Nanofluid of graphene-based amphiphilic Janus
nanosheets for tertiary or enhanced oil recovery:
High performance at low concentration
Dan Luoa,b,c,1, Feng Wanga,1, Jingyi Zhuc, Feng Caoa, Yuan Liua, Xiaogang Lic, Richard C. Willsonb,d, Zhaozhong Yangc,2,
Ching-Wu Chua,e,2, and Zhifeng Rena,2
a
Department of Physics and Texas Center for Superconductivity, University of Houston, Houston, TX 77204; bDepartment of Chemical and Biomolecular
Engineering, University of Houston, Houston, TX 77204; cState Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum
University, Chengdu, Sichuan 610500, China; dDepartamento de Biotecnología e Ingeniería de Alimentos, Tecnologico de Monterrey, Monterrey,
Nuevo Leon 64849, Mexico; and eLawrence Berkeley National Laboratory, Berkeley, CA 94720
Contributed by Ching-Wu Chu, May 25, 2016 (sent for review April 28, 2016; reviewed by Caili Dai and Dapeng Yu)
The current simple nanofluid flooding method for tertiary or
enhanced oil recovery is inefficient, especially when used with
low nanoparticle concentration. We have designed and produced
a nanofluid of graphene-based amphiphilic nanosheets that is very
effective at low concentration. Our nanosheets spontaneously
approached the oil–water interface and reduced the interfacial
tension in a saline environment (4 wt % NaCl and 1 wt % CaCl2),
regardless of the solid surface wettability. A climbing film
appeared and grew at moderate hydrodynamic condition to en-
capsulate the oil phase. With strong hydrodynamic power input, a
solid-like interfacial film formed and was able to return to its orig-
inal form even after being seriously disturbed. The film rapidly
separated oil and water phases for slug-like oil displacement.
The unique behavior of our nanosheet nanofluid tripled the best
performance of conventional nanofluid flooding methods under
similar conditions.
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nanofluid flooding amphiphilic Janus nanosheets | enhanced oil
| |
recovery climbing film interfacial film
F inding economically viable and environmentally friendly
methods to extract the huge amount of residual oil after
primary and secondary recovery remains challenging for the oil
and gas industry and is also of significant importance in efforts to
satisfy the world’s increasing energy demand. Nanofluid flooding
as an alternative tertiary oil recovery method has been recently
reported (1–5). Obviously, simple nanofluid flooding (containing
only nanoparticles) at low concentration (0.01 wt % or less)
shows the greatest potential from the environmental and eco-
nomic perspective. Several corresponding oil displacement
mechanisms have also been introduced, including reduction of
oil–water interfacial tension (6, 7), alteration of rock surface
wettability (8–10), and generation of structural disjoining pres-
sure (11–13). However, the oil recovery factor is below 5% with
0.01% nanoparticle loading in core flooding tests in a saline
environment (2 wt % or higher NaCl content). Here we show
that an oil recovery factor of 15.2% is achieved by using a simple
nanofluid of graphene-based Janus amphiphilic nanosheets.
To our knowledge, this is the first report of applying nanofluid of
amphiphilic Janus two-dimensional materials in tertiary or en-
hanced oil recovery. We found that in a saline environment, the
nanosheets spontaneously approach the oil–water interface, re-
ducing the interfacial tension. A climbing film emerges and en-
capsulates the oil phase and may carry it forward. Furthermore,
we found that a solid-like film forms with strong hydrodynamic
power. The film rapidly separates oil and water for slug-like oil
displacement. Even though there are ways to achieve 20% en-
hanced recovery by complicated alkali/surfactant/polymer flood-
ing (14) or by surfactants with added nanoparticles (5), the
necessary concentrations of the chemicals and nanoparticles
are much higher than 0.01 wt %. Our results provide a nanofluid
www.pnas.org/cgi/doi/10.1073/pnas.1608135113
flooding method for tertiary oil recovery that is comparable to the
sophisticated chemical methods. We anticipate that this work will
bring simple nanofluid flooding at low concentration to the stage
of oil field practice, which could result in oil being recovered in a
more environmentally friendly and cost-effective manner.
Materials and Methods
APPLIED PHYSICAL
Synthesis. The Janus amphiphilic nanosheets were produced by tuning the Janus
SCIENCES
balance of graphene oxide (GO) with alkylamine. Initially, GO was synthesized
from chemical oxidation of graphite (15). Single-surface hydrophobization was
then carried out (16, 17). The nanofluid was made stable to avoid agglomer-
ation of the nanosheets. Brine used in all experiments contained 4 wt % NaCl
and 1 wt % CaCl2.
Characterization. Atomic force microscopy (AFM; Veeco Dimensions 3000 atomic
force microscope) was used to examine the morphology of GO. Measurement was
conducted using silicon AFM probes (HQ:NSC15/AL BS, Mikromasch) with a resonant
frequency of ∼325 kHz, a force constant of ∼40 N m−1, and a tip radius of ∼8 nm.
Imaging was done in tapping mode with resolutions of 512 × 512. Scanning electron
microscopy (SEM; FEI Quanta 200) was used to examine the cross-section of the
sandstone cores under an accelerating voltage of 20 kV. Fourier transform infrared
spectroscopy (FTIR) spectra were recorded on a Nicolet iS50 FTIR spectrometer with
an attenuated total reflectance accessory. Thermal gravimetric analysis (TGA) was
Significance
Improving crude oil recovery by 1% worldwide would result in
a huge amount of crude oil resources becoming available.
However, the economic and environmental concerns are too
serious to ignore when chemical methods (surfactants or
polymers flooding, etc.) are used for an average 10–20% en-
hancement for tertiary oil recovery. Simple nanofluid (con-
taining only nanoparticles) flooding at low concentration
(0.01 wt % or less) is a promising alternative, but the efficiency
is below 5% in a saline environment (2 wt % or higher NaCl
content). We report a simple nanofluid of graphene-based Ja-
nus amphiphilic nanosheets for enhanced oil recovery with
efficiency of about 15.2%, comparable to chemical methods,
which is both economically and environmentally beneficial to the
petroleum industry.
Author contributions: D.L. and Z.R. conceived the original idea; D.L., F.W., R.C.W., and Z.Y.
designed research; D.L., F.W., J.Z., F.C., Y.L., and X.L. performed research; D.L., F.W., F.C.,
Y.L., and R.C.W. analyzed data; Z.Y., C.-W.C., and Z.R. supervised the project; and D.L.,
F.W., C.-W.C., and Z.R. wrote the paper.
Reviewers: C.D., China University of Petroleum, Huadong Campus; and D.Y., Peking
University.
The authors declare no conflict of interest.
1
D.L. and F.W. contributed equally to this work.
2
To whom correspondence may be addressed. Email: Yangzhaozhong@swpu.edu.cn, cwchu@
uh.edu, or zren@uh.edu.
This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.
1073/pnas.1608135113/-/DCSupplemental.
PNAS | July 12, 2016 | vol. 113 | no. 28 | 7711–7716

Fig. 1. Behaviors of unmodified GO and amphiphilic nanosheets in the
heptane/brine system. Small pieces of interfacial film were attached to the
hydrophilic glass surface in the heptane phase due to its amphiphilicity,
which appeared as black dots.
performed on a TGA Q50 (TA Instrument) under nitrogen atmosphere at a rate of
10 °C/min. Particle size and concentration were detected and visualized using a
Malvern NanoSight NS300.
Core Flooding Test. Four man-made sandstone rock cores were tested in the
flooding equipment (Fig. S1). The physical properties of the rock cores were
measured and are listed in Table S1. Crude oil samples were taken from one of
China’s oil fields. The viscosity of the crude oil was 75 cP at 25 °C. Nanofluids of
0.005 wt % and 0.01 wt % nanosheet concentration were injected into a saline
environment (4 wt % NaCl and 1 wt % CaCl2) to measure the enhanced oil
recovery factor for rock cores with both low (samples 1 and 2) and high (samples
3 and 4) liquid permeability. The core flooding test was conducted sequentially
with the following steps: cleaning of rock cores; saturating cores with brine;
establishing initial brine water and oil saturation by oil injection until no more
brine water was produced; brine water flooding until no more oil (i.e., 100%
water cut) was produced; and nanofluid flooding until no more oil was
extracted. The total injection volume of nanofluid for each flooding test was 3–4
times the pore volume (PV).
Results and Discussion
Surface Functionalization of GO with Alkylamine. The thickness of
GO was estimated to be about 1 nm from the AFM image (Fig. S2),
indicating the single-layer feature of GO, in agreement with the
previous report (18). For comparison, we have also studied the
effect of unmodified GO. Either the unmodified GO or our am-
phiphilic Janus nanosheets were injected into the heptane/brine
system. The amphiphilic Janus nanosheets spontaneously accumu-
lated at the heptane/brine interface while GO stayed only in the
brine phase and instantaneously started to aggregate. When sub-
jected to vortex-induced vibrations, the amphiphilic Janus nano-
sheets formed a thin interfacial film separating the heptane and
brine in contrast to the GO agglomeration due to the salt screening
Fig. 2. (A) FTIR spectra and (B) TGA curves of GO and amphiphilic nanosheet.
7712 | www.pnas.org/cgi/doi/10.1073/pnas.1608135113
effect (Fig. 1). After settling for 2 h, unmodified GO precipitated
while the interfacial film of our nanosheets remained intact. This
observation suggested successful asymmetrical functionalization of
GO with hydrocarbon chains. In FTIR analysis (Fig. 2A), both
GO and amphiphilic nanosheets exhibited peaks at 1,723 cm−1,
1,587 cm−1, and 1,230 cm−1, which can be assigned to C=O car-
bonyl/carboxyl, C=C aromatic, and C–O–C epoxy vibrations,
respectively. In addition, amphiphilic nanosheets clearly dem-
onstrated the presence of methylene groups (strong peaks at
1,470 cm−1, 2,850 cm−1, and 2,925 cm−1) and methyl groups
(weaker signals at 1,380 cm−1 and 2,960 cm−1), which confirmed
the successful conjugation of hydrocarbon chains onto the GO
surface. Compared with GO, the TGA curve of amphiphilic
nanosheets displayed an additional weight loss stage between
400 °C and 500 °C, which may be attributed to the decomposition
of the carbon chains (Fig. 2B).
Stability Evaluation of the Nanofluid. It is crucial that the nanofluid
has good stability before being injected into the reservoir. From
observation, both GO and amphiphilic nanosheets have very small
amounts of precipitates even after 30 d. To evaluate the stability in
microscopic view, the dispersions of GO and amphiphilic nano-
sheets were first subjected to bath sonication for 30 s before dilution
to the concentration of 0.005 wt % and then injected into the
chamber in the Malvern NS300 system, in which a laser passes
through. Particles in the path of the laser scattered light and were
visualized by a camera. Altogether, five locations were observed,
each for a period of 60 s. Fig. 3 shows the average hydrodynamic
diameter distribution of GO (Fig. 3A) and amphiphilic nanosheets
(Fig. 3B). It appeared that the mode of hydrodynamic diameter of
amphiphilic nanosheets was rather close to that of GO, implying
that no agglomeration took place after functionalization. From the
captured video of nanofluid dispersion, we did not find any no-
ticeable aggregation. Photographs of amphiphilic nanosheet nano-
fluid in three locations at different time points were selected as
examples (Fig. 3C). Each bright dot in the photographs represented
a single nanosheet in Brownian motion. No aggregation, which
would display as clusters, was detected. The excellent stability of the
nanofluid would ensure that no extra additives or methods are re-
quired to preserve the nanofluid before injection.
Oil Displacement Efficiency and Mechanisms. Approximately 90% of
the oil recovered by nanofluid flooding was extracted after the first
PV injection. As shown in Table 1, under similar conditions (0.01%
nanofluid concentration), our recovery was 15.2%, more than triple
the best reported result of 4.7% (2). In addition, for 0.005 wt %
Luo et al.
Fig. 3. Hydrodynamic diameter distributions of (A) GO and (B) amphiphilic nanosheets in nanofluids with a concentration of 0.005 wt %. (Insets) Mode sizes. (C)
Selected photographs of amphiphilic nanosheets in the nanofluid in three locations at different time points.

concentration, which to our knowledge has not been previously study the oil displacement mechanisms, and our findings showed
reported, we also achieved extraordinary performance. results quite different from those of the traditional nanofluid.

APPLIED PHYSICAL
In reservoirs, the motion of crude oil can be categorized into As shown in Fig. 4, under static conditions, the interface be-

SCIENCES
three scenarios depending on the local underground hydrodynamic tween heptane and brine was concave in a water-wet glass tube but
power: static, slow, and fast moving. Therefore, we investigated the convex in an oil-wet plastic tube, indicating relatively strong in-
behaviors of nanosheets under simulated hydrodynamic scenarios to terfacial tension. When the nanofluid was injected into the brine,

Fig. 4. Behaviors of nanosheets in oil/brine system with increasing hydrodynamic power. (A–E) Behaviors of nanosheets in oil/brine system with increasing hy-
drodynamic power in a glass tube with water-wet surface (the heptane was dyed with Sudan Red 7B). (A) Heptane/brine mixture. (B) Nanosheets adsorbing to
heptane/brine interface during nanofluid injection under static conditions. (C) Nanosheets at heptane/brine interface after injection; a climbing film appeared on
the wall. (D) Growth of climbing film after gentle shaking. (E) Formation of interfacial film after vigorous shaking. (F–J) Behaviors of nanosheets in oil/brine system
with increasing hydrodynamic power in a plastic tube with oil-wet surface (Sudan Red 7B was not used as the whole plastic tube would be dyed). (F) Heptane/brine
mixture. (G) Nanosheets adsorbing to heptane/brine interface during nanofluid injection under static conditions. (H) Nanosheets at heptane/brine interface after
injection; a climbing film appeared on the wall. (I) Growth of climbing film after gentle shaking. (J) Formation of interfacial film after vigorous shaking.

Luo et al. PNAS | July 12, 2016 | vol. 113 | no. 28 | 7713
Table 1. Oil recovery factor of nanofluid flooding with different concentrations
Average liquid Nanofluid
Rock core Porosity, % permeability, mD concentration, wt %
1 24.8 54.4 0.005
2 26.0 44.5 0.01
3 27.9 130.0 0.005
4 25.8 132.0 0.01
electrostatic repulsion was screened by salt and hydrophobic at-
traction came into play (19). As a result, nanosheets spontane-
ously accumulated at the interface in each case. With increasing
amount of nanosheets adsorbed at the interface, the interfacial
tension was further reduced (20, 21), as indicated by the in-
creasingly flattened interface (Movie S1). As with conventional
nanofluids, however, salt ions in the reservoir fluid were found to
be a permeability damage factor due to increased nanoparticle
aggregation. The climbing film was also observed because locally
raised nanosheet concentrations induced Marangoni stress (the
stress produced by the gradient of interfacial tension) to push the
oil–water interface up the tube surface (22). This film climbed
upward in the case of the water-wet tube surface, which helped
detach the oil phase at solid surface, but downward in the case of
the oil-wet tube surface. For the oil-wet surface, nanosheets may
be captured by the hydrophobic tube surface with the hydrophilic
Fig. 5. Testing the elasticity of interfacial films. (A) Interfacial film responding
to intrusion of a glass rod in a glass tube with a water-wet surface (from left to
right: before intrusion, during intrusion, after intrusion). (B) Interfacial film
responding to intrusion of a glass rod in a plastic tube with an oil-wet surface
(from left to right: before intrusion, during intrusion, after intrusion). (C) The
heptane/brine interface with amphiphilic nanosheets (Left), SDS (Middle), and
TWEEN 20 (Right) responding to intrusion of a glass rod.
7714 | www.pnas.org/cgi/doi/10.1073/pnas.1608135113
Oil recovery factor Enhanced oil recovery
after brine water factor after nanofluid
flooding, % flooding, % Total oil recovery factor, %
71.1 6.7 77.8
62.5 9.5 72.0
68.2 10.2 78.4
69.6 15.2 84.8
side facing the water phase. Such behaviors altered the wettability
of the oil-wet surface.
To simulate the condition of moderate hydrodynamic power,
the tubes were shaken gently after injection. It was observed
that for water-wet glass tubes, the climbing film grew to en-
capsulate the oil phase and may carry the oil forward at flow
conditions, leaving very little residual oil behind. For the oil-
wet plastic tube, the growth of the climbing film was not as ob-
vious as with the glass tube, possibly due to the adsorption of
nanosheets onto the wall of the tube. When subjected to vigorous
shaking, the nanosheets formed flat films at interfaces for both the
glass and plastic tubes. The formation of such a solid-like film was
Fig. 6. Testing the stability of interfacial films. (A and B) Deformation of in-
terfacial films upon tilting. (A) Image of heptane/brine interfaces in tilted glass
tubes with water-wet surfaces. (Upper) Interface with nanosheet interfacial film.
(Lower) Interface without nanosheets. (B) Image of heptane/brine interfaces in
tilted plastic tubes with oil-wet surfaces. (Upper) Interface with nanosheet in-
terfacial film. (Lower) Interface without nanosheets. (C and D) Reformation of
interfacial films after shaking. (C) Image of interfacial film under vigorous
shaking in a glass tube with water-wet surface (from left to right: before
shaking, during shaking, 1 min after shaking). (D) Image of interfacial film
under vigorous shaking in a plastic tube with oil-wet surface (from left to
right: before shaking, right after shaking, 1 min after shaking).
Luo et al.
Fig. 7. Schematic illustration of oil displacement mechanisms. (A) Climbing film encapsulation mechanism for water-wet surface. (B) Slug-like displacement mechanism.
also predicted by computer simulation for near-neutral wetting
spherical particles (23).
When subjected to intrusion of a glass rod, the surface of in-
terfacial films was deformed but not ruptured (Fig. 5 and Movie S2).
After removal of the glass rod, the films recovered to their original
state, clearly demonstrating their elasticity. The presence of nano-
sheets altered not only the normal stress balance, but also the tan-
gential stress balance, leading to a redistribution of nanosheets to
form a flat shape. The elasticity of the interfacial films kept them
intact even at 90 °C. To demonstrate that the elasticity of the inter-
facial film was unique to our amphiphilic nanosheets, we chose so-
dium dodecyl sulfate (SDS) and TWEEN 20 (purchased from
Sigma-Aldrich) as examples of ionic and nonionic surfactants, re-
spectively, for comparison. With the same concentration of 0.01 wt %,
when the interfaces formed by SDS or TWEEN 20 were subjected to
the glass rod intrusion, neither of them exhibited observable elastic
Fig. 8. SEM images of the cross-sections of (A) rock core with high per-
meability and (B) rock core with low permeability before core flooding tests;
and (C) rock core with high permeability and (D) rock core with low per-
meability after core flooding tests. Arrows in each image indicate the
smallest and largest pore openings.
Luo et al.
deformation but simply broke through, very different from the elastic
interfacial film formed by amphiphilic nanosheets (Fig. 5C). In
APPLIED PHYSICAL
terms of interfacial rheology, the interfacial films may resist dilation
and bending as characterized by the nearly flat interface after the
SCIENCES
tubes were tilted to enlarge the area of the interfaces (Fig. 6 A and B).
Vigorous agitation disrupted the films for both solid surfaces (Fig. 6 C
and D). However, the films reformed immediately at the interfaces
and separated the oil and brine phases after shaking. This process may
be driven by the amphiphilicity of nanosheets. In contrast to emulsion
flooding, the interfacial film in our case strictly separates the water
and oil phases, which may push the oil to the outlet like a slug at flow
conditions. This was confirmed in the core flooding tests, where the oil
and brine came out sequentially at the outlet. Such oil displacement
mechanism leaves less oil residue and is free of demulsification, which
is a significant advantage of our nanofluid over the traditional ones.
After careful examination of the existing mechanisms (6–13), we
found none of them was fully applicable to the above experimental
observation under different simulated hydrodynamic conditions.
Therefore, we propose two oil displacement mechanisms for
nanofluid flooding with nanosheets, as illustrated in Fig. 7:
i) The climbing film (a film of nanosheets along the tube’s surface)
encapsulation for water-wet surface. As shown in Fig. 7A, at
t = t0 the increased concentration of nanosheets due to the
adsorption at the oil–water interface produces the concentration
gradient leading to transfer of nanosheets to the three-phase
(nanofluid, oil, and rock solid) region, detaching and encapsu-
lating oil from the rock surface. When flow continues under
gentle hydrodynamic condition from t0 to t0 + Δt, the film grows
due to the ongoing supply of nanosheets from the nanofluid and
carries the oil phase forward.
ii) Slug-like displacement by the interfacial film. As seen in Fig. 7B,
at t = t0 an elastic interfacial film forms at the oil–water interface
at strong hydrodynamic power condition. The film can resist
bending and also reform after being disrupted. As a result, at
t = t0 + Δt oil is slug-like and displaced over a certain distance.
Except for these oil displacement mechanisms, the amphi-
philic Janus nanosheets are expected to have a lower chance to
be captured by the rock surface or to plug the rock pores due to
the self-accumulating at the oil–water interface, which may also
contribute to the high efficiency of oil recovery. The cross-sec-
tions of rock cores were examined by SEM before and after core
flooding and are displayed in Fig. 8. In each figure, the smallest
and largest pore openings are both labeled. As for the rock cores
with high permeability (Fig. 8 A and C), after nanofluid flooding,
the pore sizes at the two ends remained at the same level,
comparable to those before flooding. Similar results were also
detected in rock cores with low permeability (Fig. 8 B and D),
PNAS | July 12, 2016 | vol. 113 | no. 28 | 7715
with survival of narrow pore openings of around 2 μm. The
observation that there were no noticeable changes in the pore
opening sizes indicated that our nanofluid caused minimal
damage to the permeability of the rock pores.
In addition, fresh water was used to prepare the nanofluid for the
tests described above. However, brine is preferred in some opera-
tions (e.g., seawater in offshore reservoirs or when fresh water is
scarce) to reduce cost and conserve fresh-water resources. This
requires that nanosheets be stable in a saline environment for a
certain time before reaching underground reservoirs. Our study
showed that sequential addition of polyvinylpyrrolidone and poly-
vinyl alcohol provided good stability to our nanofluid in brine. We
are currently investigating the stabilization mechanism, the oil re-
covery efficiency in core flooding tests, and oil displacement
mechanisms due to the existing polymer.
Conclusion
We have presented the first (to our knowledge) tertiary or en-
hanced oil recovery experiments using simple nanofluid flooding
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