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OPEN
Innovative method for CO2 fixation
and storage
Kenji Sorimachi
The concentration of CO2 in Earth’s atmosphere has been gradually increasing since the Industrial
Revolution, primarily as a result of the use of fossil fuels as energy sources. Although coal and oil
have been vital to the development of modern civilization, it is now recognized that atmospheric CO2
levels must be reduced to avoid the serious effects of climate change, including natural disasters.
Consequently, there is currently significant interest in developing suitable methods for the fixation of
CO2 in the air and in exhaust gases. The present work demonstrates a simple yet innovative approach
to the chemical fixation of extremely low and very high CO2 concentrations in air, such as might result
from industrial sources. This process is based on the use of aqueous solutions of the water-soluble
compounds NaOH and CaCl2, which react with CO2 to produce the harmless solids CaCO3 (limestone)
and NaCl (salt) via intermediates such as NaHCO3 and Na2CO3. The NaCl generated in this process
can be converted back to NaOH via electrolysis, during which H2 (which can be used as a clean energy
source) and Cl2 are produced simultaneously. Additionally, sea water contains both NaCl and CaCl2 and
so could provide a ready supply of these two compounds. This system provides a safe, inexpensive
approach to simultaneous CO2 fixation and storage.
Although Earth has undergone many periods of significant environmental change over time, the planet’s environment has been unusually stable for the past 10,000 years1. During this time, various natural systems regulated
the Earth’s climate and maintained the conditions that enabled human development. However, these regulatory
systems have been greatly disturbed, and the planet may be nearing a threshold beyond which unpredictable
environmental changes may occur, such as increases in the mean global t emperature2. To reduce atmospheric
CO2 concentrations as a means of mitigating such effects, the so-called Paris Agreement was reached at the
United Nations Climate Change Conference (COP20) in 2015. This agreement was based on the requirement to
keep the increase in the mean global temperature below 2 °C relative to the temperature prior to the Industrial
Revolution, and preferably less than 1.5 °C. At present, this goal is challenging based solely on the development
of carbon-neutral energy systems. Even so, President Elect Joe Biden has stated that the United States of America
will rejoin the Paris Agreement (rejoined historically today, January 20, 2021) and the current Prime Minister of
Japan, Yoshihide Suga, has declared that Japan will achieve a carbon-neutral society by 2050. Additionally, the
President of the People’s Republic of China, Xi Jinping, has declared that China will be carbon neutral by 2060.
Even so, because the present atmospheric C
O2 concentration is quite high, there are ongoing efforts to reduce
the accumulated C
O2 so as to prevent a climate change crisis. Climatologists have warned that a significant
reduction in the level of CO2 in Earth’s atmosphere is required over the next decade2; therefore, it is necessary
to immediately begin this process. The urgency of this work has been communicated by climate change activists
such as Greta Thunberg, and “Fridays for Future” events have been held worldwide.
Although renewable energy sources, including solar radiation and wind, can result in reduced CO2 emissions,
these alternative systems still require energy expenditure and may also involve CO2 production. Additionally,
these renewable energy approaches do not remove CO2 that has already accumulated in the atmosphere, nor do
they address the ongoing generation of C
O2 from exhaust gases and industrial sources. Thus, even if a carbonneutral society could be immediately achieved, the accumulated atmospheric C
O2 would not be reduced. For
these reasons, it is important to lower the C
O2 level currently in Earth’s atmosphere and to develop practical
means of doing so as soon as possible. For CO2 storage, geo-sequestration by injecting CO2 into underground
geological formations, such as oil fields, gas fields, and saline formations, has been s uggested3,4, although these
systems are still projects for the future.
Plants consume large quantities of C
O2 based on photosynthesis, in which C
O2 and H2O are converted to
carbohydrates using chlorophyll under sunlight. However, the planet’s largest forest, the Amazon, which greatly
contributes to the removal of atmospheric CO2, is continually shrinking because of commercial development
1
Research Laboratory, Gunma Agriculture and Forest Development, Takasaki, Gunma 370‑0854,
Japan. 2Present address: Bioscience Laboratory, Environmental Engineering, Co., Ltd., 1‑4‑6 Higashi‑Kaizawa,
Takasaki, Gunma 370‑0041, Japan. email: [email protected]
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Figure 1. Photograph of CaCO3 precipitates. (a) A solution containing 0.05 N NaOH and 0.05 M C
aCl2. (b) A
solution treated with CO2 bubbles for 30 s at a flow rate of 2 cm3/s.
and serious fires. C
O2 also dissolves in the oceans to form H
2CO3, HCO3− and CO32−, and there is approximately
50 times as much carbon dissolved in the oceans as exists in the atmosphere5. Conversely, all living organisms
produce CO2 during respiration, such that the rates of C
O2 consumption and production were balanced before
human activities produced huge amounts of CO2. Certain CO2 derivatives are used industrially6 and in medicine7.
The synthesis of methanol from C
O2 is particularly important because methanol is a primary raw material for
the production of numerous other chemicals8. For example, our own group recently found that NaHCO3 and
Na2CO3 accelerate glucose consumption in cultured cells9,10. These materials improve serum glucose levels in
diabetes mellitus p
atients11. However, the rate of usage of C
O2 compounds in such applications is obviously much
smaller than the rate of CO2 production.
CaCO3 can be used as a component of concrete, and C
O2 can also be reacted to generate important compounds such as methanol on an industrial s cale8, although the C
O2 must first be captured and concentrated or
fixed in some manner. CaCO3 is also readily converted to CO2 by reaction with HCl and other acids. Additionally, it should be noted that large amounts of CaCO3 are produced naturally as coral or in the form of limestone.
CO2 can be captured from the ambient air or from flue gas via several techniques, including a bsorption12,
adsorption13–18 and membrane gas separation14,19. Absorption with amines is currently the dominant technology,
while membrane and adsorption processes are still in the developmental stages with the construction of primary
pilot plants anticipated in the near future. Recently, it was reported that an amine compound, spiroaziridine
oxindole, fixed efficiently C
O2 under near ambient conditions and released C
O2 under mild c onditions17. However, to the best of our knowledge, these methods alone cannot achieve the necessary worldwide reductions in
atmospheric CO2.
Results and discussion
CaCO3 precipitation. It is known that CO2 is absorbed by alkaline solution16. In the present work, CO2
was bubbled through an initially clear solution (Fig. 1a) containing 0.05 N NaOH and 0.05 M CaCl2 to form an
immediate white precipitate (Fig. 1b).
2NaOH + CaCl2 + CO2 → CaCO3 + H2 O + 2NaCl
In other trials, varying the NaOH concentration between 0 and 0.5 N in the presence of 0.05 M C
aCl2 was
found to generate a white precipitate above 0.2 N NaOH even in the absence of CO2. Because this precipitate
resulted from the formation of Ca(OH)2, the
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a
0.12
Precipitate weight (g/tube)
0.1
0.08
0.06
0.04
0.02
0
0N
0.005 N
0.01 N
0.05 N
0.1 N
0.2 N
b
0.1
Precipitate weight (g/tube)
-0.02
0.08
0.06
0.04
0.02
0
0.005 M 0.01 M 0.05 M 0.1 M
0.2 M
0.3 M
0.4 M
0.5 M
Figure 2. CaCO3 precipitates. (a) Quantities obtained from 3 mL of 0–0.4 N NaOH mixed with 3 mL of 0.1 M
aCl2 in a plastic tube followed by exposure to CO2 bubbles for 10 s at a CO2 flow rate of 2 c m3/s. (b) Quantities
C
obtained from 3 mL of 0–1.0 M CaCl2 mixed with 3 mL of 0.1 N NaOH followed by centrifugation at 3000 rpm
for 10 min (LCX-100, TOMY, Tokyo, Japan). Note that the final CaCl2 concentration was 0.5 M although the
initial concentration was 1.0 M. The tube mass was determined before and after C
O2 precipitation using an
ME 204 instrument (METTLER TOLEDO). The vertical axis represents the mass of the wet precipitate and the
plotted values are the mean plus or minus one standard deviation based on five replicates.
2NaOH + CaCl2 → Ca(OH)2 + 2NaCl
potential for C
O2 incorporation in the form of C
aCO3 was minimal under these conditions. Conversely, solutions
with lower NaOH concentrations (from 0.05 to 0.1 N NaOH) together with 0.05 M C
aCl2 remained clear, while
the addition of CO2 bubbles produced a white precipitate (Fig. 2a). Under these conditions, CaCO3 precipitation
occurred in the presence of CaCl2, which means that high NaOH concentrations were reduced by the formation
of a Ca(OH)2 precipitate. However, prolonged bubbling with C
O2 decomposed the C
aCO3 precipitates to form
Ca(HCO3)2, which is water soluble. As the concentration of C
aCl2 was changed from 0 to 0.5 M, the amount of
white precipitate was found to plateau at 0.05 M CaCl2 (Fig. 2b).
One step CO2 fixation.
The CO2 concentration in a 2-L bottle made of poly(ethylene terephthalate) (PET)
was monitored to determine whether a solution containing 0.05 N NaOH and 0.05 M CaCl2 reduced the level of
CO2. These trials showed that the CO2 reduction was clearly correlated with the time span over which the solution remained in the bottle and in contact with the internal atmosphere (Fig. 3a). Approximately 60% and 80% of
the initial CO2 was removed after 15- and 60-min treatments, respectively. After allowing the plastic bottle to sit
overnight, the CO2 in the bottle was completely removed. Thus, chemical fixation of CO2 emission, regardless of
volume/concentration of CO2 could be efficiently captured and fixed by a solution containing 0.05 N NaOH and
0.05 M CaCl2. Laying the plastic bottle on its side increased the surface area of the solution and thus increased
the CO2 removal rate (Fig. 3b).
At a high CO2 concentration of approximately 15%, the addition of 50 mL of a solution containing 0.05 N
NaOH and 0.05 M CaCl2 followed by vigorous shaking of the 2-L bottle for 30 s by hand reduced the CO2 concentration to 10% (Fig. 3c). A further slight reduction of the C
O2 concentration was obtained by subsequently
allowing the bottle to stand. The addition of 50 mL of a fresh solution also resulted in an additional slight reduction and a further addition of fresh solution after 24 h again reduced the CO2 concentration (Fig. 3c). This slow
reduction of the C
O2 level after the initial rapid removal is attributed to the presence of insufficient quantities of
NaOH and C
aCl2. The pH of the solution after 24 h and following the third addition was 6.5, while that of the
initial fresh solution was 12.19. These results indicate that the NaOH in the solution was completely consumed.
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CO2 concentraon (ppm)
a 800
600
400
200
0
0 min
15 min
30 min
60 min
Over night
-200
CO2 concentraon (ppm)
b 800
700
600
500
400
300
200
100
0
0 me
Stand
Shaken
CO2 concentraon (%)
c 20
15
10
5
0
Figure 3. CO2 concentration changes in a bottle. (a) After the transfer of 10 mL of a solution containing
0.05 N NaOH and 0.05 M CaCl2 into a 2-L plastic PET bottle with a tight cap followed by standing for 15, 30
or 60 min. (b) After the transfer of 10 mL of this solution into a 1.4-L octagonal plastic bottle with a tight cap
followed by standing or shaking for 5 min. (c) After the transfer of 50 mL of this solution into a 2-L plastic PET
bottle with 15% CO2, followed by vigorous shaking for 30 s, then standing for various time spans. After 60 min,
50 mL of fresh solution was added with shaking for 30 s followed by standing for 24 h and shaking for 30 s. C
O2
concentration in the gas phase was analyzed. All values are the means plus or minus one standard deviation
based on four or five replicates.
Two steps CO2 fixation. In the above trials, a solution containing low concentrations of NaOH and C
aCl2
was used in a one step process. When using high NaOH concentrations (above 0.2 N), the CO2 should first
be treated solely with NaOH to prevent the formation of Ca(OH)2. This produces a solution of N
aHCO3 and
Na2CO3 to which C
aCl2 can be added after reducing the NaOH concentration to less than 0.1 N. The latter
method is based on two steps and allows the use of high concentrations of NaOH and C
aCl2.
Fog formation by absorbents. Because increasing the surface area of the highly concentrated NaOH
solution is also important to ensuring efficient absorption of C
O2, the generation of a fog can be beneficial. The
formation of a fog greatly increases the liquid surface area and results in more rapid CO2 removal in the plastic
bottle (Fig. 4a). In experiments using a chimney model, when the chimney contained high CO2 concentrations,
the amounts of NaOH and CaCl2 in the solution were insufficient to react with all the C
O2 at a gas flow rate of
approximately 110 cm3/s (Fig. 4b). Thus, the solution could only capture a relatively small amount of the CO2 in
the chimney model.
Bubbling of CO2 gas. The area over which the reagent solution interacted with CO2 could also be increased
by first passing the test gases through a porous stone to form bubbles. In these trials, a poly(vinyl chloride) pipe
(40 mm in diameter and 50 cm in height) was partially filled with 250 mL each of aqueous solutions containing
0.1 N NaOH and 0.1 M CaCl2. Following this, the test gas was bubbled upwards through the solution at a flow
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a
900
CO2 concentraon (ppm)
800
700
600
500
400
300
200
100
0
0 me
Sprayed
b 10
9
CO2 concentraon (%)
8
7
6
5
4
3
2
1
0
0 me
Sprayed
Figure 4. CO2 concentration changes obtained using a spray. A solution containing 0.05 N NaOH and 0.05 M
aCl2 was sprayed 10 times at 5-s intervals to provide a total volume of approximately 4 mL. (a) The solution
C
was sprayed into a 2-L plastic PET bottle and (b) into a chimney model made from two milk boxes. In the latter
case, the air and CO2 flow rates were 100 and 10 c m3/s, respectively. All values are the means plus or minus one
standard deviation based on either six or ten replicates.
rate of approximately 20 mL/s after passing through the porous stone at the bottom of the pipe. Under these conditions, the C
O2 contained in the air was completely absorbed by the solution (Fig. 5a). In trials using this same
apparatus with a very high C
O2 concentration, the level was reduced from an initial value of 10–2.5% (Fig. 5b).
These data indicate that this concept could be employed to reduce high C
O2 levels in the exhaust streams from
industrial operations such as thermal power plants and incinerators.
Diagram showing the proposed CO2 fixation process. One means of producing NaOH on an indus-
trial scale is the electrolysis of an aqueous NaCl solution. The products of this newly developed C
O2 fixation system based on NaOH and C
aCl2 are CaCO3 and NaCl, and this NaCl could therefore be subsequently converted
to NaOH, H2 and Cl2 via an electrolytic process. Thus, CO2 could be captured using this system while simultaneously producing H
2 and C
l2 (Fig. 6). Additionally, this process could potentially be integrated with existing
generator systems based on atomic, thermal, solar, wind, hydro or wave power, and natural seawater could be
used instead of an artificial NaCl solution in the electrolysis process.
Conversely, the system presented in Fig. 6 is based on both C
O2 fixation and NaCl electrolysis. Because the
efficient absorption of C
O2 with NaOH micro-droplets requires a large volume, while the electrolysis of a NaCl
solution does not, a new CO2 capture plant design was developed, as shown In Fig. 7. This plant is intended
to continually capture C
O2 from the atmosphere or from exhaust gases. Using a large chamber equipped with
spray nozzles, C
O2 can be captured efficiently by droplets of the NaOH solution. As indicated in the figure, this
chamber could have various geometries. The cylindrical and meandering shapes would be applicable to either
reclining or standing structures, while the other morphologies would be suitable only for a standing structure.
This system could also be combined with the NaOH generating process described in the preceding section.
Recently, plastic waste has been shown to be a significant environmental pollutant, and micro-plastics have
been found to affect marine o
rganisms20. A small portion of the plastics that are used daily in human activities
are recycled, while the remainder is simply treated as waste. Many of these materials could be incinerated but
instead are typically sent to landfills. However, if a simple method of fixing C
O2 becomes available, this waste
could be readily disposed of by burning without any environmental concerns and with the potential to generate
energy. In addition, the current COVID-19 pandemic has resulted in vast quantities of waste materials potentially contaminated with the virus. It would be helpful to be able to burn contaminated plastic-based medical
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CO2 concentraon (ppm)
a 1000
900
800
700
600
500
400
300
200
100
0
Air
Inner pipe
CO2 concentraon (%)
b 12
10
8
6
4
2
0
10% CO2
Inner pipe
Figure 5. CO2 concentrations above the solution in the pipe apparatus when bubbling (a) air and (b) 10% C
O2
in air through the solution. All values are the means plus or minus one standard deviation based on either nine
(a) or three (b) replicates.
waste as a means of limiting the spread of infection. At present, chemical absorption using organic amines is
typically employed to capture C
O2 emitted from thermal power plants, but liberating C
O2 from these complexes
requires heat treatment that induces degradation. Because this treatment itself produces CO2, a new method that
fixes CO2 would be highly beneficial. The present method employing inorganic compounds generates a stable
product, based on the neutralization of NaOH along with the formation of CaCO3 and NaCl, both of which are
harmless, stable natural compounds.
This technique is applicable to thermal power plants, chemical plants, large ships, combustion operations,
incinerators and automobiles. Under strict regulations for air pollution, exhaust of oxide of nitrogen ( NOx) and
sulfur dioxide ( SO2) which have great influence on environment and human health from coal combustion21,22
have been strongly prohibited by law. Contrary, there is no CO2 emission control, and this resulted in accumulation of atmospheric CO2 since the Industrial Revolution. Using this process, atmospheric CO2 can be spontaneously fixed based on a simple apparatus at various locations to generate CaCO3. This newly developed and
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Figure 6. The figure shows proposed CO2 fixation process combined with the electrolysis of NaCl. 1: Carbon
dioxide fixation apparatus, 10: reaction vessel, 11: reaction chamber, 12A: anode chamber, 12B: cathode
chamber, 13A and 13B: partition wall, 20A and 20B: carbon dioxide fixing agent feeding units, 30: gas feeding
unit, 31: insertion end point, 40A: Cl2 extraction portion, 40B: H2 extraction portion, 40C: air extraction
portion, 50: liquid extraction portion, 51: filter, 121A: anode, and 121B: cathode. The original diagram was
drawn by the author, and it was formally traced by Tsujimaru International Patent Office.
facile system, which does not require organic chemicals, has minimal environmental impact and is completely
sustainable, and so is expected to provide a means of reducing atmospheric C
O2 levels so as to mitigate climate
change. At present, there is worldwide recognition that climate change has become a crisis2. Because humans
“who are the most evolved organisms”23,24 are responsible for this crisis, we have a moral duty to address the
situation through global cooperation.
Methods
Chemicals. Reagent grade NaOH and CaCl2 were purchased from Wako-Junyaku Kogyo (Tokyo, Japan).
Milli-Q water was used throughout the experiments.
CO2 fixation. The reaction solution containing 0.05 N NaOH and 0.05 M C
aCl2 was prepared in a commercial 2-L plastic PET bottle or a commercially available 1.4-L octagonal plastic bottle and the bottles were allowed
to stand or were shaken for the stated periods.
In the fog trials, approximately 4 mL of the solution was sprayed into a 2-L plastic PET bottle, after which
the CO2 concentration (in ppm) was measured using an RI-85 instrument (RIKEN). The chimney model was
prepared by combining two 1-L paper milk boxes, after which air (at approximately 100 cm3/s) and CO2 (approximately 10 cm3/s) were supplied into the lower box. A layer of gauze was placed between the two boxes and
approximately 4 mL of the solution was sprayed into the middle part of the lower box. The CO2 concentration (in
%) was subsequently determined at the central point of the upper box using an XP-3140 instrument (COSMOS).
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Figure 7. The figure shows proposed CO2 fixation process. The spray chamber could potentially have several
different geometries, including (a) cylindrical, (b) zig-zag, (c) meandering, and (d) spiral. Legend: 5: exit for
the CO2 fixation solution, 6: filter, 7A: fixation solution, 10A: reaction chamber, 10a: gas entrance, 10b: reaction
chamber, 10c: exit, 20, 21 and 22: nozzles, 70: water tank, 90a and 90b: sensors, and 200 and 201: pipes. The
original diagram was drawn by the author, and it was formally traced by Matsushima Patent Office, using
software “Hanako” add in “Ichitaro”.
Received: 15 October 2020; Accepted: 24 December 2021
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Acknowledgements
The author thanks Hiroyuki Okada, President of Shinko-Sangyo Co. Ltd., Takasaki, Gunma, Japan, for financial
support, Hideaki Kato, President of the Takasaki Denka-Kogyo, Co. Ltd., Takasaki, Gunma, Japan, for providing
encouragement regarding the present work, and Edanz Group (https://en-author-services.edanz.com/ac) for
editing a draft of this manuscript.
Author contributions
K.S. conceived, designed and carried out the study and also wrote the manuscript.
Competing interests
The author declares that the present data have been used to support applications to the Japan Patent Office
(PTC/JP2019/03400, PTC/JP2019/045839, PTC/JP2019/045390, PTC/JP2019/048178, PTC/JP2020/02064, PTC/
JP2020/02990, PTC/JP2020/029505, PTC/JP2020/002064, PTC/JP2020/031010, JP2021-321).
Additional information
Correspondence and requests for materials should be addressed to K.S.
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Scientific Reports |
(2022) 12:1694 |
https://doi.org/10.1038/s41598-022-05151-9
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Rasmussen University – NUR2063: Essentials of Pathophysiology
Title of Assignment:
Module 03 Written Assignment – Musculoskeletal Disorders
Purpose of Assignment:
The purpose of this assignment is to identify and analyze a musculoskeletal system disorder to process
the possible manifestations of a selected disorder. The concept map will help you identify the
pathophysiology of the musculoskeletal system disorder.
Course Competency(s):
•
Evaluate pathophysiologic alterations that affect the integumentary and musculoskeletal
systems.
Instructions:
Content:
Prepare a concept map for a musculoskeletal disorder from your readings. Use the included template to
outline the system disorder including the pathophysiology, etiology, clinical manifestations, and
treatment.
Format:
•
•
Use at least one scholarly source to support your findings. Examples of scholarly sources include
academic journals, textbooks, reference texts, and CINAHL nursing guides.
Be sure to cite your sources in-text and on a references page using APA format.
Resources:
You can find useful reference materials for this assignment in the School of Nursing guide:
https://guides.rasmussen.edu/nursing/referenceebooks
Have questions about APA? Visit the online APA guide: https://guides.rasmussen.edu/apa
09/09/2021
Rasmussen University – NUR2063: Essentials of Pathophysiology
Pathophysiology System Disorder Template
Student Name:
Disorder/Disease process:
PATHOPHYSIOLOGY OF THE DISORDER:
Sources:
ETIOLOGY:
CLINICAL MANIFESTATIONS:
Sources:
Sources:
Adapted from ATI, System Disorder Active Learning Template
09/09/2021
Rasmussen University – NUR2063: Essentials of Pathophysiology
TREATMENTS:
Sources:
Adapted from ATI, System Disorder Active Learning Template
09/09/2021
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