i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 9 2 7 9 e9 2 8 4

Available online at www.sciencedirect.com

ScienceDirect

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

Short Communication

Hydrogen production and carbon sequestration by

steam methane reforming and fracking with
carbon dioxide

John W. Andrews 1
Brookhaven National Laboratory, Upton, NY, 11973, United States

highlights graphical abstract

Hydraulic fracturing (fracking) has

transformed the U.S. oil and gas
industry.

Fracking with carbon dioxide
instead of water allows carbon to
be sequestered.

Extracting the carbon dioxide from
natural gas produces hydrogen
end product.

Could lead to carbon savings equal
to 60 nuclear plants or 1 billion
solar panels.

article info abstract

Article history: An opportunity to sequester large amounts of carbon dioxide (CO2) is made possible
Received 4 December 2019 because hydraulic fracturing is used to produce most of America’s natural gas. CO2 could
Received in revised form be extracted from natural gas and water using steam methane reforming, pressurized to its
7 January 2020 supercritical phase, and used instead of water to fracture additional hydrocarbon-bearing
Accepted 29 January 2020 rock. The useful energy carrier that remains is hydrogen, with carbon returned to the
Available online 22 February 2020 ground. Research on the use of supercritical CO2 is reviewed, with proppant entrainment
identified as the major area where technical advances may be needed. The large potential
Keywords: for greenhouse-gas reduction through sequestration of CO2 and avoidance of methane
Carbon sequestratration leakage from the natural gas system is quantified.
Carbon capture © 2020 The Author(s). Published by Elsevier Ltd on behalf of Hydrogen Energy Publications
Hydraulic fracturing LLC. This is an open access article under the CC BY-NC-ND license (http://
Climate change creativecommons.org/licenses/by-nc-nd/4.0/).
Steam methane reforming

E-mail address: candrews40@optonline.net.

1
Retired.
https://doi.org/10.1016/j.ijhydene.2020.01.231
0360-3199/© 2020 The Author(s). Published by Elsevier Ltd on behalf of Hydrogen Energy Publications LLC. This is an open access article under the CC BY-NC-
ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
9280 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 9 2 7 9 e9 2 8 4
Introduction
Many researchers have predicted that the capture and storage
of carbon in long-lived reservoirs will be needed to mitigate
climate change. Any viable scheme for sequestering carbon
must, however, address two major difficulties. The first is how
to collect the carbon, whether from fossil fuels pre- or post-
combustion or directly from the air or the oceans. The sec-
ond is where to put it. These hurdles are both technical and
economic. A scheme may be practicable in a technical sense,
but so expensive that no foreseeable economic scenario would
include it as a major player.
This article evaluates a method of carbon capture and
storage (CCS) that seeks to overcome these difficulties by
extracting hydrogen from natural gas and water using a steam
methane reformer (SMR) followed by the use of byproduct CO2
in a supercritical state (sCO2) as a substitute for water to
fracture additional methane-bearing rock in a continuing
cycle.
The role of hydrogen in a low-carbon economy has
attracted much interest, with particular attention to how the
hydrogen can be produced carbon-free. At a recent sympo-
sium on hydrogen energy at the Massachusetts Institute of
Technology [1], the options were stated succinctly: “Hydrogen
can be clean if produced by electrolysis using renewable en-
ergy or nuclear power, steam methane reforming with carbon
capture and storage, or if it is based on renewable biomass.”
A stumbling block for CCS has been the dilemma that in
schemes where the CO2 has economic value the potential
impact on global warming is generally not very significant,
whereas when the potential is great, the CO2 tends to be a
burdensome waste product. The ability to extract CO2 from
natural gas and waterdwith hydrogen as the energy car-
rierdprovides a special opportunity in that here the CO2 will
be both plentiful and useful.
Other approaches to sequestering carbon from a source of
methane have been proposed. Among these alternative
sources is methane hydrates. Wang et al. [2] reported on ex-
periments in which a CO2-rich mixture of CO2 and hydrogen
was injected into a laboratory vessel containing a hydrate
under conditions similar to those encountered in natural
reservoirs. The group later reported on experiments with
continuous injection [3] and continuous injection interrupted
by pauses [4]. They have done additional work [5] to address
problems of water intrusion and gas leakage in underwater
hydrate reservoirs. Key to their scheme is the use of SMR to
extract and separate free hydrogen from the CH4-rich mixture
of gases produced from the hydrate, leaving a CO2-rich
mixture to be re-injected. Their work is similar to the present
proposal in that SMR is used to produce hydrogen while
sequestering CO2, but different in that here the source of CH4
is not hydrates but instead tight formations of methane-
bearing rock requiring fracking for recovery.
A previous study [6] analyzed a process design that shares
some of the characteristics of the present proposal. Their
system included Fischer-Tropsch synthesis of transportation
fuels with co-feed of biomass to reduce life-cycle carbon
emissions to zero. Although their scheme involved injection
of CO2 into the ground, they did not envision is use as a
fracking medium. Their scheme shares the critical features of
the simpler concept presented herednamely the use of
reforming and combined-cycle power generationdbut with
additional features and more detail.
Another approach to CCS from methane is methane py-
rolysis. This has been analyzed [7,8] and found to be a
potentially viable option. The product is elemental carbon,
which can be used in various forms, chiefly carbon black. This
product would not, of course, be useful for fracking.
System configuration
The overall plan of the scheme is straightforward. In a
natural-gas field in which hydraulic fracturing (fracking)
would conventionally be done using water, natural gas from a
number of wells is gathered to a central location in which the
SMR is located. The SMR produces hydrogen and CO2. The
reaction is moderately endothermic, which means that heat
must be supplied to make it go, but this is counterbalanced by
the fact that the heating value of the hydrogen produced is
greater than that of the input methane.
In a hydrogen-output system configuration (Fig. 1), the
hydrogen produced by the SMR is piped to the regions where
the energy is needed. In an alternative electric-output
configuration (Fig. 2), the hydrogen is used immediately to
produce electric power in a high-efficiency combined-cycle
power plant (CCPP) and fed into the grid.
In either case the CO2 produced by the SMR would then be
compressed enough to enter a supercritical phase. The critical
pressure of CO2 is 1071 psia (7.39 MPa), so the operating
pressure at this point would need to be somewhat greater
than this. This sCO2 would then be piped to well locations in
the general vicinity of the SMR. These could be the same wells
from which the natural gas just converted to CO2 was pro-
duced (as a well may be fracked more than once), or it could be
piped to new wells as the original ones became depleted. The
relatively small-diameter sCO2 pipes could share the same
pathways as the gathering pipes used to transport natural gas
in the opposite direction. At the well sites, proppant would be
added, and its pressure would be boosted to whatever was
needed to frack that particular well. When water is used, sand
is commonly used as the proppant. With sCO2, its lower vis-
cosity will require the development of additives and/or alter-
native proppants that the sCO2 can successfully entrain.
Each of the two configurations has certain advantages
relative to the other. In the hydrogen-output system, the
hydrogen remains available for use in a variety of ways and
could be piped over long distances. The advantage of the
electric-output system is that the water which is the product
of combustion in the CCPP can be recycled into the SMR,
which otherwise would need local water as feedstock in
addition to the natural gas.
Using CO2 extracted from natural gas for fracking more
natural gas is particularly attractive because the source of the
CO2 is of necessity located near the site in which it would be
used, namely a hydrocarbon-bearing shale formation in
which fracking is productive. The need to transport CO2 over
long distances has been a stumbling block for other CCS
proposals.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 9 2 7 9 e9 2 8 4
Fig. 1 e Hydrogen output system configuration.
Fig. 2 e Electric-output system configuration.
Global warming potential reduction
The potential amount of sCO2 that could be used for fracking
may be estimated from the amount of water currently used for
this purpose. Currently, about 20,000 shale gas wells are being
drilled and completed annually [9]. A listing of water usage
values for a typical well in major shale plays ranged from 1.5
million to 15.8 million U.S. gallons (6  106 to 60  106 L) [10]. By
far the largest production comes from the Marcellus Shale,
with a typical water usage of 4.5 million gallons (17  106 L) per
well. Using this as a benchmark for 20,000 wells results in an
estimate of 90 billion gallons (340  109 L) of water nationwide.
The density of sCO2 is approximately equal to that of water.
Assuming that the same mass and volume of sCO2 would be
needed as is now needed with water, this would result in a
usage of 340 million tonnes of sCO2 annually. The amount of
CO2 sequestered using the above estimate would be equiva-
lent to the carbon avoided by 60 nuclear power plants, 30,000
large utility-scale wind turbines, or 1,000,000,000 solar panels
[11].
The energy required for this sequestration needs to be
considered. This includes the less-than-100% efficiency of an
optimized SMR, the energy needed to separate the CO2 from
the hydrogen, and the energy needed to compress the CO2 to
sCO2. If these factors (estimated below) are simply combined
and charged against the above estimate, it would be reduced
by about 20%. If the necessary incentives were in place, this
9281
could be made up by drilling more wells or by using a
renewable energy source.
Of course, much of the sCO2 that is used would be pro-
duced along with the natural gas, so to sequester it the CO2
would need to be re-injected prior to well abandonment. On
the other hand, it is possible that more CO2 could be seques-
tered than is needed for fracking. In any case, there would
need to be an incentive for this sequestration. This could be
achieved through a carbon tax with forgiveness for seques-
tered carbon or by regulation requiring sequestration as a
condition for fracking.
A detailed comparison of the potential for carbon seques-
tration of the approaches discussed in the introduction is
beyond the scope of this paper. One datum is that Ref. 8 es-
timates the total worldwide market for carbon, such as would
be produced by pyrolysis of methane, to be about 18 million
tonnes in the early 2020’s. The CO2-equivalent would be 67
million tonnes, or about one-fifth of the potential in the U.S.
alone for the application proposed here.
Also important is the reduction in methane and CO2
leakage from the natural gas system that would occur with the
proposed scheme. The latest U.S. government estimate [12] is
that the global warming potential of this leakage is 13% of the
global warming potential of the CO2 that results from com-
bustion of the natural gas itself. A study done for the Envi-
ronmental Defense Fund by researchers at Colorado State
University [13] found that leakage of methane is 60% higher
9282 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 9 2 7 9 e9 2 8 4
than that estimate. In addition, some analysts argue for a 20-
year time horizon for methane-induced warming, which
would increase the CO2-equivalent reduction from reduced
methane leakage by a factor of about 2.5. Although not all of
this leakage would be avoided by the immediate conversion of
natural gas to hydrogen, as the natural gas must still be pro-
duced and piped to the SMR, the possible reduction in leakage
is not to be ignored.
Extraction of carbon dioxide from methane
Steam methane reforming is an established technology
currently used to produce hydrogen for industrial applica-
tions. The overall chemical formula for the SMR process
(including both the initial step that produces carbon monox-
ide and the water-gas shift reaction that converts this to car-
bon dioxide) is
CH4 þ 2H2O / 4H2 þ CO2
The inputs are methane (CH4) and water (as steam). The
products are hydrogen and CO2. As the CO2 is re-injected into
the earth, the only product that remains is hydrogen. Typi-
cally, natural gas is about 94% methane, with most of the rest
being ethane (C2H6), which also reforms to CO2 and hydrogen
in a manner similar to methane.
The efficiency of SMR units currently being used to produce
commercial hydrogen ranges from 65% to 75% [14]. These are,
however, not optimized for maximum efficiency but for
lowest cost. Hydrogen produced at the scale envisioned here
and used as an energy carrier would require re-optimization
at higher efficiency. A benchmark value for achievable effi-
ciency was based on two papers [15,16]. These indicate that an
efficiency of 86%e87% can be achieved under conditions of
zero export steam, which is what this application would
entail. It should be noted that these papers quote practical
efficiency with realistic heat exchangers, and not some theo-
retical efficiency that could never be attained in the real world.
In the SMR process, the H2 and CO2 are typically separated
by pressure-swing adsorption (PSA), a process in which the
mixed gases are exposed at high pressure to an adsorbent
such as activated carbon or zeolite, which adsorbs the CO2 but
not the H2. Another possible approach envisions the use of
inorganic membranes that are permeable to H2 but imper-
meable to CO2 [17]. The potential for this approach to supplant
PSA remains to be seen.
A question may arise concerning the energy required by
PSA. This is sometimes simply described as “low.” [18] A
quantitative study [19] indicated that the exergetic efficiency
of PSA would be between 98% and 99%. Research to improve
the purity and yield of PSA-produced hydrogen is ongoing, e.g.
as in Ref. [20].
Technical applicability of supercritical CO2
Research on sCO2 fracking in the United States and China has
identified several potential advantages for it relative to the use
of water. These were nicely summarized by Wan [21]:

It eliminates several drawbacks of water caused by its
immiscibility with gas and oil and its tendency to cause
clay hydration and swelling in the fracked reservoir.

CO2’s miscibility with natural gas and oil enhances their
mobilization.

The compressibility of sCO2 during fracturing is expected
to generate more complex and finer fractures.

Strong adsorption of CO2 relative to methane drives
desorption of the latter, thereby enhancing natural gas
production.

It provides a mechanism for sequestration and storage of
carbon in subsurface formations.
Several researchers [22e25] have reported on laboratory
experiments in which rock samples were subjected to frac-
turing conditions using sCO2 with generally encouraging re-
sults. The most significant challenge has been the low
viscosity of sCO2, which makes it a poor carrier of sand as a
proppant. This is a central concern of a US-China joint project
(1) on CO2-based fracturing techniques [21]. This author noted
that some of the more promising efforts used proprietary
additives whose nature was not disclosed. She mentions a
recent discovery by her group of a “promising natural biogenic
surfactant … contained in the earth’s subsurface sediments
that is inexpensive and abundant.”
Most recently, a Chinese project [26] has shown experi-
mentally that fracking with CO2 should not only be practicable
but advantageous. The study highlighted the following
findings:

CO2 fracturing is more effective in reservoir stimulation
than water.

The multiscale mechanism of CO2 fracturing was experi-
mentally established.

A 4- to 20-fold increase in tight oil production was achieved
by CO2 fracturing.
A key question here concerns the energy needed to
compress the CO2 emerging from the SMR to the supercritical
state needed for fracking. A calculation [27] of the electrical
energy needed to compress CO2 from 250 psia (1.72 MPa) to
2215 psia (15.3 MPa) in a carbon-capture application gave an
electric energy requirement of 0.0504 kWh/kg CO2. (A theo-
retical lower limit estimated by the present author, assuming
adiabatic compression in three stages with intercooling but no
credit for any heat recovery, yielded 0.035 kWh/kg CO2.)
Assuming that the electricity is generated at 50% efficiency, as
by the CCPP described above, and taking account of the fact
that the mass of CO2 generated is 2.75 times the mass of the
input CH4, the realistic energy as calculated in Ref. 27 would
require 2% of the heat of combustion (LHV) of the methane.
To summarize, the literature suggests that the advantages
of sCO2 over water as a fracking fluid justify efforts to solve the
remaining challenges, particularly in the area of proppant
transport, even in the current economic environment. If and
when a fee on carbon emissions is enacted that includes a
rebate for carbon that is sequestered, it is reasonable to expect
that efforts by the industry to bring CO2 fracking into the
mainstream of practice will be redoubled, with a high proba-
bility of success.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 5 ( 2 0 2 0 ) 9 2 7 9 e9 2 8 4
Getting the energy where it’s needed
Most fracked natural gas in the United States is currently
produced in the Plains states and in the Appalachian region. If
hydrogen extracted is used immediately to generate electric
power, as in Fig. 2, then keeping transmission losses within
reasonable bounds using current transmission technology
would require that the point of use be within about 300 miles
(500 km) of the point of production.
The hydrogen-output system shown in Fig. 1 avoids the
electric transmission problem, though it would require
dedicated hydrogen pipelines from the regions where the
hydrogen is produced to the areas where the energy is
needed. Once that infrastructure is in place, however, it
could provide, in tandem with the electric grid, an impor-
tant degree of robustness and flexibility in energy dispatch.
Another potential advantage of this approach is that a
hydrogen pipeline would be a conduit not only for energy
but in effect, also, for water, which could be recovered as
the end product of hydrogen combustion. This would add to
the attractiveness of this option if the energy is used in an
area where water is scarce, such as the American
Southwest.
Environment and safety
Meng et al. [25] cite safety benefits from using sCO2 in that
fracturing can be achieved at lower pressures than are
required with water, stating that it “alleviates the environ-
mental problems associated with traditional fracturing
methods.” Wang et al. [28] state that sCO2 is “an environ-
mentally friendly working fluid with no risk of pollution to
reservoirs, groundwater, or surface environment.” Some
environmentalists also see advantages in fracking with
sCO2. One group states [29] “We are still a great way from
widely using the waterless CO2 fracking but even fracking
opponents are optimistic and see the environmental bene-
fits of using supercritical carbon dioxide for fracking
instead of water.”
Implementation
In order for this technology to be widely adopted, it will be
necessary to provide incentives and remove barriers.
Although it will be up to the industry to figure out the best
ways to put this approach to carbon sequestration into
practice, government could play any or all of the following
roles:

Impose a fee on carbon emissions from fossil fuels but
rebate the fee for carbon returned to the ground.

Regulate fracking to encourage the use of carbon dioxide
while limiting the use of water.

Provide research support for CO2 fracking while protecting
underground aquifers, and for SMR optimization in this
and similar applications.
9283
Conclusion
It appears that the use of SMR on natural gas and water to
produce hydrogen and CO2dwith the CO2 then used to frack
additional natural gas wells and sequestering the carbon
undergrounddshould be technically feasible with foreseeable
developments in certain areas such as proppant entrainment.
Supporting infrastructure would need to be established in
order to achieve the projected market penetration. Imple-
mentation will, however, require a favorable political-
economic environment.
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