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Correspondence to Yingying Lu or Haotian Wang. Peer review information Nature Communications thanks the anonymous reviewers for their contribution to the peer review of this work. Peer reviewer reports are available. Reprints and Permissions. Electrochemical CO 2 reduction to high-concentration pure formic acid solutions in an all-solid-state reactor.
Nat Commun 11, Download citation. Received : 31 March Accepted : 25 June Published : 20 July Anyone you share the following link with will be able to read this content:.
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Advanced search. Skip to main content Thank you for visiting nature. Download PDF. Subjects Electrocatalysis Electrochemistry Energy. Abstract Electrochemical CO 2 reduction reaction CO 2 RR to liquid fuels is currently challenged by low product concentrations, as well as their mixture with traditional liquid electrolytes, such as KHCO 3 solution.
Introduction Electrochemical carbon dioxide reduction reaction CO 2 RR is changing the way we produce chemicals and fuels, while helping to mitigate climate change 1 , 2 , 3 , 4 , 5 , 6 , 7 , 8.
Full size image. Results and discussion Fabrication and characterizations of nBuLi-Bi catalyst We selected Bi as the catalytic material for CO 2 RR due to its intrinsic high-selectivity towards formate 35 , 36 , 49 , GOV collections:.
GOV Patent: Method and system for electrochemical production of formic acid from carbon dioxide. Title: Method and system for electrochemical production of formic acid from carbon dioxide. Abstract An electrochemical device converts carbon dioxide to a formic acid reaction product. Publication Date: Research Org. Method and system for electrochemical production of formic acid from carbon dioxide. United States: N. Copy to clipboard. United States. View Patent. Poly ionic liquid s as new materials for CO.
Composite blend polymer membranes with increased proton selectivity and lifetime for vanadium redox flow batteries journal , June Chen, Dongyang; Kim, Soowhan; Sprenkle, Vincent Journal of Power Sources, Vol. Journal of the Electrochemical Society, Vol. Electrolysis of carbon dioxide in aqueous media to carbon monoxide and hydrogen for production of methanol patent , March Olah, George; Prakash, G. Anion-exchange membranes in electrochemical energy systems journal , January Varcoe, John R.
Imidazolium-functionalized poly ether ether ketone as membrane and electrode ionomer for low-temperature alkaline membrane direct methanol fuel cell journal , March Yan, Xiaoming; Gu, Shuang; He, Gaohong Journal of Power Sources, Vol. According to the configuration of the present invention, the alkali metal or alkaline earth metal electrolyte generated in the second cathode chamber of the second separator membrane electrolyte tank is supplied to the first cathode chamber of the first membrane electrolyte cell; In addition, the formate produced in the first cathode chamber may be configured to be supplied back to the second anode chamber of the second diaphragm electrolyzer.
According to another configuration of the present invention, an alkali metal or alkaline earth metal electrolyte generated in the second cathode chamber of the second membrane electrolyte is supplied to the first anode chamber of the first electrolyte membrane electrolyzer; In addition, the formate produced in the first cathode chamber may be configured to be supplied back to the second anode chamber of the second diaphragm electrolyzer.
In this case, the solution supplied from the outside into the first diaphragm electrolyzer and the second diaphragm electrolyzer may be configured to additionally supply an electrolyte including an additional alkali metal or alkaline earth metal ion to reduce electrolyte resistance. In addition, the discharge water discharged after the electrolytic reaction in the first anode chamber may be configured to be supplied to the second cathode chamber. In addition, the discharge water discharged from the second cathode chamber may be configured to be supplied simultaneously by branching to the first anode chamber and the first cathode chamber.
One electrode can be used as the anode. A formic acid production method according to the present invention comprises a first electrolytic process of producing formate by receiving carbon dioxide; And a second electrolysis process of receiving formate produced by the first electrolysis process to generate formic acid. In the first electrolytic process for producing a formate according to the present invention, oxygen O 2 and hydrogen ions are supplied through the electrolysis reaction of water H 2 O supplied to the first anode chamber of the first diaphragm electrolyzer.
In the first electrolytic process for producing another formate of the present invention, the water H 2 O supplied to the first anode chamber of the first diaphragm electrolyzer is electrolyzed at the first anode to form oxygen O 2 and hydrogen. And moving the alkali metal or alkaline earth metal cation remaining after forming formic acid through the second diaphragm to the second cathode chamber. It is configured by.
Supplying the formate solution generated in the first cathode chamber of the first diaphragm electrolyzer to the second anode chamber of the second diaphragm electrolyzer in the process of producing the formic acid of the present invention; And separately supplying the alkali metal or alkaline earth metal electrolyte solution generated in the second cathode chamber to the first anode chamber or the first cathode chamber of the first diaphragm electrolyzer, or branching them to both the first cathode chamber and the first cathode chamber.
It may be configured to include;. In addition, in the process of manufacturing the formic acid may be configured to include the step of supplying the discharged water discharged from the first anode chamber of the first diaphragm electrolyzer to the second cathode chamber of the second diaphragm electrolyzer. Effects by the formic acid production apparatus and production method according to the present invention are as follows.
First, the supply of additional chemicals to convert formate to formic acid can be minimized. Second, the alkali metal or alkaline earth metal cation required for formate production in the added electrolyzer can be supplied by a circulation loop without additional supply. Figure 2 is an exemplary view showing the configuration and operation according to the formic acid production apparatus according to the prior art.
Figure 3 is an exemplary view showing the configuration of the formic acid production apparatus according to an embodiment of the present invention. Hereinafter, the present invention will be described in detail with reference to the accompanying drawings. The first diaphragm electrolyzer a includes a first anode chamber a and a first cathode chamber a configured to face each other with respect to the first diaphragm a, and includes a first anode chamber a in the first anode chamber a.
First anode a is provided with first cathode a in first cathode chamber a. The second diaphragm electrolyzer a consists of a second anode chamber a and a second cathode chamber a configured to face each other with respect to the second diaphragm a, and includes a second cathode chamber a in the second anode chamber a.
The second anode a is provided with the second cathode a in the second cathode chamber a. Preferably, the first diaphragm a and the second diaphragm a of the first diaphragm electrolyzer a and the second diaphragm electrolyzer a are cation exchange membranes.
The second diaphragm electrolyzer a receives the formate produced in the first diaphragm electrolyzer a and converts it into formic acid to produce a desired product, and also generates an alkali metal or alkaline earth metal electrolyte.
It serves as a one-electrode membrane electrolytic cell a. In the following detailed description of the present invention, an alkali metal or alkaline earth metal electrolyte is composed of potassium hydroxide KOH and potassium sulfate K 2 SO 4 , and the formate is directed to potassium formate HCOOK produced from such an electrolyte.
Although demonstrated, it is not limited to these compounds. In the preparation of formic acid according to an embodiment of the present invention according to FIG. At this time, the direction switching valve a is set to supply potassium hydroxide KOH to the first cathode chamber a from an external supply device not shown.
When the electrolyte is supplied to the first gap membrane electrolytic cell and the DC power is supplied to each of the first anode a and the first cathode a by a respective DC power supply device not shown , the first anode a and the first cathode a are formed. In each of the first cathode a, an electrolysis reaction is performed.
In this case, an electrolyte such as potassium hydroxide KOH may be additionally supplied to the water H 2 O supplied to the first anode chamber a to reduce electrical resistance during the electrolytic reaction. Depending on the supply and type of the electrolyte, the reaction product in the first anode chamber a may vary, but the overall ion balance and the process of preparing potassium formate HCOOK may be the same. Next, potassium formate HCOOK generated in the first cathode chamber a of the first clearance membrane electrolyzer a is provided to the second anode chamber a of the second clearance membrane electrolyzer a symbol.
Each decomposition electrolysis reaction takes place. Conversion Eq. The resulting formic acid HCOOH may be configured by adding an evaporator or separator at the rear end to match the desired product concentration and purity not shown. In this case, an electrolyte such as potassium hydroxide KOH may be additionally supplied to the water H 2 O supplied to the second cathode chamber a to reduce the electrical resistance during the electrolytic reaction.
It does not affect the ion balance. The direction switching valve a transfers potassium hydroxide KOH generated in the second cathode chamber a of the second clearance membrane electrolyzer a to the first cathode chamber a of the first clearance membrane electrolyzer a.
Is switched to. Accordingly, potassium hydroxide KOH generated in the second cathode chamber a of the second gap membrane electrolyzer a is transferred to the first cathode chamber a of the first gap membrane electrolyzer a, thereby further adding potassium hydroxide. However, in the actual process, some of the electrolyte loss caused by the current efficiency, the movement and speed of the material through the membrane, the loss in the transfer and reaction of the solution may be additionally supplied.
In this embodiment, the discharge water discharged from the first anode chamber a may be further configured to be supplied to the second cathode chamber a. By such a configuration, it is possible to reduce the consumption of water and to somewhat reduce the electrical resistance of the electrolyte solution supplied to each electrolytic cell. In addition, a portion of the potassium hydroxide KOH solution supplied from the second cathode chamber a to the first cathode chamber a may be further configured to be supplied to the first cathode chamber a.
Through this configuration, the electrical resistance of the electrolyte supplied to the first anode chamber a can be reduced. First, carbon dioxide CO 2 and potassium hydroxide KOH are supplied to the first cathode chamber a of the first electrolytic cell a.
At this time, water is supplied to the first anode chamber a of the first electrolytic cell a S Potassium formate HCOOK generated in the first cathode chamber a of the first electrolytic cell a is provided in the second anode chamber a of the second electrolytic cell a S Potassium hydroxide KOH generated in the second cathode chamber a of the second electrolytic cell a is supplied to the first cathode chamber a of the first electrolytic cell a S Similar to one embodiment of the present invention, the first diaphragm electrolyzer b and the second diaphragm electrolyzer b are included.
The first diaphragm electrolyzer b is configured to face each other with respect to the first diaphragm b and includes a first anode chamber b having a first anode b therein and a first cathode b embedded therein. The first cathode chamber b, the second diaphragm electrolyzer b is configured to face each other with respect to the second diaphragm b, and the second anode chamber b having the second anode b embedded therein.
The second cathode b includes the second cathode chamber b in which the second cathode b is embedded.
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