CN113026044A - Three-chamber two-power-supply full-decomposition water electrolysis device and method - Google Patents
Three-chamber two-power-supply full-decomposition water electrolysis device and method Download PDFInfo
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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
Abstract
The invention discloses a three-chamber two-power-supply full-decomposition water electrolysis device, which comprises a cylindrical electrolytic cell and two electrochemical workstations, wherein the cylindrical electrolytic cell is divided into three groups of fan-shaped electrolytic cells by three groups of partition plates, the three groups of electrolytic cells are respectively a chamber a, a chamber b and a chamber c, a working electrode and two reference electrodes are arranged in the chamber a, and a counter electrode is arranged in each of the chamber b and the chamber c; the working electrode adopts a copper oxide nano self-supporting electrode taking a copper wire as a substrate. The invention also discloses a using method of the device, the potential of the a-c loop is set to be any potential between +0.85 to + 1.25V; the potential of the a-b loop is set to any potential between 0.00 and + 0.21V. The device can generate hydrogen in the chamber c and oxygen in the chamber b. The invention breaks through the bottleneck that the high energy consumption is required for hydrogen production by industrial water electrolysis for many years, changes the design thought of the traditional water decomposition equipment and electrode, develops a brand new industrial water electrolysis design scheme, and saves a large amount of investment and operation cost for preparing hydrogen and oxygen by industrial water decomposition.
Description
Technical Field
The invention belongs to the technical field of hydrogen and oxygen preparation by decomposing water with a catalyst, and particularly relates to a three-chamber two-power-supply full-decomposition water electrolysis device and a method.
Background
The hydrogen gas has high heat value and no toxicity, and the product after combustion is water without pollution, so that the hydrogen gas is an ideal fossil energy substitute. Pure oxygen plays an important role in chemical industry such as steel making, national defense industry, medical care and other fields. Therefore, the realization of the preparation of hydrogen and oxygen by decomposing water with electric energy consumption is one of the first-choice ways of solving the energy crisis and reducing the cost of industrial fields and the like involving hydrogen/oxygen as fuel/raw materials.
At present, noble metals such as Pt, Ir and Ru, binary or ternary alloys thereof and oxides thereof are commonly used as anode materials in an electrolytic tank for industrially electrolyzing water, and some transition metals are infiltrated into the anode materials; in the cathode electrolytic cell, a noble metal (Pt, Ir, Ru), a platinum-chromium alloy, a platinum-iridium alloy, a platinum-nickel alloy, or the like is generally used as an electrode for producing hydrogen gas. The electrolytic device for preparing hydrogen and oxygen by fully hydrolyzing water disclosed mostly uses two-chamber electrolytic cells, one/group of cathodes and one/group of anodes are separated in two different electrolytic cells, a power supply is used for supplying power, and the required potential is more than 1.6V. If a non-noble metal material such as Fe is used, the required potential is higher. The higher water decomposition potential means that the energy consumption for preparing hydrogen and oxygen in unit volume is high, and the scarcity of noble metal materials is a bottleneck for restricting the large-scale industrial development of hydrogen production and oxygen production by water electrolysis. Therefore, the cheap non-noble metal oxide is utilized, a reasonable water electrolysis scheme is designed, the potential value of hydrogen and oxygen prepared by fully decomposing water is reduced, and the energy consumption of decomposing water is reduced, so that the method has immeasurable value in solving the global energy crisis and reducing the industrial production cost.
Disclosure of Invention
Aiming at the defects and difficult problems in the prior art, the invention aims to provide a three-chamber two-power-supply full-decomposition water electrolysis device and a method thereof.
The invention is realized by the following technical scheme:
the invention provides a three-chamber two-power supply full-decomposition water electrolysis device, which comprises a cylindrical electrolytic cell and two electrochemical work stations arranged in the cylindrical electrolytic cell, wherein the cylindrical electrolytic cell is divided into three groups of fan-shaped and isovolumetric electrolytic cells by three groups of partition plates positioned on radial lines, the three groups of electrolytic cells are respectively a chamber a, a chamber b and a chamber c, wherein a working electrode and two reference electrodes are arranged in the chamber a, and a counter electrode is respectively arranged in the chamber b and the chamber c; two electrochemical workstations are used as an electrolytic bath to supply power and control potential, one electrochemical workstation is respectively connected with a counter electrode, a working electrode and a reference electrode through electrode clamps, and 1.0mol/L NaOH aqueous solution is filled in the electrolytic bath as electrolytic solution; a counter electrode, a working electrode, a reference electrode and an electrochemical workstation electrically connected with the electrodes in the chamber b form an a-b loop; c, the counter electrode, the working electrode, the other reference electrode and the other electrochemical workstation electrically connected with the electrodes in the chamber form an a-c loop; the counter electrode adopts a graphite rod/sheet; the working electrode adopts a copper nano oxide self-supporting electrode taking a copper wire as a substrate; the reference electrode is a silver-silver chloride (Ag-AgCl) electrode.
Furthermore, the cylindrical electrolytic cell is made of glass or plastic, and the bottom and the side surface of the cylindrical electrolytic cell are integrated.
Furthermore, the partition plate is made of the same material as the main body of the cylindrical electrolytic cell, and a gap is reserved between the partition plate and the bottom of the cylindrical electrolytic cell.
Furthermore, a clamping groove is arranged at the bottom of the cylindrical electrolytic cell and is positioned below two sides of the partition plate, and a plugboard is arranged in the clamping groove and is a proton exchange membrane with a tetrafluoroethylene frame on the periphery.
The invention also provides a method for catalytically decomposing water by the three-chamber two-power full-decomposition water electrolysis device, which is used for supplying power to two groups of electrolysis loops to decompose water by a potentiostatic method with two different potential values; the potential of the electrochemical workstation in the a-b loop is set to be any potential between 0.00 and +0.21V, the high-valence transition metal compound on the working electrode on the a-b loop is reduced to be low-valence, and simultaneously O is arranged on the counter electrode2-Is oxidized to O2So that the chamber b generates oxygen; the potential of the electrochemical workstation in the a-c loop is set to be any potential between +0.85 to +1.25V, and the low valence transition metal compound on the working electrode on the a-c loopThe substance is oxidized while water decomposition is effected at the counter electrode, H+Is reduced to produce H2And chamber c produces hydrogen.
Further, the current density values of the a-c loop and the a-b loop are equal and the current signs are opposite, producing a molar ratio of hydrogen to oxygen of 2: 1.
Compared with the prior art, the invention has the beneficial effects that:
(1) the electrolysis potential of the three-chamber two-power supply full-decomposition water electrolysis device is +0.85 to +1.25V and 0.00 to +0.21V, the average potential is about 0.5V to realize full-decomposition water, and the potential is in the range of 1.6V-2.5V lower than that of the full-decomposition water reported by the current industry and literature; the electric potential required by the electrolyzed water is 1/3-1/5 required by the fully decomposed water which is publicly reported at present, which means that the consumed energy can be as low as 1/3-1/5 at present, the invention breaks through the bottleneck that the hydrogen production of the industrial electrolyzed water needs high energy consumption for many years, changes the design thought of the traditional water decomposition equipment and electrode, develops a brand new design scheme of the industrial electrolyzed water, and saves a large amount of investment and operation cost for preparing hydrogen and oxygen by the industrial decomposed water.
(2) The invention utilizes two groups of electrolysis loops with different potential values to simultaneously oxidize and reduce copper or other stable electrodes almost simultaneously, thereby avoiding the defect of instability caused by the catalytic production of hydrogen or oxygen by the transition metal oxide electrode under a constant potential in the prior art.
(3) The working electrode used in the invention is a transition metal nano oxide electrode, such as a copper oxide and a doped self-supporting electrode thereof, or other working electrodes with excellent conductivity and stability; the counter electrode used may be a graphite electrode. The traditional noble metal electrode is not used, a new solution is provided for the problem that the catalyst for decomposing water to prepare hydrogen and oxygen depends on noble metal, and a large amount of investment cost is saved for preparing hydrogen and oxygen by industrially decomposing water; meanwhile, the water can be continuously decomposed for 24 hours, so that the defect of instability caused by the fact that the transition metal oxide electrode in the prior art catalyzes hydrogen or oxygen to be produced under a constant potential is overcome.
(4) According to the method, hydrogen and oxygen are generated on the graphite electrode, the graphite electrode is high in stability and strong in gas impact resistance; the working electrode has no gas generation, thereby protecting the working electrode and prolonging the service life of the working electrode.
(5) The 2 counter electrodes in the device are respectively arranged in the 2 different chambers, and hydrogen and oxygen are respectively generated on the 2 counter electrodes (such as graphite rods/sheets), so that the effective separation of the hydrogen and the oxygen is realized, and the problem that the traditional transition metal oxide electrode generates a small amount of oxygen while preparing the hydrogen and brings difficulty to gas separation is avoided.
Drawings
FIG. 1 is a side expanded view of the device of the present invention.
FIG. 2 is a top view of the apparatus of the present invention.
Illustration of the drawings: 1-cylindrical electrolytic cell, 101-a chamber, 102-b chamber, 103-c chamber, 2 ' -counter electrode, 3-working electrode, 4 ' -reference electrode, 5-plug plate, 6-spacer, 7 ' -electrochemical workstation, 8-neck.
In the description of the present invention, the terms "center", "upper", "lower", "left", "right", "vertical", "horizontal", "inner", "outer", etc. indicate orientations or positional relationships based on those shown in the drawings, and are only for convenience of description and simplicity of description, but do not indicate or imply that the referred device or element must have a specific orientation, be constructed and operated in a specific orientation, and thus, should not be construed as limiting the present invention.
In the description of the present invention, it is to be noted that, unless otherwise explicitly specified or limited, the terms "mounted," "connected," and "connected" are to be construed broadly, and may be, for example, fixedly connected, detachably connected, and integrally connected; can be mechanical connection and electrical connection; may be directly connected, indirectly connected through intervening agents, or may be interconnected between two elements. The specific meaning of the above terms in the present invention can be specifically understood by those of ordinary skill in the art.
Detailed Description
The invention will be further described with reference to the accompanying drawings.
A method for water electrolysis by three-chamber two-power full decomposition, which comprises the steps of using an apparatus as shown in fig. 1 and fig. 2, comprising a cylindrical electrolytic cell 1, two electrochemical workstations 7 and 7 ' arranged outside the cylindrical electrolytic cell 1, two counter electrodes 2 and 2 ' arranged inside the cylindrical electrolytic cell 1, one working electrode 3, and two reference electrodes 4 and 4 '.
The cylindrical electrolytic cell 1 has the following structure:
(1) the cylindrical electrolytic cell 1 takes a cylindrical barrel made of glass or plastic as a main body, the cylindrical electrolytic cell 1 in the embodiment has the height of 0.2 m and the diameter of the bottom surface of 0.2 m, and the bottom and the side surface of the cylinder of the cylindrical electrolytic cell 1 are integrated into a whole, so that the air tightness is good;
(2) three groups of partition plates 6 positioned on radial lines are divided into three groups of fan-shaped electrolytic tanks with equal capacity, the three groups of electrolytic tanks are respectively a chamber 101, a chamber 102 and a chamber 103, the partition plates 6 are made of the same material as the main body of the cylindrical electrolytic tank 1, and a 0.03 meter gap is reserved between the partition plates 6 and the bottom of the cylindrical electrolytic tank 1 and used for exchanging solutions in each chamber;
(3) the bottom of the cylindrical electrolytic cell 1 is provided with a clamping groove 8, the clamping groove 8 is positioned below two sides of the partition plate 6, the clamping groove 8 is internally provided with a plugboard 5, the plugboard 5 is a proton exchange membrane with tetrafluoroethylene frames around, in the embodiment, the plugboard 5 is 0.095 m wide and 0.04 m long, the plugboard 5 can be just inserted into the clamping groove 8, so that liquid and gas in two adjacent chambers are separated, and only H is allowed+Freely enter and exit between the two chambers;
(4) a working electrode 3 and two reference electrodes 4 are placed in the chamber a 101, and a counter electrode 2 and 2' are placed in the chamber b 102 and the chamber c 103 respectively; 2 electrochemical workstations 7 and 7' are used as power supplies and potential is controlled; the electrochemical workstation 7 is respectively connected with the counter electrode 2, the working electrode 3 and the reference electrode 4 in sequence through electrode clamps; the electrochemical workstation 7 ' is connected with the counter electrode 2 ', the working electrode 3 and the reference electrode 4 ' in sequence through the electrode clamp respectively.
The working electrode 3 may be made of a material having good stability and electrical conductivity. If the self-supporting electrode is made by the prior art, the copper nano oxide self-supporting electrode is prepared by taking a copper wire as a substrate according to the method disclosed in the patent CN 109868485.
The counter electrodes 2 and 2' are made of graphite rods/sheets or other materials with strong conductivity and good stability. Reference electrodes 4, 4' employ silver-silver chloride (Ag-AgCl) electrodes. Because the counter electrode is usually made of a material with low value, good stability and excellent conductivity, such as graphite, the gas is generated on the surface of the counter electrode, and the gas is not generated on the surface of the working electrode 3, so that the working electrode 3 is protected from unstable influence caused by gas impact, and the stability of the working electrode in the device is good.
The specific catalytic water splitting method in this example:
filling 1.0mol/L NaOH aqueous solution into the electrolytic bath as electrolytic solution;
the counter electrode 2, the working electrode 3, the reference electrode 4 and the electrochemical workstation 7 connected with the electrodes in the b chamber 102 form a-b loop oxygen generation; a counter electrode 2 ', a working electrode 3, a reference electrode 4 ' and another electrochemical workstation 7 ' electrically connected with the electrodes in the c chamber 103 form an a-c loop for hydrogen production; two counter electrodes are respectively arranged in the chamber b and the chamber c to realize the effective separation of hydrogen and oxygen;
the constant potential method is utilized to respectively supply power to two groups of electrolysis loops to decompose water, wherein the potential of an electrochemical workstation 7 in an a-b loop is set to be any potential between 0.00 and +0.21V, the potential of an electrochemical workstation 7' in an a-c loop is set to be any potential between +0.85 and +1.25V, and the potential is far lower than the potential value between +1.6V and +2.5V required by the full decomposition of water reported by the industry and literature at present; if the potential of the a-b chamber is set at +0.1V and the potential of the a-c chamber is set at +0.9V in the present embodiment, all potentials are relative to the standard hydrogen potential; the current density values of the a-c loop and the a-b loop are equal, the current signs are opposite, and the molar ratio of hydrogen to oxygen generated is 2: 1.
In the embodiment, the working electrode 3 is exemplified by a copper oxide nanosheet self-supporting electrode, and the current density reaches 2000A/m under an alkaline condition2The hydrogen and oxygen prepared by continuously decomposing water can be more than 24 hours.
At constant potential, chamber b 102 produces oxygen and chamber c 103 produces hydrogen, at aIn the c circuit, the low-valent transition metal compound on the working electrode 3 is oxidized while water decomposition is carried out on the counter electrode, H+Is reduced to produce H2(ii) a In the a-b loop, the high valence transition metal compound on the working electrode 3 is reduced to low valence while O is on its counter electrode 22-Is oxidized to generate O2(ii) a In the a-c loop, the low-valence transition metal compound on the working electrode 3 is oxidized while H is on its counter electrode 2 ″+Is reduced to H2(ii) a Thus, continuous decomposition of water to produce hydrogen and oxygen was repeated, and the mechanism of water decomposition is shown in Table 1.
TABLE 1 mechanism of electrochemical two-circuit oxygen and hydrogen production (exemplified by copper oxide nanosheet self-supporting electrode)
The gas generated by each chamber was analyzed by gas chromatography.
The foregoing merely represents preferred embodiments of the invention, which are described in some detail and detail, and therefore should not be construed as limiting the scope of the invention. It should be noted that, for those skilled in the art, various changes, modifications and substitutions can be made without departing from the spirit of the present invention, and these are all within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.
Claims (6)
1. A three-chamber two-power-supply full-decomposition water electrolysis device, comprising a cylindrical electrolytic cell (1) and two electrochemical work stations (7, 7 '), wherein the cylindrical electrolytic cell (1) is divided into three groups of fan-shaped and equal-capacity electrolytic tanks by three groups of partition plates (6) located on radial lines, the electrolytic tanks are respectively an a chamber (101), a b chamber (102) and a c chamber (103), wherein one working electrode (3) and two reference electrodes (4, 4 ') are placed in the a chamber (101), and one counter electrode (2, 2 ') is placed in each of the b chamber (102) and the c chamber (103); the two electrochemical workstations (7, 7 ') are respectively used as the electrolytic bath to supply power and control the electric potentials of an a-b chamber and an a-c chamber, the electrochemical workstation (7) is respectively connected with the counter electrode (2), the working electrode (3) and the reference electrode (4) through electrode clamps, the electrochemical workstation (7') is connected with the counter electrode (2 '), the working electrode (3) and the reference electrode (4') through the electrode clamps, and 1.0mol/L NaOH aqueous solution is filled in the electrolytic bath to serve as an electrolytic solution; the counter electrode (2), the working electrode (3), the reference electrode (4) and the electrochemical workstation (7) in the b chamber (102) form an a-b loop; the counter electrode (2 '), the working electrode (3), the other reference electrode (4 ') and the other electrochemical workstation (7 ') in the c chamber (103) form an a-c circuit; the counter electrodes (2 and 2') adopt graphite rods/sheets; the working electrode (3) adopts a copper oxide nano self-supporting electrode; the reference electrodes (4 and 4') adopt silver-silver chloride electrodes.
2. The three-chamber two-power supply full decomposition water electrolysis device according to claim 1, wherein: the cylindrical electrolytic cell (1) is made of glass or plastic, and the bottom and the side face of the cylindrical electrolytic cell (1) are integrated.
3. The three-chamber two-power supply full decomposition water electrolysis device according to claim 2, wherein: the partition plate (6) is made of the same material as the main body of the cylindrical electrolytic cell (1), and a gap is reserved between the partition plate (6) and the bottom of the cylindrical electrolytic cell (1).
4. A three-chamber two-power full decomposition water electrolysis device as claimed in claim 3, wherein: cylindrical electrolytic tank (1) bottom installation draw-in groove (8), draw-in groove (8) are located division board (6) both sides below, installation picture peg (5) in draw-in groove (8), picture peg (5) are the proton exchange membrane that has the tetrafluoroethylene frame all around.
5. Method for catalytically decomposing water by using three-chamber two-power-supply full-decomposition water electrolysis device as claimed in any one of claims 1 to 4The method is characterized in that: the method comprises the steps of respectively supplying power to two groups of electrolysis loops by a potentiostatic method to decompose water; the potential of the electrochemical workstation (7) in the a-b loop is set to be any potential between 0.00 and +0.21V, the reduction reaction is generated on the working electrode (3) in the a-b loop, and simultaneously O on the counter electrode (2) of the electrochemical workstation2-Is oxidized to O2Such that the b chamber (102) produces oxygen; the potential of an electrochemical workstation (7) in the a-c loop is set to be any potential between +0.85 and +1.25V, the oxidation reaction is generated on a working electrode (3) in the a-c loop, and H is added into water on the counter electrode (2') of the a-c loop+Is reduced to produce H2Such that the c-chamber (103) produces hydrogen.
6. The three-chamber two-power full decomposition water electrolysis device catalytic decomposition water method according to claim 5, characterized in that: the current density values of the a-c loop and the a-b loop are equal, the current signs are opposite, and the molar ratio of the generated hydrogen to the generated oxygen is 2: 1.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN113088989A (en) * | 2021-03-23 | 2021-07-09 | 南昌大学 | Novel method for greatly reducing energy consumption of electrochemical decomposition of water by platinum |
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