CN114717570A - Weakly-bound water structure modified alkaline electrolyte and preparation method thereof - Google Patents
Weakly-bound water structure modified alkaline electrolyte and preparation method thereof Download PDFInfo
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- CN114717570A CN114717570A CN202210278860.6A CN202210278860A CN114717570A CN 114717570 A CN114717570 A CN 114717570A CN 202210278860 A CN202210278860 A CN 202210278860A CN 114717570 A CN114717570 A CN 114717570A
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- alkaline electrolyte
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- 239000003792 electrolyte Substances 0.000 title claims abstract description 78
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 32
- 238000002360 preparation method Methods 0.000 title claims abstract description 19
- 239000000654 additive Substances 0.000 claims abstract description 24
- 230000000996 additive effect Effects 0.000 claims abstract description 22
- 238000003756 stirring Methods 0.000 claims abstract description 18
- 238000009210 therapy by ultrasound Methods 0.000 claims abstract description 12
- 239000002245 particle Substances 0.000 claims description 11
- 229910001860 alkaline earth metal hydroxide Inorganic materials 0.000 claims description 4
- CYPPCCJJKNISFK-UHFFFAOYSA-J kaolinite Chemical compound [OH-].[OH-].[OH-].[OH-].[Al+3].[Al+3].[O-][Si](=O)O[Si]([O-])=O CYPPCCJJKNISFK-UHFFFAOYSA-J 0.000 claims description 3
- 229910052622 kaolinite Inorganic materials 0.000 claims description 3
- 150000008044 alkali metal hydroxides Chemical class 0.000 claims description 2
- 229910052900 illite Inorganic materials 0.000 claims description 2
- VGIBGUSAECPPNB-UHFFFAOYSA-L nonaaluminum;magnesium;tripotassium;1,3-dioxido-2,4,5-trioxa-1,3-disilabicyclo[1.1.1]pentane;iron(2+);oxygen(2-);fluoride;hydroxide Chemical compound [OH-].[O-2].[O-2].[O-2].[O-2].[O-2].[F-].[Mg+2].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[K+].[K+].[K+].[Fe+2].O1[Si]2([O-])O[Si]1([O-])O2.O1[Si]2([O-])O[Si]1([O-])O2.O1[Si]2([O-])O[Si]1([O-])O2.O1[Si]2([O-])O[Si]1([O-])O2.O1[Si]2([O-])O[Si]1([O-])O2.O1[Si]2([O-])O[Si]1([O-])O2.O1[Si]2([O-])O[Si]1([O-])O2 VGIBGUSAECPPNB-UHFFFAOYSA-L 0.000 claims description 2
- 238000006243 chemical reaction Methods 0.000 abstract description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 5
- 239000001301 oxygen Substances 0.000 abstract description 5
- 229910052760 oxygen Inorganic materials 0.000 abstract description 5
- 238000004458 analytical method Methods 0.000 abstract description 2
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 48
- 238000000034 method Methods 0.000 description 16
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 12
- 239000007864 aqueous solution Substances 0.000 description 11
- 239000005995 Aluminium silicate Substances 0.000 description 10
- 235000012211 aluminium silicate Nutrition 0.000 description 10
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 description 10
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 5
- 239000001257 hydrogen Substances 0.000 description 5
- 229910052739 hydrogen Inorganic materials 0.000 description 5
- 238000005303 weighing Methods 0.000 description 5
- 239000010411 electrocatalyst Substances 0.000 description 4
- 238000011160 research Methods 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 3
- 239000011777 magnesium Substances 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 238000001878 scanning electron micrograph Methods 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 2
- 229910000272 alkali metal oxide Inorganic materials 0.000 description 2
- 150000001340 alkali metals Chemical class 0.000 description 2
- 150000001768 cations Chemical class 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000006703 hydration reaction Methods 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
- 150000001450 anions Chemical class 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000036571 hydration Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000011859 microparticle Substances 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 239000006259 organic additive Substances 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
Images
Classifications
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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
-
- 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
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/10—Process efficiency
- Y02P20/133—Renewable energy sources, e.g. sunlight
Abstract
The invention discloses a preparation method of a weak-bound water structure modified alkaline electrolyte, which comprises the following steps: preparing an alkaline electrolyte by using water and an alkaline electrolyte; adding an additive with negative surface charge into the alkaline electrolyte prepared in the step S1; and (4) carrying out ultrasonic treatment on the solution obtained in the step (S2), and then stirring to fully disperse the additive with negative surface charge in the electrolyte to obtain the modified electrolyte. Compared with the traditional electrolyte, the electrolyte modified by the surface negatively charged additive can improve the stability of the oxygen analysis reaction of the electrocatalytic water, and obviously reduce the overpotential of the electrode. In addition, the preparation method is simple in preparation process, low in cost, suitable for batch application and wide in application prospect in the fields of electrocatalysis and photoelectrocatalysis.
Description
Technical Field
The invention relates to the technical field of hydrogen production by electrochemical water decomposition, in particular to a modified alkaline electrolyte with a weak water-binding structure and a preparation method thereof.
Background
In response to the increasingly serious shortage of energy and environmental crisis, the development of renewable clean energy is a subject of great concern. The electrochemical water decomposition technology can convert electric energy obtained by converting solar energy into hydrogen energy with high energy density through water decomposition reaction. The electrochemical water splitting reaction consists of three series processes of Hydrogen Evolution Reaction (HER) at a cathode, Oxygen Evolution Reaction (OER) at an anode and mass transfer in a solution. OER involves a four-electron process, compared to HER, which involves the participation of two electrons, and the slow reaction kinetics become a major bottleneck limiting the energy conversion efficiency of water-splitting cells. Therefore, improving the OER efficiency is significant for realizing efficient photoelectrochemical water splitting.
According to the existing research, the slow Oxygen Evolution Reaction (OER) of the solid-liquid interface of the electrocatalyst/electrolyte is the speed control step of the water electrolysis reaction. Therefore, it is a first task to improve the efficiency of Oxygen Evolution Reaction (OER). Currently, the optimization strategy for improving the OER efficiency can be mainly divided into two directions: optimizing and modifying the electrocatalyst and the electrolyte. Among them, the research work of the OER electrocatalyst is extensive, for example: CN109647477B, CN111841602B and CN 111437831B. However, for the series reaction process of OER, the electrolyte with less research and poor performance will become a short plate and bottleneck limiting OER efficiency compared to the fast-developing electrocatalyst.
At present, the research on the electrolyte is less, and the Chinese patent application CN111101143A discloses a method for reducing the overpotential of an electrode by reducing the influence of bubbles on the effective working area of the electrode by using a perfluorinated organic additive, which has the defects that the influence of the bubbles on the effective working area can only be solved, the reaction kinetic process of OER can not be promoted, and the efficiency of the electrode is improved and the service life is prolonged and limited; chinese patent application CN113078331A discloses a high-performance electrolyte for magnesium water hydrogen production battery, which effectively strips reaction products Mg (OH) by using cation or anion additive2The method has the defects of narrow application range and can only be used for improving the efficiency and the service life of the magnesium water hydrogen production battery.
OER in alkaline electrolyte, reactant is OH-Due to hydration, hydrated shells can be formed around the electrode, and the transmission and adsorption of OH-to the surface of the electrode are hindered. Therefore, it is desirable to find a method for thinning the OH-hydration shell layer to effectively improve OER efficiency and stability.
Disclosure of Invention
The invention aims to: in order to solve the technical problems, the invention provides a weak-bound water structure modified alkaline electrolyte and a preparation method thereof.
The technical scheme is as follows: the invention discloses a preparation method of a weak-bound water structure modified alkaline electrolyte, which comprises the following steps:
s1: preparing alkaline electrolyte by using water and alkaline electrolyte;
s2: adding an additive with negative surface charge into the alkaline electrolyte prepared in the step S1;
s3: and (4) carrying out ultrasonic treatment on the solution obtained in the step (S2), and then stirring to fully disperse the additive with negative surface charge in the electrolyte to obtain the modified electrolyte.
Preferably, in step S1, the alkaline electrolyte is alkali metal hydroxide or alkaline earth metal hydroxide, and the concentration of the alkaline electrolyte is 1 × 10-5-10mol/L。
Preferably, in step S2, the additive with negative surface charge has a particle size of 0.1-100 μm and is added in an amount of 0.1-5% by mass of the alkaline electrolyte.
Preferably, in step S3, the ultrasonic treatment time is 1-20 min.
Preferably, in step S3, the stirring speed is 100-1000 r/min.
Preferably, in step S2, the negatively charged additive is selected from one of kaolinite, illite, or Mxene.
The invention also provides a weakly-bound water structure modified alkaline electrolyte prepared by the preparation method of the weakly-bound water structure modified alkaline electrolyte.
Has the advantages that: compared with the traditional electrolyte, the electrolyte modified by the surface negatively charged additive can improve the stability of the oxygen analysis reaction of the electrocatalytic water, and obviously reduce the overpotential of the electrode. In addition, the preparation method is simple in preparation process, low in cost, suitable for batch application and wide in application prospect in the fields of electrocatalysis and photoelectrocatalysis.
Drawings
FIG. 1 is a schematic view of an electrocatalytic testing device for kaolin modified electrolyte in the present invention;
figure 2 is an SEM image of a partially negatively charged microparticle as applied in the present invention.
In the figure, 1-electrolyte, 2-negatively surface-charged particles, 3-anode, 4-cathode.
Detailed Description
The invention will be further explained with reference to the drawings.
As shown in fig. 1, the preparation method of the weakly water-binding structure modified alkaline electrolyte of the invention comprises the following steps:
s1: preparing an alkaline electrolyte by using water and an alkaline electrolyte; specifically, a certain amount of alkali metal or alkaline earth metal hydroxide is weighed, placed in an aqueous solution, and stirred until the alkali metal or alkaline earth metal hydroxide is completely dissolved; the concentration of the electrolyte is 1X 10-5-10 mol/L; the preferred concentration is 0.05-4 mol/L.
S2: adding an additive with negative surface charge into the alkaline electrolyte prepared in the step S1; the additive is one of kaolinite and Mxene; the particle size of the additive with negative surface charge is 0.1-100 microns, preferably 0.5-10 microns, and the addition amount of the additive with negative surface charge is 0.1-5%, preferably 0.2-3% of the mass of the electrolyte.
S3: and (4) carrying out ultrasonic treatment on the solution obtained in the step (S2), and then stirring to fully disperse the additive with negative surface charge in the electrolyte to obtain the modified electrolyte. The ultrasonic treatment time is 1-20min, preferably 5-10 min. The stirring treatment is continued, with a stirring rotation speed of 100-.
In FIG. 2, a is an SEM image of Mxene particles and b is an SEM image of kaolin particles.
Example 1
The method selects a potassium hydroxide aqueous solution as an original electrolyte, and comprises the following specific implementation processes:
preparing an alkaline electrolyte: weighing 5.6g of potassium hydroxide, placing the potassium hydroxide into 100mL of aqueous solution, and stirring until the potassium hydroxide is completely dissolved to prepare 1mol/L electrolyte;
adding kaolin: 0.2g of kaolin (with the particle size of 0.5 micron) is weighed and added into 100mL of 1mol/L alkaline electrolyte, namely the additive is added in an amount of 0.2 percent, ultrasonic treatment is carried out for 5min, and then continuous stirring is carried out at the rotating speed of 200 r/min.
Example 2
The method selects a potassium hydroxide aqueous solution as an original electrolyte, and comprises the following specific implementation processes:
preparing an alkaline electrolyte: weighing 0.28g of potassium hydroxide, placing the potassium hydroxide into 100mL of aqueous solution, and stirring until the potassium hydroxide is completely dissolved to prepare 0.05mol/L electrolyte;
adding kaolin: 3.0g of kaolin (with the particle size of 9.5 microns) is weighed and added into 100mL of 0.05mol/L alkaline electrolyte, namely the additive is added in an amount of 3%, ultrasonic treatment is carried out for 10min, and then continuous stirring is carried out at the rotating speed of 200 r/min.
Example 3
The method selects sodium hydroxide aqueous solution as the original electrolyte, and comprises the following specific implementation processes:
preparing an alkaline electrolyte: weighing 4.0g of sodium hydroxide, placing the sodium hydroxide in 100mL of aqueous solution, and stirring until the sodium hydroxide is completely dissolved to prepare 1mol/L electrolyte;
adding kaolin: 3.0g of kaolin (with the particle size of 1.5 microns) is weighed and added into 100mL of 1mol/L alkaline electrolyte, namely the additive is added in an amount of 3 percent, ultrasonic treatment is carried out for 5min, and then continuous stirring is carried out at the rotating speed of 300 r/min.
Example 4
The method selects a potassium hydroxide aqueous solution as an original electrolyte, and comprises the following specific implementation processes:
preparing an alkaline electrolyte: weighing 11.2g of potassium hydroxide, placing the potassium hydroxide in 100mL of aqueous solution, and stirring until the potassium hydroxide is completely dissolved to prepare 1mol/L electrolyte;
addition of Mxene: 1.0g of Mxene (particle size of 1.04 micron) is weighed and added into 100mL of 1mol/L alkaline electrolyte, namely the additive is added in an amount of 1 percent, ultrasonic treatment is carried out for 8min, and then continuous stirring is carried out at a rotating speed of 200 r/min.
Example 5
The method selects a potassium hydroxide aqueous solution as an original electrolyte, and comprises the following specific implementation processes:
preparing an alkaline electrolyte: weighing 22.4g of potassium hydroxide, placing the potassium hydroxide in 100mL of aqueous solution, and stirring until the potassium hydroxide is completely dissolved to prepare 4mol/L electrolyte;
adding kaolin: 3.0g of kaolin (with the particle size of 9.5 microns) is weighed and added into 100mL of 4mol/L alkaline electrolyte, namely the additive is added in an amount of 3 percent, ultrasonic treatment is carried out for 10min, and then continuous stirring is carried out at the rotating speed of 250 r/min.
The performance measurements obtained for examples 1-5 are shown in the following table:
from the table above, it can be seen that in examples 1 to 5, the electrocatalytic water splitting performance of the alkaline electrolytes with different concentrations and different cations is significantly improved after being modified by the negatively charged additives with different addition amounts.
Claims (7)
1. A preparation method of a weak-bound water structure modified alkaline electrolyte is characterized by comprising the following steps:
s1: preparing alkaline electrolyte by using water and alkaline electrolyte;
s2: adding an additive with negative surface charge into the alkaline electrolyte prepared in the step S1;
s3: and (4) carrying out ultrasonic treatment on the solution obtained in the step (S2), and then stirring to fully disperse the additive with negative surface charge in the electrolyte to obtain the modified electrolyte.
2. The preparation method of the weakly water-binding structure modified alkaline electrolyte according to claim 1, characterized by comprising the following steps: in step S1, the alkaline electrolyte is an alkali metal hydroxide or an alkaline earth metal hydroxide, and the concentration of the alkaline electrolyte is1×10-5-10mol/L。
3. The preparation method of the weakly water-binding structure modified alkaline electrolyte according to claim 1, characterized by comprising the following steps: in step S2, the additive with negative surface charge has a particle size of 0.1-100 microns and is added in an amount of 0.1-5% of the mass of the alkaline electrolyte.
4. The preparation method of the weakly water-binding structure modified alkaline electrolyte according to claim 1, characterized by comprising the following steps: in step S3, the ultrasonic treatment time is 1-20 min.
5. The preparation method of the weakly water-binding structure modified alkaline electrolyte according to claim 1, characterized by comprising the following steps: in step S3, the stirring speed is 100-1000 r/min.
6. The preparation method of the weakly water-binding structure modified alkaline electrolyte according to claim 1, characterized by comprising the following steps: in step S2, the negatively charged additive is selected from one of kaolinite, illite, or Mxene.
7. The weakly water-binding structure modified alkaline electrolyte is characterized by being prepared by the preparation method of the weakly water-binding structure modified alkaline electrolyte disclosed by any one of claims 1-6.
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1507098A (en) * | 2002-12-12 | 2004-06-23 | ����Sdi��ʽ���� | Nano composite electrolytic solution film and fuel battery utilizing the same |
| US20140205909A1 (en) * | 2011-08-23 | 2014-07-24 | Nippon Shokubai Co., Ltd. | Negative electrode mixture or gel electrolyte, and battery using said negative electrode mixture or said gel electrolyte |
| CN109980302A (en) * | 2019-04-29 | 2019-07-05 | 中南大学 | A kind of water system Zinc ion battery colloidal electrolyte and its preparation method and application |
| CN111905783A (en) * | 2020-06-29 | 2020-11-10 | 复旦大学 | Molybdenum carbide/carbon nano hydrogen production catalyst synthesized by using ink |
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- 2022-03-21 CN CN202210278860.6A patent/CN114717570B/en active Active
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1507098A (en) * | 2002-12-12 | 2004-06-23 | ����Sdi��ʽ���� | Nano composite electrolytic solution film and fuel battery utilizing the same |
| US20140205909A1 (en) * | 2011-08-23 | 2014-07-24 | Nippon Shokubai Co., Ltd. | Negative electrode mixture or gel electrolyte, and battery using said negative electrode mixture or said gel electrolyte |
| CN109980302A (en) * | 2019-04-29 | 2019-07-05 | 中南大学 | A kind of water system Zinc ion battery colloidal electrolyte and its preparation method and application |
| CN111905783A (en) * | 2020-06-29 | 2020-11-10 | 复旦大学 | Molybdenum carbide/carbon nano hydrogen production catalyst synthesized by using ink |
Non-Patent Citations (1)
| Title |
|---|
| 李能等: "MXenes电催化析氢的研究进展", 《华中师范大学学报（自然科学版）》 * |
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