X-CT [44,52]. Fig. 3 shows the VGV spectra of the HCP samples
before and after the MIP tests with different testing conditions. When
operating the VGV analysis, the selected VOIs are slightly smaller than
the real sample bodies, so the epoxy coatings can be excluded. The
details of VOI selection are shown in the supplementary figure S3.
Several features can be figured out. First, the dual-peak VGV spectra
before MIP reduce to the single-peak ones after MIP. For the HCPs
before MIP, the peaks at low gray values represent the pores with lower
X-ray attenuation (see the shadowed areas shown in Fig. 3), whereas
these at high gray values denote the solid phases (unhydrous cement
clinkers and hydration products) with higher X-ray attenuation. For
the HCP samples after MIP, the pores have been partially filled with
mercury, so the VGV peaks of the pores disappear. The gray values
of the solids and the pores partially filled with mercury may merge
together to form the single-peak VGV spectra. Second, the operation
of mercury intrusion greatly augments the gray values and broadens
the VGV spectra of the HCP samples. All the spectra shift from left
(low gray value area) to right (high gray value area), and the spectra
width is substantially enlarged (Fig. 3). Those observations are the
consequences of mercury intrusion in the HCP bodies. The intruded
mercury drops augment the gray values by raising the X-ray attenuation
on one hand, and eliminate the peaks at low gray values by partially
filling the empty pores on the other hand.
If HCP samples with higher porosity are used, dual peaks may
still appear, but the first peak (empty pores) at the lower gray value
region for the samples before MIP transforms to be the second peak
(entrapped mercury) at the higher gray value region for the same
samples after MIP. In short words, MIP can induce the exchange of
5
Cement and Concrete Composites 122 (2021) 104111
VGV peak positions. This feature has been used for pore structure
characterization by tracing the mercury drops entrapped in the pores
of HCP samples with/without surface conformance control [7], and
for pore damage assessment by quantifying the pore sizes of HCP and
mortar samples before and after MIP [18]. In this work, the dual peaks
of VGV spectra for the samples after MIP are not observed (Fig. 3)
because of the limited intrusion of mercury in the HCP with densely
compacted microstructure at low w/c ratio (W/C=0.35).
In order to better demonstrate the gray value changes induced by
mercury intrusion, local sectional analysis is performed. As an example,
Fig. 4 comparatively displays the sectional X-CT images of the 1-10-
35 sample before and after MIP. It is clear that the large dark areas
inversely change to the bright ones after MIP test (Fig. 4a and d). A gray
value analysis is performed on an ROI (327 × 374 pixels) for specific
demonstration (Fig. 4b and e). Before MIP, the ROI shows a rough
surface plot of gray values with the mean gray value of 140/255. A pit
with the gray value down to 40/255 and a bulge with the gray value up
to 180/255, respectively, represent a pore and an unhydrated cement
clinker (Fig. 4c). After MIP, the surface plot of gray values changes
greatly. Several gray value peaks, that represent the entrapped mercury
drops, appear in the plot, resulting in the sharply enhanced surface plot
roughness (Fig. 4f). Owing to the gray value rises by mercury intrusion,
the unhydrous cement clinkers are not detectable any more (Fig. 4d and
e).
It is noteworthy that the gray values of X-CT images vary greatly
with scanning conditions, environments and sample statuses. Even for
the same sample, two X-ray scans can hardly generate the same VDV
spectra [56]. Therefore, specific imaging analysis is required to unravel
the microscopic changes between the HCP samples before and after
MIP.
Y. Qi et al.
Fig. 4. Gray value changes of the 1-10-35 sample (a, b and c) before and (d, e, and e) after MIP test: the selected horizontal sectional X-CT images (a and d), local ROIs with
the pixels of 327 × 374 (b and e) and the surface plots of gray values (c and f).
3.3. Mercury distributions
Figs. 5 and 6 show the vertical sectional images of the HCP cylinders
before and after MIP tests with different testing conditions. For each
sample, only the bottom end is open for mercury intrusion. The average
gray values at different heights are used to demonstrate the gray value
heterogeneity along the mercury intrusion direction (bottom to up).
For the HCP cylinders before MIP, all images show the similar gray
levels, suggesting the relatively isotropic and homogeneous material
microstructure (Figs. 5a–c and 6a–c). This conclusion is also supported
by the smooth and linear gray value distributions along the sample
height for all the non-intruded HCP samples. For the 1-5-035 sample
before MIP, some big island-like aggregates can be observed (Fig. 5a),
which may be caused by the agglomerations of cement clinkers. The
dark edges around the agglomerations may be due to the formation of
a water-rich layer, which will generate a porous structure that is more
feasible for mercury intrusion. This hypothesis can be proved by the
X-CT images of the same sample after MIP. As illustrated in Fig. 5d,
some polygons with the bright edges clearly evidence the structure of
porous edges around the agglomerations.
After the HCP samples experience a complete MIP test, the vertical
X-CT images show different characteristics. A plausible one can be the
significant enhancement in the contrast of X-CT images for the mercury
intruded samples (Figs. 5d–f and 6d–f). The phase in bright color,
representing the mercury drops entrapped in the HCP bodies, is rather
obvious (see also the gray value analysis displayed in Fig. 4). Further-
more, due to the significant X-ray attenuating effect of mercury, the
areas of the mercury drops seem to be larger than those of the empty
pores of the same sample before MIP. The image contrast enhancement
by mercury intrusion enables the characterization of microstructure
below the resolution of the X-CT device. Similar conclusion is evidenced
by an X-CT investigation on low-porosity rocks [56].
The mercury distributions along the sample height can be char-
acterized by the gray value distributions. Unlike the HCP samples
before MIP tests that show smooth and linear gray value distributions,
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Cement and Concrete Composites 122 (2021) 104111
the same samples after MIP tests have rather rough and nonlinear
gray value distributions due to the existence of the heterogeneously
entrapped mercury drops (Figs. 5d–f and 6d–f). An extreme case can
be the results of the 1-5-035 sample (Figs. 5d), which shows great
gray value gradients along the sample height. It reflects the mercury
distribution gradients along the sample height: higher position contains
less mercury.
The position dependent vertical gray value distributions are still
valid for the other samples, which are the consequences of mercury
intrusion and extrusion. As an example, we comparatively plot the
vertical gray value distributions of the 1-30-035 and 3-30-035 samples,
and demonstrate the mechanisms in Fig. 7. For the 1-30-035 sample
(the maximum applied pressure=10,000 psi), the gray value gradients
occur at both the top and bottom ends, owing to the insufficient
mercury intrusion and the withdrawing of mercury, respectively, (left
half of Fig. 7). For the 3-30-035 sample (the maximum applied pres-
sure=30000 psi), the entire sample has been completely intruded, so
no obvious gray value gradient can be observed at the top end. But the
mercury release always occurs, so the significant gray value gradient
still appear (right half of Fig. 7).
3.4. Mercury clusters
Segmentation and reconstruction on the X-CT data are performed
to explore the mercury clusters entrapped in the HCP cylinders with
different MIP testing conditions. Fig. 8 shows the results of the 1-5-035
sample after the MIP test with the maximum pressure of 10,000 Psi and
the equilibrium time of 5 s. The phase contrast image shows a rough
gradient distribution of mercury in the sample body owing to the partial
pore percolation (Fig. 8a). A large number of mercury drops are isolated
in thin pores, while some entrapped mercury drops form large mercury
clusters (Fig. 8b). The mercury clusters larger than > 0.01 mm3 are
specifically demonstrated in Fig. 8c. The connection of mercury drops
entrapped in the pores generates irregular mercury clusters (Fig. 8d).
The phase segmentation results of the 1-10-035 sample are used to
explore the effect of equilibrium time (Fig. 9). With the equilibrium
Y. Qi et al.
Fig. 5. Selected vertical sectional X-CT images and average gray value distributions along the sample height for the samples before (a–c) and after (d–f) MIP tests with different
conditions: (a, d) 1-5-035, (b, e) 1-10-035 and (c, f) 1-30-035. The 𝑋-axis range of gray value distribution is uniformly set as 8000.
time of 10 s, a default parameter in MIP tests [1], mercury can almost
thoroughly penetrate the sample with the length of 10 mm (Fig. 9a and
b). This tells that a longer equilibrium time allows a greater penetration
of mercury though thin pore throats. The results also evidence that
mercury intrusion is a dynamic process [23,24]. Some large irregu-
lar mercury clusters are located at different positions of the sample
(Fig. 9c), suggesting the hierarchical pore structure of HCP.
When the maximum intrusion pressure is raised up to 30,000
Psi, more mercury entrapment can be observed (Fig. 10a and b).
Those entrapped mercury drops form more and larger mercury clusters
(Fig. 10c). Those clusters cannot be probed in the un-intruded samples.
In cement matrix, pores are generally isolated and/or connected by
very thin channels. Under high pressures, mercury can enter into the
pores and penetrate through the thin channels. Those thin channels
may deform or expand after mercury intrusion. Then the pores, to-
gether with the channels, form large clusters (Fig. 11). The percolated
mercury clusters (Figs. 8d–10d), to the best of the authors, have never
been demonstrated in the previous literature. Furthermore, the mercury
clusters show significant spatial heterogeneity. This is in accordance
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Cement and Concrete Composites 122 (2021) 104111
with the knowledge of CBMs, a type of highly heterogeneous compos-
ites with complex pore structure [61]. Similar results are reported by
Qian et al. [41,42].
3.5. Interactions between mercury drops and pore wall
Even with high entrapment, mercury drops may not always have
direct contact with pore walls. Fig. 12 shows the 3D microstructure
of local HCP segments that consist of the solid skeleton, empty pores
and the entrapped mercury drops. The top and bottom parts of each
sample (at the heights of 1 and 9 mm, respectively) are selected, and
all figures are displayed in the same scale (Fig. 12a). As expected, the
mercury drop distribution is dependent of the sample position . For
example, the top part of the 1-5-035 sample almost contains no mercury
drops, whereas the bottom part has large continual and connected
mercury clusters (Fig. 12a). In the cases of the MIP tests with the higher
maximum pressures and the longer equilibrium time, the mercury drops
and empty pores share the pore chambers at both the top and bottom
parts of each sample (Fig. 12). The results are in line with our previous
X-CT measurements on HCP samples without surface coats [34].
Y. Qi et al.
Fig. 6. Selected vertical sectional X-CT images and average gray value distributions along the sample height for the samples before (a–c) and after (d–f) MIP tests under different
conditions: (a, d) 3-5-035, (b, e) 3-10-035 and (c, f) 3-30-035. The 𝑋-axis range of gray value distribution is uniformly set as 8000.
The mercury fraction in the bottom part of an HCP sample is not
always higher than the top part due to the release of the mercury drops
outward the sample (see, for instance, the 3D microstructure images
of the 1-30-035 displayed in Fig. 12b and the analysis in Fig. 7). The
coexistence of mercury drops and empty pores are the consequences
of the thermodynamic equilibrium among tiny mercury drops, pore
walls and the air [24]. One shall understand that the detected pores
(empty pores plus mercury drops) may be overestimated because of the
microstructure damages of HCP under high mercury pressures [18,21].
3.6. Mercury intrusion spectra
Figs. 13 and 14 show the accumulative and differential PSD spectra
of the coated HCP samples determined by the MIP tests with the
different equilibrium time and maximum applied pressures. Generally,
the accumulative PSD spectra of porous CBMs follow a three-stage
intrusion character [7]: (a) a slow rise stage at the initial intrusion
period under low applied pressures; (b) a plateau stage at the middle
intrusion period under moderately high applied pressures; and (c) a
rapid rise stage at the late intrusion period under high applied pres-
sures. For some CBM samples with interfacial zones and fine blends,
8
Cement and Concrete Composites 122 (2021) 104111
more characteristic stages may be figured out [18]. In our tests, the
MIP pore data characteristics are summarized as follows:
• At the first mercury intrusion stage, obvious mercury volume
rises are recorded for the samples of 1-5-035, 1-30-035, 3-5-035
and 3-10-035. These heavy and rapid rises of mercury volume
at the light pressure (1.8 psi) lead to the differential PSD peaks
at 100 μm (Figs. 13 and 14). The results are contrast to the
normally observed first mercury rise stage that shows relatively
low intrusion volume and slow rate [7]. However, this does not
mean that the surface coating has changed the pore structure of
the HCP sample, because the PSD spectra of the first mercury
intrusion stage do not reflect the real pores filled by mercury.
Indeed, a highly likely explanation of the observation can be that
some voids in the epoxy coatings of the HCP samples have been
partially penetrated and filled with the mercury at this intrusion
stage (see the shadowed areas in Figs. 13 and 14). This regime
also accounts for the tiny mercury drops detected by X-CT (Fig. 2).
• At the plateau stage, the accumulative PSD spectra of all samples
stay stably in the pressure range between 3.6 and 90 psi (or the
pore range between 50 and 2 μm) (Figs. 13 and 14). The material
Y. Qi et al. Cement and Concrete Composites 122 (2021) 104111

Fig. 7. Comparative plots of gray value distributions of 1-30-035 (left) and 3-30-035 (right).

Fig. 8. Analysis of mercury clusters in the 1-5-035 sample: (a) phase contrast image of the samples after MIP, (b) all the mercury clusters (aligned in different colors), (c) large
mercury clusters (volume > 0.01 mm3 ), and (d) 3D structure of a local mercury cluster.

9
Y. Qi et al. Cement and Concrete Composites 122 (2021) 104111

Fig. 9. Analysis of mercury clusters in the 1-10-035 sample: (a) phase contrast image of the samples after MIP, (b) all the mercury clusters (aligned in different colors), (c) large
mercury clusters (volume > 0.01 mm3 ), and (d) 3D structure of a local mercury cluster).

Fig. 10. Analysis of mercury clusters in the 3-10-035 sample: (a) phase contrast image of the samples after MIP, (b) all mercury clusters (aligned in different colors), (c) large
mercury clusters (volume > 0.05 mm3 ), and (d) 3D structure of a local mercury cluster.

has relatively dense compactness, so almost no mercury intrusion
takes place in the pressure range. As a matter of fact, except
for some highly porous materials, like aerogel-modified cement
composites [62], this plateau stage is commonly observed.
• As the applied pressure increases further, mercury rapidly pen-
etrates into the thin pores of the material matrix comprising of
unhydrous cement clinkers and hydration products (and/or the
epoxy coatings). For example, the PSD peaks around 1000 nm
for the 1-10-35, 1-30-35 and 3-30-35 samples (Figs. 13 and 14),
which have not been observed for well cured ordinary HCPs, can
be attributed to the extra mercury intrusion into the epoxy coat-
ings. The PSD spectra at the pores below 100 nm represent the
penetration of mercury through thin capillaries between cement
grains and/or large gel pores between C-S-H layers [43]. The ex-
pected rapid mercury rises do not take place in the accumulative
PSD of the 1-5-035 sample. This is caused by the uncompleted
mercury intrusion under the low maximum pressure and short
equilibrium time (Fig. 8).
The extrusion spectra of all samples show the similar characteristics.
As the applied pressure fades, the probed mercury volume does not

10
Y. Qi et al. Cement and Concrete Composites 122 (2021) 104111

Fig. 11. Mechanism of forming mercury clusters in the HCP samples after MIP.

Fig. 12. 3D microstructure of local VOI areas in the samples: (a) selected 3D images at the top (height=9 mm) and bottom positions (height=1 mm), and (b) representative
illustration of the entrapped mercury drops (yellow), empty pores (transparent gray) and cement paste skeleton (brown) in the 1-30-035 sample. (For interpretation of the references
to color in this figure legend, the reader is referred to the web version of this article.)

decrease immediately, but increases slightly followed by a very slow mercury volume of the 1-5-035 sample is 0.059 ml/g, higher than
decrease (Figs. 13 and 14). After the unloading process completes, the that at the pressure of 10,000 psi (0.053 ml/g) by 10% (Fig. 15).
recorded residual mercury volumes are close to or even higher than These are heavily different from the MIP extrusion spectra of open
the total intrusion ones (Fig. 15). For instance, the recorded residual CBMs that show obvious volume decays when the applied pressure

11
Y. Qi et al. Cement and Concrete Composites 122 (2021) 104111

Fig. 13. Accumulative (a) and differential (b) PSD spectra of the HCP samples under the maximum applied pressure of 10,000 psi with the equilibrium time of 5, 10 and 30 s.
The shadowed areas represent the possible mercury intrusion in the surface cavities and/or epoxy layers.

Fig. 14. Accumulative (a) and differential (b) PSD spectra of the HCP samples under the maximum applied pressure of 30,000 psi with the equilibrium time of 5, 10 and 30 s.
The shadowed areas represent the possible mercury intrusion in the surface cavities and/or epoxy layers.

withdraws [61]. The abnormal mercury decaying behaviors are the
consequences of mercury entrapment and redistribution in the neigh-
boring empty pores due to the partial surface coatings on the samples.
The results of Fig. 15 imply that the partial surface coating may
enhance the ’ink-bottle’ effect.
Some characteristic quantities (i.e., the intrusion volume of surface
and coat (S&C), body intrusion, total intrusion and residual volume)
are acquired and displayed in Fig. 15. It seems that the S&C to total
intrusion volume ratios are between 50% and 70%, suggesting that a
large amount of mercury is captured in the epoxy coats due to their

12
Y. Qi et al.
Fig. 15. The characteristic intrusion results for all samples with the equilibrium time of 5, 10 and 30 s under different maximum pressure: (a) 10,000 psi, and (b) 30,000 psi
(S&C: surface and coating).
soft and porous texture. As a consequence, the intrusion volumes into
the HCP bodies are less (Fig. 15). As the maximum applied pressure
increases, more pores at thinner sizes can be filled with mercury, so
all the intrusion quantities increase (Fig. 15). Moreover, pores may
deform and microstructure may damage under the intrusion of mercury
in high pressures, which will cause the unexpected intrusion volume
increases [18].
The characteristic MIP quantities also change with equilibrium time,
but they do not show appealing correlations (Fig. 15). One may note
that the body intrusion of the sample at the equilibrium time of 5 s
(1-5-035) is greatly lower than that of the samples with the longer equi-
librium time (1-10-035 and 1-30-035). This tells that the equilibrium
time of 5 s does not allow the completion of mercury intrusion, in line
with the X-CT results (Figs. 2 abd 8).
3.7. Further discussion
In this work, we specifically design a double coating scheme to
control the mercury intrusion directions, and conduct X-ray scans to
the materials after MIP tests under different conditions. While we may
first visually probe the percolation of mercury in a porous HCP and
resolve the 3D microstructure of mercury clusters (Figs. 8–10), some
issues deserve rigorous discussion.
• First, mercury, under high pressures, can penetrate into the first
epoxy layer, forming the mercury drops probed by X-CT. This
unexpected mercury intrusion brings the additional mercury rises
at low applied pressures (Figs. 13 and 14). Furthermore, the
penetration of mercury through the first epoxy coating may also
break the pattern of one-direction percolation, so homogeneous
mercury clusters are observed for most samples. New coating
methods or materials are wanted in the future work to guarantee
the one-direction mercury intrusion in CBMs.
• Second, the surface coating can greatly change the extrusion
spectra. For instance, one can hardly observe the decreases in
mercury volume during mercury extrusion (Figs. 13 and 14),
which is greatly different from the ordinary MIP extrusions. This
difference may come from the enhanced mercury entrapment in
the HCP body (Figs. 5 and 6). Mercury drops may be entrapped
13
Cement and Concrete Composites 122 (2021) 104111
in big air voids and the nearby capillary pores. Indeed, because
of the high mercury entrapment, we can observe the ganglia-
like structures that reflect the high connectivity of the pores.
This is different from our previous work [34], in which only the
mercury drops entrapped in big voids were addressed to resolve
the ’ink-bottle’ pore structure. It is also a challenge to establish
the quantitative relationships between the mercury entrapment
and pore connectivity, while previous attempts have been made
in the relevant issues [61].
• Third, mercury is a liquid metal with high surface energy, so it
can hardly stay in thin capillary pore throats. This means that the
entrapment and releasing of mercury drops in micro porous ma-
terials are always beyond the thermodynamic equilibrium [24].
Low-melting point metals (such as Bi-based alloys [58]) may be
used as the intrusion medium to have stably intrusions in CBMs.
Furthermore, the technique of focused ion beam/scanning elec-
tron microscopy [63,64] may be applied to quantify the changes
of percolation paths in HCPs after low-melting point metal intru-
sion.
4. Conclusion
A double coating scheme is specifically designed to prepare the
partially sealed HCP samples before MIP and to prevent the leakage
of mercury after MIP. The first coat enables the one-direction intrusion
of mercury into the HCP segments, and the second coat guarantees the
technicians’ safety when handling with the mercury intruded samples.
The X-CT images directly and visually demonstrate the percolation
paths of mercury in the HCP samples. This is probably the first visual
evidence of mercury percolation in porous CBMs.
Mercury entrapment can change the gray value distributions of
the HCP samples. The dual-peak VGV spectra reduce to the single-
peak ones, and the total gray values are greatly increased for the
HCP samples after MIP tests. The vertical gray value spectra become
rougher, and show obvious gradients near the bottom ends due to
the release of the entrapped mercury. Gray value distributions change
along the sample height, reflecting the mercury distribution. Mercury
drops are heterogeneously entrapped in the pore system of the HCP.
Y. Qi et al.
The penetration of mercury into the epoxy coats at low pressures
leads to the early PSD peaks before mercury percolates through the HCP
bodies. The recorded mercury extrusion spectra do not fade obviously
as the applied pressures decrease because the surface coatings restrict
the retraction of the intruded mercury. The ’ink-bottle’ effect can be
enhanced by the first surface coating.
Overall, the combination of MIP with the continually advanced
testing techniques (e.g., X-CT in this work) helps better understand the
physical process of MIP. The high X-ray attenuation of mercury makes
it a preferable tracing agent to enhance the contrast of X-CT images of
a porous material after mercury intrusion, enabling the pore structure
characterization of densely compacted porous materials. The coating
scheme used in this work facilitate the reconstruction of the perco-
lated mercury clusters by X-CT. The methodological improvements may
allow us to approach the true pore structure of CBMs as closely as
possible.
Declaration of competing interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Acknowledgments
The authors acknowledge the Civil Engineering Experiment Cen-
ter of Zhejiang University, PR China for the experiment supports.
QZ acknowledges the National Natural Science Foundation of China
(No. 51878602). YP acknowledges the Experimental Technology Re-
search Project of Zhejiang University (No. SJS 202007), and Zhe-
jiang Public Welfare Technology Application Research Project (No.
LGC19E020001)).
Appendix A. Supplementary data
Supplementary material related to this article can be found online
at https://doi.org/10.1016/j.cemconcomp.2021.104111.
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