Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908

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Journal of Rock Mechanics and

Geotechnical Engineering
journal homepage: www.rockgeotech.org

Review

Application of nuclear magnetic resonance technology to carbon capture,

utilization and storage: A review
Liang Xu a, b, Qi Li a, b, *, Matthew Myers c, Quan Chen a, Xiaochun Li a
a
State Key Laboratory of Geomechanics and Geotechnical Engineering, Institute of Rock and Soil Mechanics, Chinese Academy of Sciences, Wuhan, 430071, China
b
University of Chinese Academy of Sciences, Beijing, 100049, China
c
CSIRO Energy, Australian Resources Research Center, 26 Dick Perry Avenue, Kensington, Western Australia, 6151, Australia

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

Article history: Carbon capture, utilization and storage (CCUS) is considered as a very important technology for miti-
Received 9 October 2018 gating global climate change. Carbon dioxide (CO2) injected into an underground reservoir will induce
Received in revised form changes in its physical properties and the migration of CO2 will be affected by many factors. Accurately
29 December 2018
understanding these changes and migration characteristics of CO2 is crucial for selecting a CCUS project
Accepted 9 January 2019
Available online 30 May 2019
site, estimating storage capacity and ensuring storage security. In this paper, the basic principles of
nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) technologies are briefly
introduced in the context of laboratory experiments related to CCUS. The types of NMR apparatus,
Keywords:
Geologic carbon storage
experimental samples and testing approaches applied worldwide are discussed and analyzed. Then two
Nuclear magnetic resonance (NMR) typical NMR core analysis systems used in CCUS field and a self-developed high-pressure, low-field NMR
Core flooding rock core flooding experimental system are compared. Finally, a summary of the current deficiencies
Experimental apparatus related to NMR applied to CCUS field is given and future research plans are proposed.
Low-field NMR Ó 2019 Institute of Rock and Soil Mechanics, Chinese Academy of Sciences. Production and hosting by
High-field NMR Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/
licenses/by-nc-nd/4.0/).

1. Introduction
Rapid development of human society and continued dominance
of fossil energy have led to increasing carbon dioxide (CO2) emis-
sions. The total amount of CO2 emissions from human activities was
estimated at 41 billion tonnes in 2017, and the impact of these
continued emissions on global climate change is significant.
Addressing climate change and searching for cleaner and less car-
bon intensive sources of energy compared to coal-like methane
have drawn the attention of researchers, industries, governments
and the general population (Ranathunga et al., 2016). Carbon cap-
ture, utilization and storage (CCUS) technology, which seeks to
achieve massive emission reductions for fossil energy, refers to as
the separation of CO2 from industrial or energy production-related
gas sources followed by compression, transport and storage in
appropriate subsurface reservoirs. The main sites for CO2 storage
include oil and gas reservoirs (Alfarge et al., 2018), coal fields (Wang
* Corresponding author.
E-mail address: qli@whrsm.ac.cn (Q. Li).
Peer review under responsibility of Institute of Rock and Soil Mechanics, Chi-
nese Academy of Sciences.
et al., 2016) and deep saline aquifers (Li et al., 2016a; Ringrose,
2018). CCUS is not merely a cost-intensive exercise with no re-
turn, but it can bring considerable economic benefits and mitigate
the energy crisis. For example, Vishal et al. (2018) showed that
there is a significant increment in methane production from coal-
beds due to injection of CO2. To reliably and securely inject CO2 in
large quantities for storage, suitable reservoirs should have high
porosity and interconnected pores (Doughty et al., 2008). Further-
more, the caprock must have low porosity to prevent vertical
leakage of CO2, helping to keep the CO2 in the reservoir for a long
period of time (Bentham and Kirby, 2005). Permeability, like
porosity, is also one of the important physical parameters deter-
mining whether the CO2 can be stored steadily and enduringly.
Suitable reservoirs for CO2 storage cover a permeability range
typically larger than 10 mD. However, compared to many areas in
the world (e.g. Sleipner and Weyburn with multi-Darcy perme-
abilities), the permeabilities of most oil and gas reservoirs in China
suitable for CO2 storage tend to be quite lower (i.e. less than 10 mD).
In this sense, CO2 leakage is easier in high-permeability reservoirs
than those with low permeability. Injecting CO2 will increase the
pore pressure of the formation, thus impact the original stress
equilibrium state of the formation, and subsequently change the
physical properties of the rock and influence the characteristics of

https://doi.org/10.1016/j.jrmge.2019.01.003
1674-7755 Ó 2019 Institute of Rock and Soil Mechanics, Chinese Academy of Sciences. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-
NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
storage (Li et al., 2016b). Meanwhile, when CO2 is injected into the
target reservoirs to displace brine or oil in natural rocks, due to the
presence of fractures developed in the long geologic periods,
fingering phenomenon that can cause early breakthrough often
prevails (Ebrahimi et al., 2015). Capillary forces will drive the
injected CO2 to preferentially fill pores within a certain size range,
as a result, the displacement efficiency of CO2 is far lower than
100%, as CO2 can react with rock minerals or dissolve in water
within the formation. It may re-activate the existing fracture sys-
tem or create new fractures in the formation potentially, leading to
seal failure (Schembre-McCabe et al., 2007).
As such, it is of great significance to assess the porosity, pore
structure, permeability and other parameters of the reservoir
quickly and accurately before and after CO2 injection. Analyzing
reservoir physical property changes and monitoring fluid migration
characteristics are crucial with respect to the security and stability
of CO2 target reservoir and caprock. Nuclear magnetic resonance
(NMR) technology, which is likely to address all of concerns, has
now attracted wide attention.
Purcell et al. (1946) at Harvard University and Bloch et al. (1946)
at Stanford University independently observed the phenomenon of
NMR absorption in different ways. Seevers (1966) observed that the
relaxation time of NMR signals is correlated with the permeability
of rock samples. Timur (1968, 1969) pioneered the concept of free
fluid index and suggested a method to measure the porosity,
permeability and free fluid index of sandstone by NMR simulta-
neously. Brownstein and Tarr (1979) proposed the theory of NMR
relaxation in porous media. In the same year, Gummerson et al.
(1979) applied magnetic resonance imaging (MRI) technology to
porous media for the first time. Rothwell and Vinegar (1985) used a
0.84 T superconducting MRI apparatus at Bruker to analyze the
pore structure of aquifer Berea sandstone. This marks the first
application of MRI technology to rock core analysis. Baldwin and
Yamanashi (1989) used an improved 0.5 T medical MRI apparatus
to monitor the water flooding process in Berea cores. In the early
1980s, Wuhan Institute of Physics and Mathematics of Chinese
Academy of Sciences (CAS) carried out rock structure analysis using
NMR microscopic imaging technology (Xiao, 1995). Jianghan Pe-
troleum University (China) analyzed the applicability of NMR log-
ging technology in China (Xiao, 1995). In 1991, Institute of Porous
Flow and Fluid Mechanics of CAS purchased the world-class
superconducting MRI system in China for the first time, and
designed a low-field NMR rock core analysis system independently
in 1996. Since then, other researchers have carried out studies on
the secondary migration of oil and gas by NMR; especially, it comes
to the burgeoning field of CCUS recently.
In this paper, the types of NMR apparatus, experimental sam-
ples and test procedures applied to CCUS are summarized and
critically reviewed. Meanwhile, some advantages and drawbacks
of the NMR rock core analysis systems designed by Tsinghua
University and Dalian University of Technology, China, as well as
Institute of Rock and Soil Mechanics (IRSM) of CAS, for CCUS
application, are considered. This paper also illustrates the appli-
cation of NMR technology to CCUS field, and proposes future
research works, if likely.
2. Principles of NMR
Generally, protons and neutrons form a nucleus, and nuclei with
either an odd number of protons and/or neutrons have a magnetic
moment and are considered as NMR active. The nucleus whose spin
vector is in the same direction of the magnetic field is at low-energy
level, and the nucleus whose spin vector is in the opposite direction
of the magnetic field is at high-energy level. Matter is made up of a
large number of atoms and the nuclei of these atoms present a
893
longitudinal magnetization vector Mz (Mz ¼ M0, where M0 is the
initial longitudinal magnetization vector). If a pulsed electromag-
netic wave with the Larmour frequency u ¼ gB (g is the magne-
togyric ratio of the nucleus and B is the magnetic field intensity) is
only related to the type of nucleus and its propagation direction is
perpendicular to the direction of the magnetic field, the nuclei at
the low-energy level will absorb electromagnetic energy and
transit to the high-energy level. The magnetization vector Mz is
reduced or even reversed at the macroscopic level. At the same
time, these transition nuclei will have the same spin phase and a
transverse magnetization vector Mxy appears, which is perpendic-
ular to the direction of the magnetic field. This phenomenon is
called NMR (Xiao, 1998; Coates et al., 1999). After the electromag-
netic wave induced resonance disappears, the nuclei will release
the absorbed energy and return to the low-energy level. The phase
will be reclassified into the disordered state, which is reflected in
the macroscopic level as the longitudinal magnetization vector
gradually recovers to M0 and the transversal magnetization vector
gradually recovers to 0. This process is called “relaxation”. The
process that the nuclei release energy and return back to the low-
energy level is called “spin-lattice” relaxation, and the process
that the nuclei return back to the disordered state is called “spin-
spin" relaxation (Kabal and Chizhik, 1982). The schematic diagram
illustrating the principle of NMR and relaxation is shown in Fig. 1.
After applying a 90 pulsed electromagnetic wave and then
cancelling it, the time required for the longitudinal magnetization
vector to recover from 0% to 63% of M0 is called T1 (see Fig. 2a), and
the time required for the transverse magnetization vector to decay
to 37% of its original state is called T2 (see Fig. 2b). On the macro-
scopic level, it is found that T2  T1 (Bernstein et al., 2004) and that
fluids in rock pores have three different relaxation mechanisms:
free relaxation, surface relaxation and diffusion relaxation of
gradient magnetic fields. For most liquids in natural rocks, the
system is in a fast diffusion zone. Compared with the surface
relaxation, the effect of free relaxation on the total relaxation can be
neglected. Meanwhile, the water molecules colliding with the pore
wall diffuse very quickly, as such diffusion relaxation can also be
neglected. Thus the relaxation processes are dominated by the
surface relaxation.
1 1 1
¼ þ (1)
T1 T1b T1s
1 1 1 1 1 s
¼ þ þ z ¼ r2 (2)
T2 T2b T2s T2d T2s v
where Tlb is the longitudinal volume relaxation time, which refers
to as the relaxation time of the fluid in free state; Tls is the longi-
tudinal surface relaxation time; T2b is the transverse relaxation
time; T2s is the transverse surface relaxation time; T2d is the
transverse diffusion relaxation time; r2 is the transverse surface
relaxation intensity (or transverse surface relaxation rate), mainly
related to pore geometry and rock type (Kenyon, 1997); s is the pore
surface area; and v is the pore volume (for typical spherical, tubular
and plate pore models, v/s ¼ d/6, d/4, and d/2, respectively, where
d is the pore diameter). These three models are only idealized as-
sumptions. Due to the complex pore structure inside the rock, the
pore inside the rock cannot be simply described with a singular
model. In the actual experiment, the pore size distribution (PSD)
curve of this kind of rock sample is usually measured by other
methods, and the three models (typical spherical, tubular and plate
pore models) are used for comparison. Then, through iterative al-
gorithm, we could obtain which model is suitable for this kind of
rock sample.
894 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
Fig. 1. Schematic diagram of NMR and relaxation process.
Fig. 2. The diagram of relaxation time: (a) Longitudinal relaxation time T1; and (b)
Transverse relaxation time T2.
A gradient magnetic field distributed in three-dimensional (3D)
space added to the original static magnetic field results in a spatial
organization of the nuclei with different resonance frequencies,
spin frequencies and phases. Then, through different de-
convolution methods, the intensity distribution map of different
location signals can be drawn to obtain NMR images. This way of
obtaining the internal structure of a porous medium is called nu-
clear MRI. Foe this, the spatial encoding technique is used and it can
be roughly divided into two methods: Fourier transform and pro-
jection reconstruction. The Fourier transform method realizes
spatial orientation through a combination of a linear gradient field
and a shaped pulse. The projection reconstruction method mea-
sures the projection of the spin density in each direction by
changing the direction of linear gradient field providing an image of
interior sample. Comparing the two methods, the Fourier trans-
form method is simple and flexible with a short data acquisition
and processing time, but it cannot clearly image the samples with
respect to short relaxation times. The projection reconstruction
method can be used to image samples clearly with relatively short
relaxation time or for multi-echo processing of samples with a long
relaxation time. However, this method has its limit due to a long
collection and processing time and requires a large amount of
computer memory. Therefore, appropriate imaging methods
should be carefully selected according to the required imaging ac-
curacy. For materials with higher porosity and permeability and
longer relaxation times, the Fourier transform method can be used
for rapid imaging. Given the low porosity and permeability char-
acteristics of the CCUS reservoirs in China, the projection recon-
struction method is preferred despite the longer acquisition times
for clearer imaging (Clarke et al., 1995; Zhao et al., 2013).
3. NMR core experimental system
There are two kinds of NMR rock core experimental systems
used for CCUS in laboratory. One is to use NMR apparatus as an
independent system to measure the change of fluid inside the core
before and after other experiments (e.g. centrifugal experiments).
The other is an in situ measurement system to monitor changes of
rock‘s physical properties in real time during the course of an
experiment (e.g. core flooding). The advantage of the second one is
that it can continually monitor the change in physical parameters
and migration of pore fluid during the process of CO2 injection,
which is also the main method in the world.
3.1. NMR apparatus
According to the type of magnet and the intensity of magnetic
field, NMR apparatuses can be divided into two types: low- and
high-field. The low-field system uses permanent magnets instead
of superconducting coils to build magnetic fields, and its magnetic
field intensity is generally not greater than 0.5 T. Table 1 summa-
rizes the NMR systems generally used in the CCUS field and pub-
lications regarding experiment types and sample types/sources.
According to Table 1, it can be seen that NMR systems applied to
CCUS core analysis have the following characteristics:
(1) The main suppliers of the NMR systems for CCUS applica-
tions are the Oxford Instruments in UK, the Bruker Corpo-
ration in USA, the Varian Corporation in USA and the Suzhou
Niumag Analytical Instrument Technology Corporation in
China. A few systems have been developed by universities or
research institutes for specific scientific research needs.
Among them, the Oxford Instruments and Suzhou Niumag
Analytical Instrument Technology Corporation focus on low-
field NMR while the Bruker and Varian Corporations in USA
Table 1
NMR apparatus and test contents.

Instrument type Supplier Type of field Owner/user Sample Source of samples Experimental Reference
intensity parameter

CPS-NMR e Low-field, China University of Low permeability Changqing oilfield, T2 Guo and Gu (2005)
3.75 MHz Petroleum, Beijing sandstone China
RecCore-2500 Self-made Low-field Institute of Porous Flow Low permeability Xujiahe Group in Optimum centrifugal Zhang et al. (2015a, b)
2.05 MHz and Fluid Mechanics of sandstone Central Sichuan force, T2
CAS Basin
MacroMR-12 Suzhou Niumag Low-field China University of Tight sand e T1, T2, MRI Ge et al. (2017a, b)
Analytical 0.3 T Petroleum, Qingdao
Instrument 12.8 MHz
Technology
Corporation, China
MacroMR-12-150HeI Suzhou Niumag Low-field Southwest Petroleum Shale Longmaxi T2 Chen et al. (2016)

L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908

Analytical 2.05 MHz University, China Formation in
Instrument Sichuan Basin
Technology University of Mining Tight coal Henan province, T2 Xue et al. (2018)
Corporation, China and Technology, China China,
Maran-2L3 Oxford Low-field Shengli Oilfield Shaly sandstone Jidong oilfield, T2 Yun et al. (2002)
Instruments, Company China
UK
Maran-2M Oxford Low-field Research Institute of Natural core Daqing oilfield, T2 Liu (2012)
Instruments, Exploration and China
UK Development of Daqing
Oilfield Company Ltd.,
China
Maran-2S2 Oxford Low-field China University of Sandstone Shengli oilfield, Primary echo Wang et al. (2006)
Instruments, Petroleum, Beijing, China sequence, T1, T2
UK China
MesoMR23-060HeI Suzhou Niumag Low-field, Tsinghua University, Chaunoy sandstone Paris basin, France T2 Manceau et al. (2015)
Analytical 0.5 T China
Instrument 21.3 MHz,
Technology
Corporation, China
MiniMR-60 Suzhou Niumag Low-field, 0.5 T Tsinghua University, sandstone e T2, MRI Ma et al. (2013)
Analytical China
Instrument Xi’an Petroleum Sandstone Zhongyuan oilfield T2 Gao et al. (2015)
Technology University, China
Corporation, China Xi’an Petroleum Low permeability Northeast T2 Wang et al. (2017)
University, China artificial core Petroleum
University, China
Biospec47/40 Bruker Corporation, High-field, Institute of Porous Flow Granite A shear zone (VE T2, Chen and Kinzelbach (2002)
USA 4.7 T, and Fluid Mechanics of tunnel, location
200 MHz CAS 422.3 m) at the
Grimsel test site,
Switzerland
Sand-packed cores e MRI Wang et al. (1996)
Bruker AVANCE 300 Bruker Corporation, 300 MHz University of Berea sandstone e T2, Cody et al. (2016)
USA Birmingham, UK
Bruker Biospin Bruker Corporation, High-field, University of Borosilicate glass e T2, MRI Hussain et al. (2011)
AV85 USA 2T Cambridge, UK beads
(continued on next page)

895
 896
Table 1 (continued )

Instrument type Supplier Type of field Owner/user Sample Source of samples Experimental Reference
intensity parameter

Bruker MSL-400 Bruker Corporation, High-field, Wuhan Institute of Limestone, e MRI Xiao et al. (1994)
USA 100.63 MHz Physics and dolomite,
Mathematics of CAS sandstone
Maran Oxford High-field, University of New Unconsolidated, Ottawa sand, MRI Romero-Zerón et al. (2010)
Instruments, 7T Brunswick, Canada high permeability Canada
UK model sand packs
NMR MOUSE e High-field, University of Sandstone North Sea oil MRI Bencsik and Ramanathan (2001)
2.35T Nottingham reservoir
Unity Inova 85/310 Varian Corporation, High-field, University of Bergen, Bentheim e MRI Ersland et al. (2010)
USA 2T Norway sandstone

L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908

Edwards limestone Garden City, Texas, MRI, MRI signal intensity Fernø et al. (2011)
USA
Unity Inova Varian Corporation, High-field, Tokyo Institute of Glass tube e MRI Hirai et al. (2000)
300/150 SWB USA 7.05 T Technology, Japan
Varian NMR 400 Varian Corporation, High-field, Dalian University of Glass sand Japan MRI Liu et al. (2011)
USA 9.4 T, Technology, China Quartz glass bead MRI, MRI signal intensity Teng et al. (2017)
400 MHz Quartz glass bead T2, MRI Jiang et al. (2017)

Table 2
The experiment related to CCUS conducted by Dalian University of Technology, China.

Experimental sample Size (mm) Max. temperature Experimental Fluids Reference

and pressure condition

Glass bead (diameter) (mm) Core (diameter  length) (mm  mm) T (K) P (MPa) T (K) P (MPa)

Packed glass beads 0.11 15  200 e 12 286 4.8 Water, CO2 Yang et al. (2011),
Teng et al. (2016)
Packed glass beads 2, 0.2 15  200 343 15 295e313 6e8 Water, CO2, SC-CO2 Song et al. (2012)
Packed glass beads 2, 0.2 15  200 343 15 298 6 Water, CO2 Jiang et al. (2013a)
Packed glass beads 2, 0.2 15  200 e e 298 6 Water, CO2 Jiang et al. (2013b)
Packed glass beads 0.177e0.25 e e e 311 9 Crude oil from Daqing Song et al. (2014)
Oilfield, polymer, SC-CO2
Synthetic sandstone e 15.3  40.4 343 12 311 7.5e8.3 Decane, CO2, SC-CO2 Liu et al. (2017)
Berea sandstone and e 15  40 421 34 313 6e8 Brine, CO2, SC-CO2 Teng et al. (2018)
synthetic sandstone
 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908 897

Fig. 3. Low-field NMR core flooding experimental system at Tsinghua University, China.

produce and sell high-field NMR. At the same time, some
scholars have modified nuclear magnetic equipment used for
medical research to adjust for CCUS field.
(2) Low- and high-field systems have their specific advantages
and limits. In general, paramagnetic materials in natural
rocks have a negative effect on measurements. Low-field
NMR is not very sensitive to this effect while high-field
NMR is much limited in the presence of paramagnetic ma-
terials. Low-field nuclear is more suitable when the object of
study is a natural rock (with paramagnetic materials).
However, high-field NMR apparatus can have its strengths
when special samples (containing little or no paramagnetic
materials), such as Berea sandstone, glass bead and chalk
rock, are used to study the effects of hysteresis, gravity, vis-
cosity and buoyancy on the flow of CO2.
(3) The test parameters between high- and low-field NMR sys-
tems for CCUS applications are also different. Low-field NMR
is often used to study the changes in porosity, moveable fluid
content and CO2 injection permeability by measuring T2
spectrum in rock samples. High-field NMR is used to analyze
not only the changes in rock properties derived from the T2
spectrum, but also the flow process, hysteresis effect, and

Fig. 4. High-field NMR core flooding experimental system at Dalian University of Technology, China.
898 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
influences of gravity, viscosity and buoyancy by high-
precision MRI images.
(4) The research focus of NMR core analysis in the CCUS field has
been changed. Based on a review of the published literature,
before 2010, NMR core analysis was mainly used to analyze
and interpret the T2 spectrum of the whole sample. After
2010, the research focus shifts to the meso-scale level, mainly
monitoring the distribution and movement of liquids in rock
samples with MRI images.
(5) Economic benefits determine the direction of scientific
research. CCUS is not a purely profit/cost driven exercise as it
can be used to help with climate change through reduction of
CO2 emissions. For example, it is estimated that by 2030, the
industrial output value of China’s CO2-EWR (enhanced water
recovery) ranges from 450 million yuan to 950 million yuan
per year, and that of China’s CO2-EOR (enhanced oil recovery)
ranges from 34.4 billion yuan to 51.6 billion yuan annually.
3.2. Typical NMR systems used in China for CCUS
3.2.1. Low-field NMR core flooding system at Tsinghua University
A schematic of the low-field NMR core flooding experimental
system developed by Tsinghua University, China is shown in Fig. 3.
During the course of a test with this system, a pump is used to inject
supercritical CO2 (SC-CO2) at the desired pressure and flow rate
conditions. At the same time, brine is pressurized through a pump
to the same pressure and rate as those of CO2. After measurement
through their respective flow meters, both the CO2 and brine enter
a thermostatic water bath heating box. Mechanical mixing is then
used to fully equilibrate the two-phase system prior to injection
into the core holder. The core holder has a design pressure and
temperature of 12 MPa and 60  C, respectively, and is placed in a
low-field NMR apparatus for real-time monitoring. The mixed fluid
flows out of the core holder via a back-pressure regulator to
maintain pore pressure within the core holder. The flow rate of each
component in the gaseliquid system is determined using a
specially designed separator (Luo et al., 2011; Ma et al., 2013; Xu
et al., 2017). Due to the minimal impact of paramagnetic mate-
rials on low-field NMR measurements, this system can be used to
analyze the variation in PSD and monitor the migration charac-
teristics of fluids in natural cores during the CO2-EWR process.
However, there are some major disadvantages with this system:
(1) The spatial resolutions of MRI image for this system are
0.44 mm and 0.47 mm in horizontal and vertical directions,
respectively. As such, with a low-resolution system, it is
impossible to analyze the fluid flow rates and hysteresis ef-
fects at the pore-scale.
(2) The design pressure and temperature of the core holder are
considerably low. For example, the perfect temperature
condition for carbon sequestration in a depleted oil and gas
reservoir is 80  Ce90  C. This system fails to analyze the
displacement behavior of CO2 in some environments of
certain natural storage sites.
(3) This core holder cannot be used to simultaneously measure
rock mechanical properties such as stress and strain and to
study multi-field coupling effects such as stress, temperature
and chemical fields.
3.2.2. High-field NMR core flooding experimental system at Dalian
University of technology
A schematic of high-field NMR core flooding system at Dalian
University of Technology, China is shown in Fig. 4. The system
consists of three parts: a pressure control module, a temperature
control module, and a MRI module. During the experiment, CO2 and
brine are injected using two separate ISCO syringe pumps at a
constant flow rate, and the pore pressure is controlled by a back-
pressure regulator (BP-2080-M, Jasco, Japan), with an accuracy of
0.1 MPa. The signal of the pressure sensor is collected by the A/D
module (Advantech). In order to ensure that the CO2 reaches the
supercritical state, the experimental temperature is controlled by a
heating circulator (F25-ME, Julabo, German) with a range of 245e
473 K and an accuracy of 0.1 K (Yang et al., 2011; Teng et al., 2016).
The core holder is placed in a high-field NMR system that uses a
9.4 T magnet equipped with shielded gradient coils providing a
maximum gradient strength of 50  104 T/cm. The core holder
material is made of polyimide and titanium alloy which do not
interfere with the nuclear magnetic signal. The design temperature
is 70  C and the design pressure is 15 MPa (Zhao et al., 2013). After
several updates, the core holder can now reach a maximum pres-
sure of 34 MPa and temperature of 148  C (Teng et al., 2018). As
shown in Table 2, the experimental samples are mainly packed
glass beads and synthetic rock samples. The system can monitor the
behavior of either gas or SC-CO2 during the displacement of water
or organic fluids in real time by MRI module. However, the core
analysis system of NMR still has some shortcomings:
(1) According to Table 2, most of the experimental samples are
packed glass beads or synthetic sandstone, but the cores in
natural reservoirs contain more paramagnetic materials. As
high-field NMR is more sensitive to these paramagnetic
materials, it will cause significant image distortion and
deleterious impact on experimental results.
(2) According to the published literature, the core holder can
only accommodate short core samples. For the displacement
process, a longer core is preferred as it can better reflect the
internal migration characteristics of rock.
(3) Similar to the low-field system, this core holder cannot be
used to simultaneously measure the rock mechanics prop-
erties and multi-field coupling effects.
3.2.3. Low-field NMR rock core experimental system at IRSM of CAS
The high-field NMR system is not suitable for paramagnetic
materials, thus most tests are conducted on either glass beads or
Berea sandstone representing reservoirs with a high porosity and
permeability. However, the porosity and permeability of actual CO2
reservoirs in China are quite different. The systems developed at
Tsinghua University and Dalian University of Technology in China
can only carry out experiments under hydrostatic pressure as the
field horizontal stress is not always equal to the vertical stress. In
this instance, the coupling effects of the stress, chemical and tem-
perature fields are rarely studied. As a result, a system was designed
to study the physical properties and fluid migration characteristics
in rocks when CO2 displaces water or oil under different temper-
ature and stress conditions.
The high-pressure NMR rock core flooding system at ISRM of
CAS is shown in Fig. 5. It consists of three modules: a fluid injection
module, a NMR module and a fluid production module. The rock
core sample is placed in the core holder and different pressures are
applied to the sample using an ISCO syringe pump. CO2 and brine
are pressurized using separate ISCO syringe pumps and enter a
mixer to be fully equilibrated. The equilibrated and mixed fluid
flows are then allowed into the sample. The pressure of the whole
system is controlled by the ISCO pumps and back-pressure valve.
The core holder is placed in a low-field NMR system, and its
maximum pressure and temperature are 20 MPa and 90  C,
 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
Fig. 5. Schematic diagrams of the high-pressure NMR rock core flooding experimental system at the IRSM of CAS: (a) The NMR rock core experimental system; and (b) The
schematic of holder.
respectively. This setup has the following advantages and
disadvantages:
(1) It uses low-field NMR which has low sensitivity to para-
magnetic materials, and thus can be used to analyze the
natural reservoir rocks.
(2) The core holder can be used for various rock sample sizes and
shapes including cylindrical rock samples of various sizes
(e.g. a core with a diameter of 25 mm and a length of 50 mm,
or a core with a diameter of 50 mm and a length of 100 mm)
and cubic rock samples of different sizes.
(3) CO2 can be injected from either the end of the rock sample, or
the middle of the rock sample. The migration of CO2 from the
middle of the rock sample to both ends can be observed.
(4) The core holder has axial compression loading parts and can
simulate the process that CO2 displaces brine or oil in a real
stress environment to analyze the changes of rock physical
properties.
(5) The image accuracy of this low-field MRI system is less than
that of high-field MRI system. As such, high-performance
imaging algorithms and software packages are required.
899
(6) Although a displacement sensor is installed at one end of the
core holder, merely the axial deformation of the whole
sample can be measured. The stress and strain in all di-
rections cannot be measured as traditional gages such as
extensometer can influence the NMR signals. Application of
multichannel fiber Bragg grating sensor technology has been
successfully implemented at IRSM of CAS in recent years
(Sun et al., 2017). It is necessary to combine the low-field
NMR rock core experimental system with the multichannel
fiber Bragg grating sensor in order to monitor the stress and
strain of each part of the surface of the rock sample during
CCUS displacement.
4. Application of NMR to CCUS core analysis
4.1. Measuring porosity and pore size distribution
Porosity and PSD play significant roles in most natural materials
and influence the physical properties of these materials such as
diffusion coefficient, thermal conductivity, fluid permeability and
capillary force (Yu et al., 2016). At present, the main methods for
900 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
measuring the porosity and PSD of reservoir include mercury
intrusion porosimetry (MIP), the gas research institute (GRI) method,
nitrogen adsorption, NMR and so on (Wang et al., 2014). MIP is used
to establish the relationship between mercury content and pressure
using the characteristic that mercury will be injected into pores of
varying size under different pressures allowing both the pore volume
and PSD of a porous medium to be determined (Chen et al., 2018).
However, actual CCUS reservoirs in China are usually tight sandstone
or carbonate rocks with small natural pores. If the MIP method is
adopted, a high pressure of mercury injection is required putting
significant strain on both the equipment and the rock being studied.
At the same time, MIP will destroy the core and thus it cannot be
used to analyze the change in pore structure before and after CO2
injection. The GRI method can be utilized to calculate the porosity of
irregular samples using Boyle’s law and Archimedes buoyancy
principle (Jochen et al., 1993; Luffel et al., 1993). However, there are
many factors that cause significant experimental errors, and the
degree of influence of these factors is uncertain. It is rather difficult to
use this method for measuring low permeability cores. Furthermore,
when the porosity of rock samples before and after CO2 injection is
measured by GRI, the drying and cooling process will lead to CO2
escape or evaporation of water and oil, resulting in a measured
porosity that has lost practical meaning. The nitrogen adsorption
method is based on the adsorption characteristics of liquid nitrogen
on solid surfaces to determine the specific surface area and PSD of
rock samples. The adsorption capacity of liquid nitrogen changes
with the relative pressure P/P0, where P is the partial pressure of
adsorbate, and P0 is the saturated vapor pressure of adsorbent. Multi-
point BET (BrunauereEmmetteTeller) analysis method is used to
obtain the specific surface area of rock samples and density func-
tional theory is used to obtain the PSD (Scherdel et al., 2010). Despite
the advantage of not being a destructive method, the nitrogen
adsorption method cannot be used to monitor the change in sample
porosity in real time. With the principles and application of NMR,
there are many methods to measure porosity and PSD, such as NMR
cryoporometry where samples undergo a freezing-thawing cycle,
NMR diffusometry which is based on the diffusion coefficient, and
traditional NMR relaxation method. NMR cryoporometry is a quan-
titative method based on the GibbseThomson equation to measure
the PSD. With this method, water-saturated rock samples undergo a
process of freezing-thawing and NMR is used to measure the liquid
change of water in the process of phase change. The PSD inside the
rock sample is obtained by analyzing the melting curve (Zhou et al.,
2016, 2017; Zhou, 2018). NMR diffusometry involves measuring the
diffusivity of liquid inside the porous material for differing mea-
surement times. The method provides a measure of the surface to
volume ratio of the pore structure in a short observation time, and a
measure of the tortuosity of the pore structure in a long observation
time (Collins et al., 2007). Both these methods can be used to analyze
rock porosity and PSD; however, they are not suitable for real-time
analysis of changes in rock properties when CO2 is injected in a
core flooding scenario. In this instance, the traditional relaxation
method is more suitable for linkage with the displacement system
used for CCUS in determining the porosity characteristics.
According to Eq. (2), the NMR signal intensity value of fluid in
the pore of a saturated core is directly proportional to the volume of
fluid. Since heavy water which does not present NMR activity can
simulate rock skeletons, a known ratio mixture of water and heavy
water can be used as a standard porosity sample. Glass micro-
spheres or porous ceramics can also be used as standard samples.
As such, after the NMR instrument is calibrated with a set of
standard samples, the porosity of the core can be measured directly.
However, the complex mineral composition of a natural core ac-
celerates the signal attenuation. If the measurement parameters are
not chosen properly, it will lead to obvious errors; therefore, it is
better to use the same kind of rock samples for calibration (Xiao
et al., 2016). For different core samples from CCUS reservoirs, the
measurement parameters should be optimized.
The NMR signals from a saturated core are the superposition of
responses from different pore sizes. The dominant relaxation pro-
cess of pore fluid is the surface relaxation, which is mainly affected
by pore structure. According to the model of surface relaxation and
specific surface area, a smaller pore size will result in a shorter
relaxation time. By using different inversion methods to obtain the
ratio of different relaxation time signals in the total signal, the PSD
in the core can be obtained. Common inversion methods include
singular value decomposition (SVD), joint iterative reconstruction
inversion, conjugate gradient method (Dunn and LaTorraca, 1999),
smooth and block inversion (Mohnke and Yaramanci, 2002) and
genetic algorithm (Lin et al., 2011). Ge et al. (2017a, b) proposed a
CPMG (Carr, Purcell, Meiboom, and Gill) pulse sequence that
changes the echo time. The stability and convergence of this
inversion algorithm were enhanced by a combination of truncated
singular value decomposition (TSVD) and simultaneous iterative
reconstruction technique (SIRT) algorithms. And Liu et al. (2019)
proposed a joint inversion algorithm named ‘‘composite-data-
processing” to obtain the 3D correlation map.
A histogram of the NMR signals from different relaxation times
is obtained. In this way, the distribution of pores and pore fluids can
be determined. Surface relaxation time is related to the pore size,
but the relationship between the surface relaxation intensity and
specific surface area cannot be directly measured. Toumelin et al.
(2007) and Talabi et al. (2009) proposed a random walk method
and a maximal ball algorithm to estimate the surface relaxation
intensity. This method is cumbersome and complex and its appli-
cability is very limited. At present, MIP is still commonly used for
calibration of this method. Comparing the PSD curve obtained by
MIP with the T2 spectrum obtained by NMR, the conversion coef-
ficient between the NMR determined T2 spectrum and the PSD can
be obtained (Li et al., 2018).
Fig. 6 shows the PSD of five different samples measured by NMR
and MIP (Gao et al., 2018). The curves obtained by the two methods
are similar, both generally showing a bimodal distribution and a
consistency in curve shape, suggesting that it can transform the T2
spectra into a PSD. Fig. 6 also compares the PSD measured by MIP
and NMR, showing several anomalous artefacts and shifts pre-
sumably due to large amounts of diamagnetic materials. The pore
size measured by MIP ranges from 3 nm to 120 mm, which is not
completely accurate and comprehensive for nano-scale pores. For
an ultra-low permeability rock, the pore size measured by MIP is far
lower than the actual porosity. Theoretically, NMR can be used to
measure PSD even in these more extreme ranges (Scherdel et al.,
2010; Gao et al., 2018). As shown in Fig. 6, the range of PSD
measured by NMR is wider than that measured by MIP. Further-
more, the MIP method is destructive, which can compromise the
experimental results. However, there are still some aspects that
should be improved in order to quantify the pore structure of rocks
by conventional relaxation method:
(1) Short relaxation time components are very important for
pore structure measurement of low permeability rocks.
However, high-performance algorithms and equipment are
required to analyze these short relaxation time components.
(2) The relationship between pore size and T2 is generally based
on spherical, tubular, and plate models, which are simplifi-
cations of complex pore structures. New models need to be
developed according to the pore morphology and connec-
tivity characteristics of natural cores.
(3) The PSD cannot be obtained directly from T2 distribution of
the NMR signals. It needs to be calibrated by other
 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908 901

Fig. 6. Comparison between pore size distributions of MIP and NMR (Gao et al., 2018).

measurement methods. Thus, a reliable and accurate method (1) SDR model:
for doing this needs to be standardized.
(4) It is often necessary to try to combine other methods (such as
4
cryoporometry and diffusometry) with the systems used for fNMR
K ¼ CSDR T 22g (3)
CCUS to improve the accuracy of experimental results. 100
(5) For tight rock, as the rock sample is dominated by very small
pores with possible diffusional couplings between the
nanopores, traditional relaxation method may not hold for
such a tight rock system. (2) Coates model:
(6) Paramagnetic materials in natural cores can accelerate the
attenuation of NMR signals and make the T2 shift, compli- !4
2
cating the detection of liquids in some small pores. fNMR FEI
K ¼ (4)
CCoates­cutoff BVI

4.2. Measuring permeability

Table 3 lists the traditional methods for determining the (3) Coates-Sbvi model:
permeability of rock samples and summarizes their advantages and
disadvantages. Compared with the traditional methods for

4
2
permeability measurement, NMR technology has the advantage of fNMR fNMR­mobile
K ¼ (5)
being nondestructive, non-toxic, harmless, non-polluting, faster, CCoates­Sbvi fNMR­immobile
simpler and only sensitive to fluid. With this technique, there are
three empirical models for calculating rock sample permeability: where K is the permeability; CSDR, CCoates-cutoff, and CCoates-Sbvi are
SDR model (Kenyon et al., 1988), Coates model (Coates et al., 1998), the correction coefficients of the three models, respectively; fNMR-
and Coates-Sbvi model (Xiao, 1998). mobile and fNMR-immobile are the porosities of bound and movable

Table 3
The methods of measuring permeability in laboratory.
Method Principle
Steady state Constant The sample is provided with a
method flow method constant flow rate, and the pressure
difference at both ends of the
sample is monitored by the
pressure differential meter. The
permeability of the sample is
calculated by Darcy’s law
Constant The sample is provided with a
pressure method constant pressure difference at both
ends of the sample, and the flow
rate of the sample is monitored by
the flow meter. The permeability of
the sample is calculated by Darcy’s
law
Non-steady Pulse decay An instantaneous pressure pulse is
state method method applied at one end of the sample
and the pressure difference
between the two ends is monitored.
The permeability of the sample is
calculated according to Darcy’s law
Pressure The specific oscillating pressure is
oscillation method applied at one end of the sample
and the pressure response at the
other end is monitored. The
permeability and specific volume
water of the sample are measured
Unconventional The sample is provided with a
steady state constant pressure difference at both
method ends of the sample, and the flow
rate of the sample is monitored by
the flow meter. The permeability of
the sample is calculated by Darcy’s
law
Range (mD) Advantage
0.1 The method is simple with few
influence factors, and is suitable for
measuring the mediumehigh
permeability materials
0.1 It is easier to control pressure with
high accuracy than flow rate. The
method is simple with few
influence factors, and is suitable for
measuring the mediumehigh
permeability materials
Traditional pulse Since the flow does not need to be
decay method: stable and experiment time is
1  105 to 0.1 saved, especially for mediumelow
Storage-variable permeability materials, the
pulse decay method: experiment is fast and the accuracy
1  105 to 100 is high
1  106 to 10 Fast and adaptable
1  106 The flow does not need to be stable,
and the flow is monitored by a
high-resolution metering pump.
Experiment time is saved
902
Disadvantage
L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
The measuring time of low
permeability materials is long. The
instability factors are increased, and
non-Darcy flow may be caused by
high hydraulic gradient
The measuring time of low
permeability materials is long. The
instability factors are increased, and
non-Darcy flow may be caused by
high hydraulic gradient
This method is not suitable for
determination of high permeability
materials, as its basic hypothesis is
invalid
This method is greatly influenced
by environmental factors, and the
cost of equipment is high, which is
not conducive to popularization
This method requires a specific high
precision metering pump, which is
not conducive to popularization
 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908 903

fluids, respectively; FEI is the volume of movable water; BVI is the permeability rock, the permeability is consistent with the
volume of bound water; and T2g is the geometric average of the T2 predictions of the above model. However, it is not suitable for
spectrum. low and ultra-low permeability rock samples, such as shales.
In the Coates model, it is necessary to determine T2-cutoff. The (4) As the relative permeability of water and gas in rocks
value of T2-cutoff can be determined only if the optimum centrifugal measured by NMR technology is not accurate, more accurate
force is known first. It is generally obtained by comparing the T2 models need to be developed to overcome these
spectrum accumulation curve before and after centrifugation. inaccuracies.
Wang et al. (1998) measured the moveable fluid porosity in the rock
matrix of Xiaoguai oilfield with a centrifugal force of 1 MPa How-
ever, many scholars propose that different centrifugal forces should
4.3. Monitoring distribution and migration of fluid in pores
be used to calculate T2-cutoff for different rocks. Some scholars
proposed that 2.25 MPa is the most suitable centrifugal force for
Table 4 lists the current major methods for monitoring the
low permeabale rock samples.
distribution and migration of fluid, associated with the experi-
By studying four different types of low permeability cores
mental principles, advantages and disadvantages. NMR technology
sampled from Xinjiang oilfield, China, Peng et al. (2006) proposed
has the advantages of nondestructive detection, as it is able to
another SDR-REV model, which considers two indices used in the
locate the fluid in the rock pore space, characterized by less inter-
SDR model as correction coefficients. These correction coefficients
ference from other factors, simple operation, and high precision.
were obtained using statistical analysis of the measured data of
This method can be used to monitor the fluid migration in fluid
local rock samples. This model has its own advantages in calcu-
displacement studies for CCUS.
lating the permeability of different core samples, such as CO2
The NMR signals of core directly reflect the volume of hydrogen-
storage and caprock.
containing fluid in the core. Interpolating the NMR signals of un-
In addition to absolute permeability, NMR is used to measure the
saturated and saturated cores allows for core saturation to be
relative permeability of CO2 and water as it can measure saturation
determined. Furthermore, local saturation changes can be obtained
nondestructively (Ma et al., 2013). Song et al. (2012) analyzed the
through the brightness change in MRI images (Ronen and Kim,
influence of viscosity, gravity and capillary force on two-phase flow
2000). The NMR signals correspond to the residual saturation of
by Goodfield method. Kadkhodaie et al. (2019) proposed a method to
the core through CCUS displacement experiment. The T2 spectrum
get the relative permeability curves from the NMR-derived MICP
shows the distribution of residual fluid in different pores, and the
(mercury injection capillary pressure) data by using the Wyllie and
complementary signal amplitude and distribution correspond to
Gardner equations. But it needs a lot of complicated steps and not
the distribution of movable fluid in the core.
suitable for the laboratory scale.
Although CO2 flooding technology has been developed for many
There are still some shortcomings using NMR technology to test
years, the methods for monitoring CO2 injected into full-diameter
the permeability of rock samples:
core by NMR technology are less than 20 years old, an active
research area to date. When a core contains both water and oil, the
(1) There is no uniform standard for selection of T2-cutoff, and the
proportions of water and oil can be distinguished by addition of
calculation of T2-cutoff by centrifuge tests should be improved.
MnCl2 to the water phase to shorten the relaxation time of the pore
Furthermore, for natural samples containing paramagnetic
water (Zhang et al., 2018). This method has been widely used to
materials, the measurement of T2-cutoff can be affected.
evaluate the displacement effect of oil and gas fields, and it is also
(2) For rock samples with natural fractures or heterogeneities,
effective to analyze the residual oil and gas in high water cut oil and
the existing models cannot accurately determine the true
gas fields displaced by CO2. Mehana and El-monier (2016) analyzed
permeability of the sample, and as a result, better models for
the pore structure and fluid distribution of shale samples by T2
permeability determination need to be developed.
spectrum. Khatibi et al. (2019) proposed a new approach to identify
(3) The above permeability models were developed primarily
different components in tight shale samples and to establish a
for sandstone and limestone samples, i.e. for mediumehigh
relationship between the NMR T1-T2 map. Zhang et al. (2012)

Table 4
The methods of monitoring fluid inside cores in laboratory.

Method Principle Advantage Disadvantage

X-ray computed The object is irradiated by high energy
tomography (CT) ray, and the internal structure of the
object is detected by analyzing the
attenuation coefficient of X-ray
Resistivity Resistivity is a comprehensive
measurement reflection of the resistivity of rock
skeleton and pore fluid.
Fluid migration is inversed by
measuring the resistivity changes on
the surface of the rock sample
Ultrasonic wave Based on the attenuation changes of the
measurement velocity and amplitude of the ultrasonic
wave in the rock samples, the fluid
characteristics in the pores of the rock
were retrieved
NMR Mapping the intensity distribution of
NMR signals at different positions to
obtain NMR images
Nondestructive detection, high
resolution, digitization
Easy to operate, adaptable, easy to
solve, low cost in experiment
Simple, intuitive, relatively economic,
repeatable, applicable to multiple scales
Only detecting the location of fluid in
the pores of the rock, few influence
factors, simple operation, high precision
(1) Resolution and vision are
contradictory;
(2) It is impossible to distinguish certain
objects of similar density
(1) Low precision and only
measurement of the rock surface;
(2) Inversion is non-unique
(1) The sensitivity of P-wave velocity is
low under low saturation condition;
(2) They are greatly influenced by the
external environment
Paramagnetic substances have an effect
on NMR signals
904 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
Fig. 7. T2 spectrum in the process of CO2 displacing oil in ultra-low permeability
sandstone (Xiao et al., 2017).
combined the NMR and component analysis technology to study
the mechanism of CO2 flooding in ultra-low permeability reser-
voirs. They found that the CO2 mainly extracts the components of
C5eC18 in immiscible flooding, and the recovery efficiency is 18%
higher than that of water flooding. They also found that the com-
ponents of C19eC25 can be extracted in miscible flooding, and the
recovery efficiency is 34% higher than that of water flooding. Xiao
et al. (2017) considered that CO2 injection schemes has the
different effect by comparing four kinds of CO2 injection schemes
which are waterealternating-gas (CO2/water), immiscible flooding,
Fig. 8. MRI images of CO2 immiscible displacement in packed glass beads with different glass sizes (Jiang et al., 2017). The yellow part represents the water, while the CO2 without
NMR signal is represented in black.
miscible flooding, and cyclic CO2 injection in extra/ultra-low
permeability reservoir using NMR technology. Fig. 7 shows the T2
spectrum changes of the whole sample when CO2 displaces oil in
ultra-low permeability sandstone (Xiao et al., 2017).
Due to the heterogeneity and anisotropy of natural rocks, actual
CCUS projects will not only monitor the overall distribution of fluids
in rock samples, but also observe the flow of fluids in various parts of
the rock samples. MRI technology is used to solve this issue through
real-time imaging during the displacement process. Fig. 8 presents an
MRI image showing the process that the SC-CO2 displaces deionized
water in packed glass beads (Jiang et al., 2017). It can be clearly seen
that there are dominant channels in the experimental sample. CO2
displaces the edge water of rock sample at the beginning. With an
increase in CO2 content, CO2 passes through the center of rock sample
preferentially and there is an obvious fingering phenomenon. The
final displacement efficiency can be obtained through the relaxation
time spectrum to correlate with the MRI image.
MRI and X-ray computed tomography (CT) are both real-time
nondestructive imaging methods; however, their imaging princi-
ples are totally different. X-ray CT is used to irradiate the object
being imaged with high energy X-rays and the internal structure of
detected object through attenuation of the X-ray beam in the im-
aging voxel. The CT number closely related to the density of the
material describes the intensity of the X-ray attenuation in a small
voxel inside the sample and it is used to map the porosity and fluid
saturation inside porous materials (Zhang et al., 2014). Generally,
slices were reconstructed at 512  512 pixels in each scan (Zhang
et al., 2015a, b). The image reflects the 3D spatial distribution of
material density or atomic number, nevertheless it provides no
information on the interaction between fluid and rock matrix (Sun
et al., 2016). Furthermore, it cannot be used to understand multi-
phase and multi-field coupling seepage mechanics. On the other
 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
hand, MRI can detect the location of fluids in the rock pore space
and the interfacial effects of fluid and surrounding pores; however,
it does not provide information on the rock skeleton, making it
complementary to X-ray CT as an imaging approach. The geometric
space covered by MRI images is called the field of view and is
divided into grids to distinguish the location of magnetic resonance
signals. Generally, it is divided into grids of either 128  128 or
256  256, which are called imaging matrices. Image resolution is
the field of view divided by the number of matrix grids. At present,
the resolution of MRI is generally at the submillimeter level (Werth
et al., 2010).
However, there are still some problems when using NMR
technology to monitor fluid migration:
(1) NMR technology can be divided into low- and high-field ones.
It is generally believed that increasing the field intensity can
improve the signal-to-noise ratio, thus speed up the imaging,
and at the same time, the higher field intensity can improve
the chemical displacement difference of 1H atoms in different
fluids, so as to improve the resolution of different liquid types.
However, for natural materials such as rocks, the in-
homogeneity of the internal magnetic field gradient will in-
crease correspondingly with the external stress field. This will
lead to an increase in artifacts associated with motion and
change, affecting the accuracy of measurement.
(2) There is a trade-off between accuracy and vision. If a higher
resolution is achieved, the field of vision needs to be limited
within a certain range.
(3) At present, there is no multi-functional and commercial
post-processing software for MRI core analysis. According to
the literature, most of the image processing is performed
using ImageJ or other medical MRI software packages.
(4) The paramagnetic material has an effect on the NMR signals,
which may distort the image and affect the imaging quality.
5. Conclusions
A deep understanding of the physical changes of reservoirs and
caprock and the migration of CO2 in reservoir is essential for site
selection and safety risk assessment of CCUS projects. At present,
there are many NMR systems used in the CCUS field throughout the
world. From low-field to high-field, from NMR to MRI, from CO2-
EWR to CO2-EOR, a large number of models have been proposed to
date. Some progress has been made in manufacture of NMR sys-
tems and development of NMR displacement systems, but more
works are needed. The development of porosity models and
establishment of robust and practical empirical permeability
formulae are the areas where we should focus on. For China’s actual
CCUS reservoirs, which are usually low or ultra-low permeability
reservoirs, the issues using NMR based methods are challenging.
Many Chinese scholars have made significant contributions to NMR
signal processing algorithms, selection of optimal centrifugal force
and T2-cutoff determination of permeability and relative perme-
ability, analysis of lag effect, and viscosity and buoyancy by high-
resolution MRI. Nevertheless, based on the existing experimental
studies, there are still some challenges:
(1) The paramagnetic materials such as rocks have an effect on
the NMR signals, which will accelerate the attenuation of
NMR signals. As a result, the relaxation time spectrum is
offset and the NMR signals of liquids in some small pores
cannot be well monitored. Paramagnetic materials also affect
905
MRI, which will make the images being deformed. Therefore,
many paramagnetic materials need to be analyzed by NMR
apparatus, such as designing different pulse sequences.
Technical breakthroughs are needed to account for the ef-
fects of paramagnetic materials on NMR signals.
(2) It is not likely to obtain the PSD of rock samples directly from
T2 using NMR signals. It needs to be calibrated by other
measuring methods. For the calibration methods, a unified
standard should be established. Meanwhile, the relationship
between pore size and T2 generally adopts spherical, tubular
and plate models, which are slightly simpler for rather
complex pore structures. New models need to be developed
according to the pore morphology and connectivity charac-
teristics of natural cores. For tight rock, as the rock sample is
dominated by very small pores with possible diffusional
couplings between the nanopores, the traditional relaxation
method may not hold.
(3) The target reservoirs and caprock of CCUS are basically
characterized by strong heterogeneity and anisotropy. Un-
fortunately, although the current NMR signals can give T2 of
the whole experimental samples, the spatial characteristics
of the samples cannot be well described.
(4) As natural structures such as caverns and fractures may exist
in natural rocks, using NMR and MRI to identify natural
structures and analyze the effects of these structures on
reservation and security of reservoir will become a hot topic.
(5) Most of the image processing software packages currently
used in CCUS core analyses are ImageJ or other medical MRI
software packages. As the threshold value of medical imag-
ing software is different from that of natural rocks, new
commercial multifunctional MRI software for geotechnical
engineering is needed.
(6) Temperature, stress and chemical coupling fields can affect
the pore fluid in rocks. Currently, NMR core analysis focuses
on the occurrence state and seepage characteristics of fluids
in rocks, but the coupling effects of stress (confining pres-
sure, pore pressure), temperature and chemistry should be
studied.
(7) The traditional stress and strain gages such as extensometer
have significant influence on the NMR signals. It is necessary
to combine the NMR rock core experimental system with
multichannel fiber Bragg grating sensor to monitor the stress
and strain of each part of the surface of the rock sample
during CCUS displacement.
(8) NMR core analysis used in CCUS field has introduced a series
of theories from physics, biology and chemistry. In fact, core
analysis echoes on new requirements for NMR technology. It
is likely that we should develop new technologies or theories
upon these basic scientific issues.
Conflicts of interest
The authors wish to confirm that there are no known conflicts of
interest associated with this publication and there has been no
significant financial support for this work that could have influ-
enced its outcome.
Acknowledgments
This work is mainly supported by the Open Research Fund of
State Key Laboratory of Geomechanics and Geotechnical
906 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908
Engineering, IRSM, CAS (Grant No. Z017002), and the National
Natural Science Foundation of China (Grant Nos. 41872210 and
41274111). Q. Li and M. Myers also acknowledge the financial sup-
port from the China-Australia Geological Storage of CO2 (CAGS)
Project funded by the Australian Government under the auspices of
the China-Australia Joint Coordination Group on Clean Coal Tech-
nology. Additionally, the authors give special thanks to three
anonymous reviewers for their insightful comments on this article.
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Liang Xu is a doctoral student from the Institute of Rock
and Soil Mechanics, Chinese Academy of Sciences. His in-
terest is to observe the migration characteristics of carbon
dioxide in anisotropic rocks using diverse monitoring
methods. His research is under the direction of Prof. Qi Li
(IRSM, CAS). E-mail: 1921212637@qq.com
Qi Li holds a BS in Earth Sciences with diploma of minor
programme on Computer Science from Nanjing University,
China (1995), and a MS in Hydrogeology and Engineering
Geology from the same University (1998). In 2004, he
received a PhD degree in Civil Engineering from Ibaraki
University, Japan. Before joining the State Key Laboratory of
Geomechanics and Geotechnical Engineering, Institute of
Rock and Soil Mechanics (IRSM), Chinese Academy of Sci-
ences, Wuhan, China, he has been a member of Geological
Survey of Japan, Tsukuba, from 2005 to 2010. Dr. Li is now the
Professor of IRSM; he is a geoscientist with expertise in the
fields of hydrogeology and engineering mechanics. The focus
of Prof. Li’s research is to understand and use laboratory and
numerical tools to design novel subsurface disposal pro-
cesses and site monitoring systems on different temporo-spatial scales.
908 L. Xu et al. / Journal of Rock Mechanics and Geotechnical Engineering 11 (2019) 892e908

Matthew Myers obtained his B.S. in Chemical Engineering
from the California Institute of Technology in 2003 and his
Ph.D. in organic chemistry and materials science with Prof.
Colin Nuckolls at Columbia University (New York City) in
2008, for work on curved polycyclic aromatic hydrocar-
bons and their applications in organic electronics. He is
currently a senior research scientist at CSIRO (Australia)
working on oil and gas related technologies with a
particular focus on carbon capture and storage and the
utilization of CO2 for enhanced oil recovery. His research
interests focus on chemical sensor development, envi-
ronmental gas monitoring, high pressure/temperature
rock core flooding and chemical tracers.