CN214458365U - Electrolytic tank device for preparing sodium borohydride by direct current electrolytic method - Google Patents
Electrolytic tank device for preparing sodium borohydride by direct current electrolytic method Download PDFInfo
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- CN214458365U CN214458365U CN202120211590.8U CN202120211590U CN214458365U CN 214458365 U CN214458365 U CN 214458365U CN 202120211590 U CN202120211590 U CN 202120211590U CN 214458365 U CN214458365 U CN 214458365U
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- sodium borohydride
- cathode chamber
- direct current
- chamber
- anode
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- 239000012279 sodium borohydride Substances 0.000 title claims abstract description 36
- 229910000033 sodium borohydride Inorganic materials 0.000 title claims abstract description 36
- 238000000034 method Methods 0.000 title claims abstract description 17
- 238000005868 electrolysis reaction Methods 0.000 claims abstract description 38
- 239000012528 membrane Substances 0.000 claims abstract description 37
- 238000005341 cation exchange Methods 0.000 claims abstract description 12
- 238000002360 preparation method Methods 0.000 claims description 4
- 238000007789 sealing Methods 0.000 claims description 4
- 150000002500 ions Chemical class 0.000 abstract description 12
- 230000005684 electric field Effects 0.000 abstract description 6
- 238000010531 catalytic reduction reaction Methods 0.000 abstract description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 12
- 238000006722 reduction reaction Methods 0.000 description 10
- 229910052739 hydrogen Inorganic materials 0.000 description 9
- 239000001257 hydrogen Substances 0.000 description 9
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 8
- 238000012360 testing method Methods 0.000 description 8
- 230000009467 reduction Effects 0.000 description 7
- 238000002484 cyclic voltammetry Methods 0.000 description 6
- 230000006872 improvement Effects 0.000 description 6
- 239000000243 solution Substances 0.000 description 6
- 230000000694 effects Effects 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 4
- 239000000446 fuel Substances 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- 238000010586 diagram Methods 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 238000004064 recycling Methods 0.000 description 3
- NVIFVTYDZMXWGX-UHFFFAOYSA-N sodium metaborate Chemical compound [Na+].[O-]B=O NVIFVTYDZMXWGX-UHFFFAOYSA-N 0.000 description 3
- 239000011232 storage material Substances 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 2
- 239000010931 gold Substances 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- 239000002608 ionic liquid Substances 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 230000008929 regeneration Effects 0.000 description 2
- 238000011069 regeneration method Methods 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 229920000557 Nafion® Polymers 0.000 description 1
- 229910001069 Ti alloy Inorganic materials 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 239000010405 anode material Substances 0.000 description 1
- 230000002146 bilateral effect Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 238000006477 desulfuration reaction Methods 0.000 description 1
- 230000023556 desulfurization Effects 0.000 description 1
- 230000003009 desulfurizing effect Effects 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000002848 electrochemical method Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000000295 fuel oil Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 239000003014 ion exchange membrane Substances 0.000 description 1
- RPZHFKHTXCZXQV-UHFFFAOYSA-N mercury(i) oxide Chemical compound O1[Hg][Hg]1 RPZHFKHTXCZXQV-UHFFFAOYSA-N 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 238000001308 synthesis method Methods 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 238000009827 uniform distribution Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
The utility model discloses an electrolytic tank device for preparing sodium borohydride by a direct current electrolytic method, which comprises a cathode chamber and anode chambers symmetrically arranged at two sides of the cathode chamber; the cathode chamber is communicated with the anode chambers on the two sides through a connecting pipe; or the cathode chamber and the anode chamber are connected through a branch pipe integrally connected at the side surface; the device also comprises a cation exchange membrane arranged on the cross section of the joint of the cathode chamber and the anode chamber. The utility model discloses the structure of two membrane three room electrolysis trough that adopts can form the electric field of evenly distributed in the negative pole left and right sides to reduce the electric field to the influence of metaborate ion electromigration, improve the electrolysis catalytic reduction probability of metaborate ion and negative pole, improve electrolysis efficiency.
Description
Technical Field
The utility model belongs to the field of hydrogen storage material manufacturing, in particular to an electrolytic cell device for preparing sodium borohydride by a direct current electrolytic method.
Background
Sodium borohydride is an excellent hydrogen storage material, the hydrogen storage density of the sodium borohydride can reach 10.8 wt%, the regenerated product is pollution-free, the hydrogen release purity is high, and the sodium borohydride is an ideal hydrogen source for fuel cells, and the sodium borohydride is a promising candidate hydrogen storage material in Proton Exchange Membrane Fuel Cells (PEMFC) and Direct Borohydride Fuel Cell (DBFC) systems, but the sodium borohydride is expensive, the hydrogen production cost is too high, the regeneration is difficult, and the development of the sodium borohydride is restricted by the problems of the need of a noble metal catalyst and the like.
The prior preparation method of sodium borohydride comprises an industrial synthesis method, a direct reduction method and the like. Compared with other methods, the electrochemical reduction method for preparing the sodium borohydride can realize the on-line preparation of the sodium borohydride and the recycling of hydrogen production stored by the sodium borohydride, and has the advantages of low raw material cost, low energy consumption and simple operation. U.S. Pat. No. 3,3734842 discloses a process for synthesizing borohydride by electrolysis, which does not need to add a reducing agent, reduces the production cost, but has low electrolysis efficiency and no recycling. Chinese patent CN1239748C discloses a method for recycling sodium borohydride fuel cell, which decomposes borohydride to generate metaborate, a byproduct of hydrogen, by using electrolysis, and regenerates borohydride, but the reaction rate of the process is slow, and titanium alloy is used as anode material, which is expensive. Shuchenhua patent publication No. CN110457461A discloses a NaBH-based catalyst4The fuel oil extraction-reduction desulfurizing method of electrochemical regeneration combines sodium borohydride reduction and reduction desulfurization, sodium metaborate and ionic liquid are added into a working electrode electrolytic cell, the ionic liquid is added into a counter electrode electrolytic cell, and the sodium borohydride is obtained by electrolysis by applying pulse voltage.
The utility model adopts an electrochemical method to prepare sodium borohydride, but BO is adopted in the preparation process2 -The negative ions will move towards the anode, causing BO near the cathode2 -Decrease in ion concentration, resulting in BO2 -Reduction of ions to BH4 -The ions are very difficult, although reduction to BH still occurs at the cathode4 -Ion, BH4 -The ions will also move from the anode surfaceAnd the oxidation reaction occurs and is consumed, thereby reducing the electrolytic reduction efficiency. The BO can be effectively blocked by installing an ion exchange membrane between the cathode and the anode2 -And BH4 -Ion migration to the anode to promote BO2 -Reduction to BH4 -. Therefore, during the electrolysis process, the cathode chamber and the anode chamber need to be isolated by a Nafion membrane.
NaBH from currently used single-membrane two-compartment cell devices4Low concentration, low conversion rate, large electricity demand and is still not suitable for preparing NaBH4The industrial requirements of (1).
SUMMERY OF THE UTILITY MODEL
Aiming at the problem that the prior electrolytic cell device can not efficiently improve NaBH4The utility model provides an electrolytic cell device with a two-membrane three-chamber structure for preparing sodium borohydride by a direct current electrolytic method.
Realize above-mentioned technical purpose, reach above-mentioned technological effect, the utility model discloses a following technical scheme realizes:
an electrolytic cell device for preparing sodium borohydride by a direct current electrolytic method comprises a cathode chamber and anode chambers symmetrically arranged on two sides of the cathode chamber;
the cathode chamber is communicated with the anode chambers at two sides through a connecting pipe;
or the cathode chamber and the anode chamber are connected through a branch pipe integrally connected at the side surface;
the device also comprises a cation exchange membrane arranged on the cross section of the joint of the cathode chamber and the anode chamber.
As a further improvement of the utility model, the main body chambers of the anode chambers on both sides have the same size and are arranged in mirror images of the connected branch pipes.
As a further improvement of the utility model, the bilateral symmetry of the cathode chamber is provided with a group of branch pipes.
As a further improvement of the utility model, the cation exchange membrane is arranged at the position of the junction surface of the branch pipe.
As a further improvement of the utility model, a sealing ring is arranged at the position corresponding to the position of the cation exchange membrane.
As a further improvement of the utility model, two sides the anode in the anode chamber is connected with the same cathode in the cathode chamber, and the direct current power supply with the same load is loaded between the anode and the cathode.
As a further improvement of the utility model, the device also comprises an electrochemical workstation connected with the direct current power supply.
The utility model has the advantages that: the utility model discloses the structure of two membrane three room electrolysis baths that adopts can form the electric field of balanced distribution in the negative pole left and right sides to reduce the electric field to the influence of metaborate ion electromigration, improve the electro-catalytic reduction probability of metaborate ion and negative pole, improve electrolysis efficiency.
Drawings
FIG. 1 is a schematic diagram of the distribution of the structure of the electrolytic cell of the present invention;
FIG. 2 is a schematic view of the operation principle of the electrolytic cell of the present invention;
FIG. 3 is a schematic structural view of a first embodiment of the electrolytic cell of the present invention;
FIG. 4 is a schematic structural view of a second embodiment of the electrolytic cell of the present invention;
FIG. 5 is a cyclic voltammogram of the two-membrane three-compartment cell of example 1 at 4v for various times of electrolysis;
FIG. 6 is a cyclic voltammogram of a single-membrane two-compartment cell in comparative example 1 at an electrolysis voltage of 4v for various times of electrolysis;
FIG. 7 is a graph comparing the peak current densities of two-membrane three-chamber cells and a single-membrane two-chamber cell during electrolysis for different periods of time;
FIG. 8 is a cyclic voltammogram at different electrolysis voltages for a two-membrane three-chamber electrolyzer having an electrolysis time of 30min in example 2;
FIG. 9 is a cyclic voltammogram of a single-membrane two-compartment cell of comparative example 2 at different electrolysis voltages for an electrolysis time of 30 min;
FIG. 10 is a comparison of peak current densities for different voltages for two-membrane three-chamber cells and for single-membrane two-chamber cells;
wherein: 1-cathode chamber, 2-anode chamber, 100, 200-branch pipe, 3-cation exchange membrane, 4-cathode, 5-anode, 6-direct current power supply, 7-connecting pipe and 8-sealing ring.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail with reference to the following embodiments. It should be understood that the specific embodiments described herein are for purposes of illustration only and are not intended to limit the invention.
The following description is made in detail for the application of the principles of the present invention with reference to the accompanying drawings.
The structure schematic diagram of the two-membrane three-chamber electrolyzer shown in fig. 1-3 of the present invention comprises a cathode chamber 1 and anode chambers 2 symmetrically disposed at both sides of the cathode chamber 1, wherein the cathode chamber 1 and the anode chambers 2 are connected in the following two ways.
The first connection mode is as follows: the cathode chamber 1 is communicated with the anode chambers 2 at two sides through a connecting pipe.
And a second connection mode: the cathode chamber 1 and the anode chamber 2 are connected by branch pipes 100 and 200 integrally connected at the side surfaces.
In addition, the device also comprises a cation exchange membrane 3 arranged on the cross section of the joint of the cathode chamber 1 and the anode chamber 2. Thereby forming the structure of the two-membrane three-chamber electrolytic cell.
In addition, for the second connection mode cathode chamber 1, the anode chamber 2 is structured as follows: the body chambers of the anode chambers 2 located at both sides have the same size, and the branch pipes 200 connected thereto are arranged in a mirror image. A set of branch pipes 100 are symmetrically arranged on both sides of the cathode chamber 1. The cation exchange membrane 3 is provided at the position of the junction surface of the branch pipes. And a sealing ring 8 is arranged at the position corresponding to the position where the cation exchange membrane 3 is arranged.
Based on the container device, the connected electrode device has the specific structure that an anode 5 in the anode chamber 2 is connected with the same cathode 4 in the cathode chamber 1, and a direct current power supply 6 with the same load is loaded between the anode 5 and the cathode 4. Two electrolytic cells are produced in series, which are connected in parallel and share the same cathode chamber 1. The electrode is fixed inside the electrolytic cell device through the electrode fixing hole position of the cathode chamber 1 or the anode chamber 2. As can be seen from fig. 2, the left and right sides of the electrodes in the cathode chamber 1 form the electric fields with uniform distribution, so that the influence of the electric fields on the electromigration of the metaborate ions and the periphery of the metaborate ion aggregation exchange membrane are reduced, the probability of electrolytic catalytic reduction of the metaborate ions and the cathode is improved, the working voltage can be effectively reduced, and the electrolytic efficiency is improved.
As shown in fig. 3, a specific embodiment of the present invention is made of organic glass, and is composed of a left 50ml anode chamber, a right 50ml anode chamber and a middle 50ml cathode chamber 1, each chamber is connected by a connecting pipe 7, and a cation exchange membrane 3 is arranged in parallel with the cross section of the connecting pipe 7; the anode chamber is provided with a cover plate for fixing an anode and a counter electrode, and the cathode chamber 1 is provided with a cover plate for fixing a cathode.
The following is the embodiment of the utility model completed by testing:
in the embodiments, a three-electrode system is adopted, a gold electrode is used as a working electrode, a graphite electrode is used as a counter electrode, a mercury-mercury oxide electrode is used as a reference electrode, left-right symmetry is ensured, and then the three-electrode system is connected with an electrochemical workstation. The electrochemical workstation used in the present invention is a CHI660B electrochemical workstation manufactured by shanghai chenhua instruments.
The specific tests are as follows:
the first embodiment is as follows:
50ml of lmol/L NaOH solution is added into two anode chambers of the electrolytic cell, and 50ml of lmol/L NaOH solution and 0.5mol/L sodium metaborate mixed solution are added into a cathode chamber 1.
Carrying out direct current electrolysis at normal temperature and normal pressure, wherein the electrolysis voltage is 4v, and testing the sodium borohydride concentration of the solution after 30, 90, 120, 150, 180, 210, 240, 270 and 300min of electrolysis under the voltage respectively; the test is carried out by adopting cyclic voltammetry, the test voltage range is-1 v, the scanning speed is 0.05v/s, and as can be seen from the peak current of figure 5, the peak current is the maximum at the time of electrolysis for 270min and is 14.46 multiplied by 10-4A·cm-2At this time, the concentration of sodium borohydride was the highest.
Comparative example one:
for comparison with the present invention, a single membrane two-compartment cell was used to compare the same raw materials and procedures as in example 1. The single-membrane two-chamber electrolytic cell is divided into an anode chamber and a cathode chamber, NaOH solution is added into the anode chamber, mixed solution of NaOH and sodium metaborate is added into the cathode chamber, and direct current electrolysis is carried out at normal temperature and normal pressure. FIG. 6 is a CV diagram of the electrolyzed water in a single-membrane two-chamber electrolyzer, showing that the peak current density at 300min of electrolysis time is 7.136X 10-4A·cm-2At this time, the concentration of sodium borohydride was the highest.
FIG. 7 is a comparison graph of peak current densities at different times after electrolysis in the two-membrane three-chamber electrolyzer and the single-membrane two-chamber electrolyzer, and it can be seen that the electrolysis effect of the three chambers is better than that of the two chambers.
Example two:
the electrolyte concentration was the same as in example one.
Carrying out direct current electrolysis at normal temperature and normal pressure, wherein the electrolysis voltage is 1.5v and 4v respectively, and testing the concentration of sodium borohydride in the solution after 30min of electrolysis at each voltage; the test method is to use a gold electrode as a cathode to perform cyclic voltammetry test, the test voltage range is-1 v, the scanning speed is 0.05v/s, and as can be seen from the peak current in FIG. 8, the peak current is the largest when the electrolytic voltage is 1.5v, and is 7.521 multiplied by 10-4A·cm-2At this time, the concentration of sodium borohydride was the highest.
Comparative example two:
a single membrane two-compartment cell was used to compare the same raw materials and procedures as in example 1. As can be seen from FIG. 9, the electrolysis effect was the best when the electrolysis voltage was 1.5v, and the peak current density was 3.398X 10-4A·cm-2At this time, the concentration of sodium borohydride was the highest.
Fig. 10 is a comparison graph of peak current densities at different voltages after electrolysis in the two-membrane three-chamber electrolyzer and the single-membrane two-chamber electrolyzer, which shows that the three-chamber electrolyzer has better electrolysis effect than the two-chamber electrolyzer, and in general, the three-chamber electrolyzer has better effect in reduction of sodium borohydride than the traditional two-chamber electrolyzer.
The basic principles and the main features of the invention and the advantages of the invention have been shown and described above. It will be understood by those skilled in the art that the present invention is not limited to the above embodiments, and that the foregoing embodiments and descriptions are provided only to illustrate the principles of the present invention without departing from the spirit and scope of the present invention. The scope of the invention is defined by the appended claims and equivalents thereof.
Claims (7)
1. An electrolytic cell device for preparing sodium borohydride by a direct current electrolytic method is characterized in that: comprises a cathode chamber and anode chambers symmetrically arranged at two sides of the cathode chamber;
the cathode chamber is communicated with the anode chambers at two sides through a connecting pipe;
or the cathode chamber and the anode chamber are connected through a branch pipe integrally connected at the side surface;
the device also comprises a cation exchange membrane arranged on the cross section of the joint of the cathode chamber and the anode chamber.
2. An electrolytic cell apparatus for producing sodium borohydride by direct current electrolysis according to claim 1, wherein: the main body chambers of the anode chambers located at both sides have the same size, and branch pipes connected thereto are arranged in a mirror image.
3. An electrolytic cell apparatus for producing sodium borohydride by direct current electrolysis according to claim 2, wherein: a group of branch pipes are symmetrically arranged on two sides of the cathode chamber.
4. An electrolytic cell apparatus for producing sodium borohydride by direct current electrolysis according to claim 1, wherein: the cation exchange membrane is arranged at the position of the joint surface of the branch pipe.
5. An electrolytic cell apparatus for producing sodium borohydride by direct current electrolysis according to claim 4, wherein: and a sealing ring is arranged at the position corresponding to the position where the cation exchange membrane is arranged.
6. An electrolytic cell apparatus for producing sodium borohydride by direct current electrolysis according to claim 1, wherein: anodes in the anode chambers on two sides are connected with the same cathode in the cathode chamber, and direct current power supplies with the same load are loaded between the anodes and the cathodes.
7. The electrolyzer apparatus for the preparation of sodium borohydride according to claim 6, characterized in that: and the electrochemical workstation is connected with the direct current power supply.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202120211590.8U CN214458365U (en) | 2021-01-26 | 2021-01-26 | Electrolytic tank device for preparing sodium borohydride by direct current electrolytic method |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202120211590.8U CN214458365U (en) | 2021-01-26 | 2021-01-26 | Electrolytic tank device for preparing sodium borohydride by direct current electrolytic method |
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| Publication Number | Publication Date |
|---|---|
| CN214458365U true CN214458365U (en) | 2021-10-22 |
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| CN202120211590.8U Expired - Fee Related CN214458365U (en) | 2021-01-26 | 2021-01-26 | Electrolytic tank device for preparing sodium borohydride by direct current electrolytic method |
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| CN (1) | CN214458365U (en) |
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2021
- 2021-01-26 CN CN202120211590.8U patent/CN214458365U/en not_active Expired - Fee Related
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| GR01 | Patent grant | ||
| GR01 | Patent grant | ||
| TR01 | Transfer of patent right | ||
| TR01 | Transfer of patent right |
Effective date of registration: 20221108 Address after: 230031 Room 539, Block A, Building J2, Phase II, Innovation Industrial Park, No. 2800, Innovation Avenue, Free Trade Pilot Zone, Hefei Hi tech Zone, Anhui Province Patentee after: China National Hydrogen (Anhui) Technology Co.,Ltd. Address before: 221200 Anlan Avenue East and Linkong Avenue North, Airport Economic Development Zone, Suining County, Xuzhou City, Jiangsu Province Patentee before: Xuzhou Aviation Materials Research Institute Co.,Ltd. |
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| CF01 | Termination of patent right due to non-payment of annual fee | ||
| CF01 | Termination of patent right due to non-payment of annual fee |
Granted publication date: 20211022 |