CN115161665A - Application of trifluoroacetic acid as synergist for hydrogen production by water electrolysis, and electrolyte for hydrogen production by water electrolysis - Google Patents

Application of trifluoroacetic acid as synergist for hydrogen production by water electrolysis, and electrolyte for hydrogen production by water electrolysis Download PDF

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CN115161665A
CN115161665A CN202211005447.9A CN202211005447A CN115161665A CN 115161665 A CN115161665 A CN 115161665A CN 202211005447 A CN202211005447 A CN 202211005447A CN 115161665 A CN115161665 A CN 115161665A
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electrolyte
hydrogen production
water electrolysis
trifluoroacetic acid
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孙晓明
丁小倩
罗亮
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Beijing University of Chemical Technology
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    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C25B1/01—Products
    • C25B1/02—Hydrogen or oxygen
    • C25B1/04—Hydrogen or oxygen by electrolysis of water
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
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    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract

The invention provides application of trifluoroacetic acid as a synergist for hydrogen production by water electrolysis, and electrolyte for hydrogen production by water electrolysis, belonging to the technical field of water electrolysis. According to the invention, trifluoroacetic acid is used as the synergist for hydrogen production by water electrolysis, so that the electrochemical hydrogen evolution reaction in the water electrolysis process can be promoted, the current of the electrochemical reaction is increased to a greater extent, and the peak starting potential can be changed to advance the peak starting, thereby improving the efficiency of the whole electrochemical reaction; and the trifluoroacetic acid is used as a synergist for hydrogen production by water electrolysis and is suitable for acidic, neutral and alkaline electrolyte systems. The results of the examples show that the trifluoroacetic acid as the synergist for hydrogen production by water electrolysis can improve HER efficiency and advance the peak potential under different pH conditions.

Description

Application of trifluoroacetic acid as synergist for hydrogen production by water electrolysis, and electrolyte for hydrogen production by water electrolysis
Technical Field
The invention relates to the technical field of water electrolysis, in particular to application of trifluoroacetic acid as a synergist for hydrogen production by water electrolysis and electrolyte for hydrogen production by water electrolysis.
Background
With the continuous consumption of fossil fuels and the increasing increase of environmental pollution, scientists have been working on developing new clean and inexpensive energy sources, such as nuclear energy, solar energy, ocean energy, geothermal energy, wind energy, hydrogen energy, etc., in an effort to move toward sustainable energy structures. Among them, hydrogen energy has a high energy density, and does not generate atmospheric pollutants when used as a fuel carrier to provide energy, and can realize carbon-free emission, and is receiving more and more attention.
At present, among numerous hydrogen energy production processes, the hydrogen production process by electrolysis from water is simple and mature. Hydrogen production by water electrolysis is a convenient method for producing hydrogen, direct current is introduced into an electrolytic cell filled with electrolyte, and water molecules respectively generate electrochemical reactions on two electrodes, namely an electrochemical Hydrogen Evolution Reaction (HER) and an electrochemical Oxygen Evolution Reaction (OER), so that hydrogen and oxygen are obtained.
In the process of hydrogen production by water electrolysis, a commonly used electrolyte is strong acid or strong base. However, the electrochemical reaction is not efficient using a strong acid or a strong base alone as an electrolyte. In the prior art, sodium Dodecyl Sulfate (SDS) is often added into the electrolyte, but the amplitude of the SDS for improving the electrochemical reaction efficiency is very small.
Disclosure of Invention
In view of the above, the invention aims to provide an application of trifluoroacetic acid as a synergist for hydrogen production by water electrolysis, and an electrolyte for hydrogen production by water electrolysis.
In order to achieve the above object, the present invention provides the following technical solutions:
the invention provides application of trifluoroacetic acid as a synergist for hydrogen production by water electrolysis.
Preferably, the amount of the trifluoroacetic acid added to the electrolyte is 0.01 to 0.6mol/L.
The invention provides an electrolyte for hydrogen production by water electrolysis, which comprises trifluoroacetic acid and an electrolyte solution, wherein the pH value of the electrolyte solution is 0-14.
Preferably, the electrolyte solution is an inorganic strong acid solution, an inorganic strong base solution or a buffer solution.
Preferably, the strong inorganic acid is sulfuric acid.
Preferably, the inorganic strong base is potassium hydroxide and/or sodium hydroxide.
Preferably, the buffer solution is KH 2 PO 4 Buffer solution, dipotassium hydrogen phosphate-potassium dihydrogen phosphate buffer solution or sodium carbonate-sodium bicarbonate buffer solution.
Preferably, the molar concentration of the trifluoroacetic acid in the electrolyte for hydrogen production by water electrolysis is 0.01-0.6 mol/L.
The invention provides a method for producing hydrogen by electrolyzing water, which comprises the following steps:
and electrolyzing the electrolyte for hydrogen production by water electrolysis by using a three-electrode system to obtain hydrogen.
The invention provides application of trifluoroacetic acid as a synergist for hydrogen production by water electrolysis. According to the invention, trifluoroacetic acid is used as a synergist for hydrogen production by water electrolysis, the addition of trifluoroacetic acid reduces the surface tension of bubbles, the adhesion of the bubbles is weakened, the supersaturation degree of generated bubbles is reduced, and nano bubbles are easier to grow into macroscopic bubbles, so that the reaction efficiency is improved, the electrochemical hydrogen evolution reaction in the hydrogen production process by water electrolysis can be promoted, the current of the electrochemical reaction is increased to a greater extent, the peak starting potential can be changed, the peak starting is advanced, and the efficiency of the whole electrochemical reaction is improved. Trifluoroacetic acid is used as a synergist for hydrogen production by water electrolysis and is suitable for acidic, neutral and alkaline electrolyte systems. The results of the examples show that the trifluoroacetic acid as the synergist for hydrogen production by water electrolysis can improve HER efficiency and advance the peak potential under different pH conditions.
The invention provides an electrolyte for hydrogen production by water electrolysis, which comprises trifluoroacetic acid and an electrolyte solution, wherein the pH value of the electrolyte solution is 0-14. The electrolyte for hydrogen production by water electrolysis takes trifluoroacetic acid as a synergist for hydrogen production by water electrolysis, and has high electrochemical reaction efficiency.
Drawings
Figure 1 is an LSV curve of the HER reaction of example 1 performed under acidic conditions;
figure 2 is an LSV curve of the HER reaction of example 2 under alkaline conditions;
figure 3 is an LSV curve of HER reaction of example 3 under neutral conditions;
FIG. 4 is the LSV curve at pH 0 for example 4;
FIG. 5 is the LSV curve at pH 4 for example 4;
FIG. 6 is the LSV curve at pH 7 for example 4;
FIG. 7 is the LSV curve at pH 10 for example 4;
FIG. 8 is the LSV curve at pH 14 for example 4;
figure 9 is a LSV curve of comparative example 1 for HER reaction;
figure 10 is an LSV curve of the HER reaction performed in comparative example 2.
Detailed Description
The invention provides application of trifluoroacetic acid as a synergist for hydrogen production by water electrolysis.
In the present invention, the amount of trifluoroacetic acid added to the electrolyte is preferably 0.01 to 0.6mol/L, more preferably 0.1 to 0.5mol/L, and still more preferably 0.2 to 0.4mol/L.
According to the invention, trifluoroacetic acid is used as the synergist for hydrogen production by water electrolysis, so that the electrochemical Hydrogen Evolution Reaction (HER) in the water electrolysis process can be promoted to be carried out, the current of the electrochemical reaction is increased to a greater extent, and the peak starting potential can be changed in the electrochemical hydrogen evolution reaction to advance the peak starting, so that the efficiency of the whole electrochemical reaction is improved; and the trifluoroacetic acid is used as a synergist for hydrogen production by water electrolysis and is suitable for both an acidic electrolyte system and an alkaline electrolyte system.
The invention provides an electrolyte for hydrogen production by water electrolysis, which comprises trifluoroacetic acid and an electrolyte solution, wherein the pH value of the electrolyte solution is 0-14, preferably 1-12, more preferably 3-10, and further preferably 5-7.
In the present invention, the electrolyte solution is preferably an inorganic strong acid solution, an inorganic strong base solution, or a buffer solution.
In the present invention, the strong inorganic acid is preferably sulfuric acid.
In the present invention, the inorganic strong base is limited to potassium hydroxide and/or sodium hydroxide.
In the present invention, the buffer solution is preferably KH 2 PO 4 Buffer solution, dipotassium hydrogen phosphate-potassium dihydrogen phosphate buffer solution or carbonic acidSodium-sodium bicarbonate buffer solution.
In the invention, the potassium dihydrogen phosphate buffer solution is an acid electrolyte; the dipotassium hydrogen phosphate-potassium dihydrogen phosphate buffer solution is neutral electrolyte; the sodium carbonate-sodium bicarbonate buffer solution is an alkaline electrolyte.
In the present invention, the molar concentration of the trifluoroacetic acid in the electrolyte for hydrogen production by electrolysis of water is preferably 0.01 to 0.6mol/L, more preferably 0.1 to 0.5mol/L, and still more preferably 0.2 to 0.4mol/L.
The invention provides a preparation method of the electrolyte for hydrogen production by electrolyzing water, which comprises the following steps:
and mixing trifluoroacetic acid with an electrolyte solution to obtain the electrolyte for hydrogen production by water electrolysis.
In the present invention, the mixing is preferably performed in the following manner:
in the present invention, the mixing is preferably performed by stirring. The invention has no special requirement on the specific operation mode of stirring and mixing.
In the present invention, the temperature of the mixing is preferably 20 to 30 ℃, more preferably 25 ℃.
The invention provides a method for producing hydrogen by electrolyzing water, which comprises the following steps:
and electrolyzing the electrolyte for hydrogen production by water electrolysis by using a three-electrode system to obtain hydrogen and oxygen.
In the invention, when the hydrogen is produced by electrolyzing water, the three-electrode system comprises a counter electrode, a working electrode and a reference electrode; the counter electrode is preferably a platinum wire and the working electrode is preferably a platinum sheet.
In the present invention, when the electrolyte solution is acidic or neutral, the reference electrode is preferably a saturated calomel electrode; when the electrolyte solution is alkaline, the reference electrode is preferably a mercury oxide electrode.
In the present invention, the electrode for producing hydrogen by electrolyzing water is preferably an alkaline membrane electrode.
The following examples are provided to illustrate the application of trifluoroacetic acid as a synergist for hydrogen production by water electrolysis and an electrolyte for hydrogen production by water electrolysis in detail, but they should not be construed as limiting the scope of the present invention.
Example 1
Preparing a solution:
KH with pH =4 was formulated 2 PO 4 Buffer solution, take 40mL of this solution as blank control. A further amount of the above solution was taken so that the concentration of trifluoroacetic acid (TFA) was 0.01M, 0.05M, 0.1M, respectively, and the total volume of the solution was 40mL.
The four solutions are used as electrolytes for electrolyzing water, a platinum wire is used as a counter electrode, a platinum sheet is used as a working electrode, and a saturated calomel electrode is used as a reference electrode to form a three-electrode system. HER was performed under acidic conditions, and LSV curves of the above four solutions were measured, and the results are shown in fig. 1; the corresponding voltage at-1 mA is shown in Table 1.
TABLE 1 Voltage at different trifluoroacetic acid contents at a current of-1 mA
TFA content/(mol/L) 0 0.01 0.05 0.1
Voltage/(mV) -114.8 -94.95 -58.53 -25.76
As can be seen from fig. 1 and table 1, as TFA concentration increases, current increases, peak potential advances, and HER efficiency increases. Too high a concentration may reduce the conductivity of the solution and may not be effective.
Example 2
Preparing a solution:
a sodium carbonate-sodium bicarbonate buffer solution with pH =10 was prepared and 40ml of this solution was taken as a blank. Then, a certain amount of the above solution was taken so that the trifluoroacetic acid concentration was 0.1M, 0.2M, 0.4M, and 0.6M, respectively, and the total volume of the solution was 40mL.
The five solutions are used as electrolytes for electrolyzing water, a platinum wire is used as a counter electrode, a platinum sheet is used as a working electrode, and a mercury oxide electrode is used as a reference electrode to form a three-electrode system. HER was performed under alkaline conditions, and LSV curves of the above five solutions were measured, and the results are shown in fig. 2; the corresponding voltage at-1 mA is shown in Table 2.
TABLE 2 Voltage at different trifluoroacetic acid contents at a current of-1 mA
TFA content/(mol/L) 0 0.1 0.2 0.4 0.6
Voltage/(mV) 8.421 17.28 29.57 51.86 99.58
As can be seen from table 2 and fig. 2, under alkaline conditions, as TFA concentration increases, current increases, peak potential advances, and HER efficiency increases.
Example 3
Preparing a solution:
a dipotassium hydrogen phosphate-potassium dihydrogen phosphate buffer solution with pH =7 was prepared, and 40ml of this solution was taken as a blank control. Then, a certain amount of the above solution was taken so that the concentration of trifluoroacetic acid was 0.01M, 0.05M and 0.2M, respectively, and the total volume of the solution was 40mL.
The four solutions are used as electrolytes for electrolyzing water, a platinum wire is used as a counter electrode, a platinum sheet is used as a working electrode, and a saturated calomel electrode is used as a reference electrode to form a three-electrode system. HER was performed under neutral conditions, and LSV curves of the above four solutions were measured, and the results are shown in fig. 3; the voltage at-1 mA is shown in Table 3.
TABLE 3 Voltage at different trifluoroacetic acid contents at a current of-1 mA
TFA content/(mol/L) 0 0.01 0.05 0.2
Voltage/(mV) 32.77 44.70 52.24 77.39
As can be seen from table 3 and fig. 3, under neutral conditions, the onset of peak potential advances and HER efficiency increases with increasing TFA concentration.
Example 4
Electrolyte solutions with pH values of 0, 4, 7, 10 and 14 were prepared, and 40ml of the solution was used as a blank control. And then a certain amount of the solution is taken, and trifluoroacetic acid is added to ensure that the concentration of the trifluoroacetic acid is 0.01M and the total volume of the solution is 40mL. The electrolyte composition is shown in Table 4.
TABLE 4 electrolyte composition
Figure BDA0003808480800000061
The five solutions are used as electrolytes for electrolyzing water, a platinum wire is used as a counter electrode, a platinum sheet is used as a working electrode, and a saturated calomel electrode (with acidic or neutral pH) or mercuric oxide electrode (with alkaline pH) is used as a reference electrode to form a three-electrode system. HER was performed, and the LSV curves of the above five solutions were measured, and the results are shown in fig. 4 to 8, in which fig. 4 is the LSV curve at pH 0, fig. 5 is the LSV curve at pH 4, fig. 6 is the LSV curve at pH 7, fig. 7 is the LSV curve at pH 10, and fig. 8 is the LSV curve at pH 14.
As can be seen in fig. 4-8, TFA promotes HER under acidic, neutral and basic conditions.
Comparative example 1
Formulation pH = 1H 2 SO 4 Solution, 50mL of this solution was used as a blank. And adding a certain amount of the solution into Sodium Dodecyl Sulfate (SDS) of 0.1CMC, 0.3CMC, 0.5CMC, 0.7CMC and 1CMC, wherein the total volume of the solution is 50mL, and the CMC represents the critical micelle concentration. In the above six solutions, HER was performedMeasuring the LSV curve, and obtaining the result shown in figure 9; the corresponding voltage at-1 mA is shown in Table 5.
TABLE 5-1mA voltages at different SDS contents
SDS content 0 0.1CMC 0.3CMC 0.5CMC 0.7CMC 1CMC
Voltage/(mV) -31.68 -24.83 -22.54 -22.05 -25.79 -26.63
As can be seen from fig. 9 and table 5, the addition of SDS can increase the current to a certain extent, and also has a certain effect on advancing the peak potential, thereby improving the HER efficiency, but the improvement amplitude is small and the effect is not significant enough.
Comparative example 2
Formulation pH = 1H 2 SO 4 Taking 50mL of the solution as the solutionBlank control. And then adding a certain amount of the solution into 0.1CMC, 0.3CMC, 0.5CMC, 0.7CMC and 1CMC of Cetyl Trimethyl Ammonium Bromide (CTAB), wherein the total volume of the solution is 50mL, and the CMC represents the critical micelle concentration. HER was performed on the above six solutions, and the LSV curves thereof were measured, and the results are shown in fig. 10; the voltage at-1 mA is shown in Table 6.
TABLE 6-1mA voltages at different CTAB contents
TFA content 0 0.1CMC 0.3CMC 0.5CMC 0.7CMC 1CMC
Voltage/(mV) -27.53 -28.97 -33.05 -30.93 -35.33 -34.04
As can be seen from fig. 10 and table 6, addition of CTAB rather inhibits increase of current and also lags behind the peak potential, probably because CTAB is a cationic surfactant, and inhibits migration of hydrogen ions, which is not favorable for improvement of HER efficiency.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.

Claims (9)

1. The application of trifluoroacetic acid as synergist for hydrogen production by water electrolysis.
2. The use according to claim 1, wherein the trifluoroacetic acid is added in the electrolyte in an amount of 0.01 to 0.6mol/L.
3. An electrolyte for hydrogen production by water electrolysis comprises trifluoroacetic acid and an electrolyte solution, wherein the pH value of the electrolyte solution is 0-14.
4. The electrolyte solution for producing hydrogen by electrolyzing water as recited in claim 3, wherein said electrolyte solution is a strong inorganic acid solution, a strong inorganic base solution or a buffer solution.
5. The electrolyte for hydrogen production by electrolysis of water according to claim 4, wherein the strong inorganic acid is sulfuric acid.
6. The electrolyte for producing hydrogen by electrolyzing water as recited in claim 4, wherein said inorganic strong base is potassium hydroxide and/or sodium hydroxide.
7. The electrolyte for producing hydrogen by electrolyzing water as claimed in claim 4, wherein the buffer solution is KH 2 PO 4 Buffer solution, dipotassium hydrogen phosphate-potassium dihydrogen phosphate buffer solution or sodium carbonate-sodium bicarbonate buffer solution.
8. The electrolyte for hydrogen production by electrolysis of water according to claim 3, wherein the molar concentration of trifluoroacetic acid in the electrolyte for hydrogen production by electrolysis of water is 0.01 to 0.6mol/L.
9. A method for producing hydrogen by electrolyzing water comprises the following steps:
electrolyzing the electrolyte for hydrogen production by water electrolysis as claimed in any one of claims 3 to 8 by using a three-electrode system to obtain hydrogen.
CN202211005447.9A 2022-08-22 2022-08-22 Application of trifluoroacetic acid as synergist for hydrogen production by water electrolysis, and electrolyte for hydrogen production by water electrolysis Pending CN115161665A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115558947A (en) * 2022-10-24 2023-01-03 云南电网有限责任公司电力科学研究院 Electrochemical hydrogenation cathode electrolyte and electrochemical hydrogenation method

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115558947A (en) * 2022-10-24 2023-01-03 云南电网有限责任公司电力科学研究院 Electrochemical hydrogenation cathode electrolyte and electrochemical hydrogenation method

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