CN112133990B - Metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction - Google Patents
Metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction Download PDFInfo
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- CN112133990B CN112133990B CN202011031933.9A CN202011031933A CN112133990B CN 112133990 B CN112133990 B CN 112133990B CN 202011031933 A CN202011031933 A CN 202011031933A CN 112133990 B CN112133990 B CN 112133990B
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Abstract
The invention discloses a metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction, which consists of negative electrolyte, positive electrolyte, a negative (anode) metal plate, an ion semipermeable membrane, a graphite electrode, a breather pipe and an air pump. The metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction disclosed by the invention has the advantages that the balance potential of the electrochemical reduction reaction is higher, the discharge voltage and the discharge current density are higher than those of the traditional catalyst type metal-air battery, and the problem of low oxygen electrochemical reduction reaction speed in the traditional air battery is solved. The electrolyte and the graphite electrode of the battery are extremely stable, the problems of poisoning, decomposition and reduction of catalytic efficiency do not exist, and the preparation material is cheap and easy to obtain, low in cost and environment-friendly. And the electrolyte and the electrode can be regenerated, the replacement is convenient and rapid, the use is safe, and the application prospect and the use value are good.
Description
Technical Field
The invention relates to the field of new energy, in particular to a metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction.
Background
The metal-air battery uses active metal as a negative electrode (anode) and oxygen as a chemical power supply of a positive electrode (cathode), but because the partial pressure of oxygen in the air is only 21 percent, and the discharge can be realized through the steps of adsorption, diffusion and liquid-phase electrochemical reduction, the diffusion path is long, the oxygen electrochemical reduction reaction speed is slow, the overpotential of the oxygen ionization and reduction reaction is high, so that the traditional metal-air battery has low discharge voltage, small discharge current and insufficient working capacity.
Therefore, the anode of the traditional metal-air battery usually adopts noble metal catalysts such as platinum and palladium as electrode materials to accelerate the electrochemical oxidation of oxygenChemical reduction reaction rate (discharge rate). However, the noble metal catalyst has poor stability, catalytic activity is difficult to maintain for a long time, and the cost is very high, so that the noble metal catalyst is difficult to apply on a large scale. In addition, a metal oxide catalyst (such as oxides of valence-variable metals including Mn, Co, and Fe) can be used as the positive electrode material, but the metal oxide catalyst is not as active as a noble metal catalyst and is likely to react with Co in the air2The activity is lost due to toxic reaction, the service life is short and the stability is insufficient; meanwhile, some metal oxide catalysts contain heavy metals, so that the environment is polluted, the preparation is complex, and the cost is higher.
Disclosure of Invention
In order to solve the technical problems, the invention provides a metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction, which comprises a negative electrode electrolyte, a positive electrode electrolyte, a negative electrode (anode) metal plate, an ion semi-permeable membrane, a graphite electrode, a vent pipe and an air pump;
the negative electrode (anode) metal plate is immersed in a negative electrode electrolyte;
the graphite electrode is immersed in the positive electrolyte;
the negative electrolyte and the positive electrolyte are separated by an ion semipermeable membrane;
one end of the vent pipe is immersed in the anode electrolyte, and the other end of the vent pipe is connected with the air pump.
Further, the negative electrode electrolyte of the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) is one of degassed sodium chloride or potassium chloride solutions.
Further, the concentration of the negative electrode electrolyte of the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) is 1mol/L to saturation.
Further, the positive electrode electrolyte of the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) is acidic soluble Fe with the pH value less than 33+The ionic solution is acidic. When the pH of the positive electrolyte is less than 3, Fe can be effectively prevented3+The ions are hydrolyzed, which is beneficial to the stability of the battery.
Further, the concentration of the positive electrode electrolyte of the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) is 0.5mol/L to saturation.
Further, the positive electrode electrolyte of the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) is one or more of ferric nitrate, ferric chloride or ferric sulfate.
Furthermore, the material of the negative electrode metal of the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) is one of magnesium, aluminum, zinc and iron.
Furthermore, the semipermeable membrane of the metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction is one of an anionic semipermeable membrane, a cationic semipermeable membrane and a mixed semipermeable membrane.
Further, the graphite electrode of the metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction is one of a carbon plate or a carbon felt electrode
Further, the breather pipe of the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) does not react with acid and alkali.
When the metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction discharges outwards (does work), the negative metal plate loses electrons, becomes metal ions, enters a negative electrolyte, and becomes a precipitate through hydrolysis; electrons flow into the graphite plate or graphite felt of the anode through the electric appliance, and Fe in the electrolyte of the anode3+The ions gain electrons on the graphite electrode and are reduced into Fe2+Ions.
The air vent pipe and the air pump are used for continuously or intermittently aerating the electrolyte in the positive electrode area when necessary so as to lead Fe2+Regeneration of ions to Fe3+Ions, thereby the positive electrode Fe can be maintained3+The concentration of the ions ensures the long-term stability of the discharge voltage and the discharge current of the battery (improves the continuous discharge work capability of the battery).
Negative electrode reaction formula: m-ne → Mn+
In the formula: m is a metal; mn+Is a metal positive ion; e is an electron.
Positive electrode reaction formula: fe3++e→Fe2+
The metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) can be regenerated (charged) after the discharge. During regeneration, the anode electrolyte system can be directly exposed to the air, and the oxygen in the air can directly oxidize Fe through chemical oxidation2+Oxidation of ions to Fe3+Ions while consuming H in the positive electrolyte+Ions. If the regeneration speed of the positive electrolyte is increased, air can be continuously or intermittently pumped by using an air pump. Although the oxygen in the air has a slow electrochemical reduction reaction speed and a high ionization overpotential, the oxygen chemically oxidizes Fe2+The ion time rate is extremely high, mainly because the step of oxygen ionization is omitted and the influence of equilibrium potential is avoided, the rapid regeneration of the anode electrolyte can be realized; the regeneration of cathode material can be carried out by directly replacing the consumed cathode metal plate, and the cathode electrolyte solution is low-value sodium chloride or potassium chloride solution which can be directly replaced. Meanwhile, when the battery is maintained, a proper amount of acid liquor can be added into the electrolyte of the positive electrode.
The positive electrode electrolyte regeneration reaction formula: 4Fe2++O2+4H+→2H2O+4Fe3+
The metal-air battery based on the Fe (II)/Fe (III) chemical oxidation and electrochemical reduction can realize the enhancement of the continuous discharge capability of the battery by continuously introducing air into the positive electrolyte in the discharge process of the battery, and can also supplement the metal plate material consumed by the negative electrode and the negative electrolyte at any time to realize the uninterrupted stable power supply of the battery.
Compared with the prior art, the invention has the beneficial technical effects that:
(1) the invention relates to Fe of a metal-air battery based on chemical oxidation and electrochemical reduction of Fe (II)/Fe (III)3+The equilibrium potential of the ionic electrochemical reduction reaction is higher (the potential of a hydrogen standard electrode is 0.771V), and a higher anode potential and a higher battery voltage can be obtained after the battery is formed.
(2) The invention relates to a chemical oxidation and electrochemical reduction method based on Fe (II)/Fe (III)Original metal-air battery Fe3+The ion concentration far exceeds the dissolved concentration of oxygen in air in the water-based electrolyte and is along with Fe3+The increase in ion concentration may further increase the discharge voltage of the metal-air battery.
(3) The invention relates to Fe of a metal-air battery based on chemical oxidation and electrochemical reduction of Fe (II)/Fe (III)3+The ion diffusion speed and the electrochemical reduction reaction speed are higher than those of oxygen (the discharge rate is higher), and the battery can keep higher discharge voltage under the condition of larger discharge current. Therefore, the open-circuit voltage, the discharge voltage and the discharge current density of the battery are higher than those of the traditional catalyst type metal-air battery.
(4) The invention relates to Fe of a metal-air battery based on chemical oxidation and electrochemical reduction of Fe (II)/Fe (III)3+Electrochemical reduction of ions, and oxygen on Fe2+The chemical oxidation reaction of the ions is fast, and the combination of the ions and the ions solves the problem of slow oxygen electrochemical reduction reaction speed in the traditional air battery.
(5) The metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) can utilize oxygen in air to react with Fe3+Fe produced by reduction of ions2+The ions are chemically oxidized to rapidly generate Fe again3+Ions, maintaining the reaction capability of the positive electrolyte system.
(6) The Fe used for the positive electrode of the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) is Fe3+The ionic electrolyte and the graphite electrode are extremely stable, the problems of poisoning, decomposition and reduction of catalytic efficiency do not exist, and the long-term stable operation can be realized.
(7) All materials selected by the metal-air battery based on the chemical oxidation and electrochemical reduction of Fe (II)/Fe (III) are cheap and easily-obtained substances, the cost is extremely low, the metal-air battery is environment-friendly, the negative electrolyte can be directly discharged, and the positive electrolyte can be harmlessly discharged after acid-base neutralization.
(8) The metal air battery anode and cathode electrolyte and the electrode based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction can be regenerated, are convenient and quick to replace, and do not have the risks of combustion, explosion and the like even if short circuit occurs.
Drawings
The invention is further illustrated in the following description with reference to the drawings.
Fig. 1 is a schematic structural diagram of a metal-air battery based on chemical oxidation and electrochemical reduction of Fe (ii)/Fe (iii) according to the present invention.
Description of reference numerals: the air pump comprises a negative electrode electrolyte, a positive electrode electrolyte, a negative electrode (anode) metal plate, an ion semipermeable membrane, a graphite electrode, a breather pipe and an air pump.
FIG. 2 shows a conventional MnO2Catalyst air-metal cell open circuit voltage.
FIG. 3 shows a conventional MnO2Catalyst air-metal battery cell discharge voltage-current.
FIG. 4 shows different concentrations of Fe3+Open circuit voltage of air-metal battery cell.
FIG. 5 shows different concentrations of Fe3+Air-metal battery cell discharge voltage-current.
Detailed Description
Example 1
Immersing an industrial pure aluminum metal plate into a degassing saturated sodium chloride solution to obtain a negative electrode of the battery;
immersing a graphite felt electrode into 0.5mol/L acidic ferric nitrate solution to obtain a positive electrode of the battery;
the negative electrolyte and the positive electrolyte are separated by an anion semipermeable membrane;
one end of the vent pipe is immersed in the anode electrolyte, and the other end of the vent pipe is connected with an air pump to form the metal air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction.
The discharge performance of the battery is tested, the open-circuit voltage is 1.33V, and the maximum discharge current density is 70mA multiplied by cm-2。
Example 2
Immersing an industrial pure aluminum metal plate into a 3mol/L degassed sodium chloride solution to obtain a cathode of the battery;
immersing the graphite felt electrode into 1mol/L acidic ferric sulfate solution to obtain the anode of the battery;
the negative electrolyte and the positive electrolyte are separated by an anion semipermeable membrane;
one end of the vent pipe is immersed in the anode electrolyte, and the other end of the vent pipe is connected with an air pump to form the metal air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction.
The discharge performance of the battery is tested, the open-circuit voltage is 1.41V, and the maximum discharge current density is 80mA multiplied by cm-2。
Example 3
Immersing an industrial pure aluminum metal plate into a 2mol/L degassed sodium chloride solution to obtain a cathode of the battery;
immersing a graphite felt electrode into 2mol/L acidic ferric chloride solution to obtain a positive electrode of the battery;
the negative electrolyte and the positive electrolyte are separated by an anion semipermeable membrane;
one end of the vent pipe is immersed in the anode electrolyte, and the other end of the vent pipe is connected with an air pump to form the metal air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction.
The discharge performance of the battery is tested, the open-circuit voltage is 1.41V, and the maximum discharge current density is 80mA multiplied by cm-2。
Example 4
Immersing an industrial pure iron metal plate into a degassing saturated potassium chloride solution to obtain a negative electrode of the battery;
immersing a graphite plate electrode into 0.5mol/L acidic ferric nitrate solution to obtain a positive electrode of the battery;
the negative electrolyte and the positive electrolyte are separated by a sodium polyacrylate ion semipermeable membrane;
one end of the vent pipe is immersed in the anode electrolyte, and the other end of the vent pipe is connected with an air pump to form the metal air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction.
The discharge performance of the battery is tested, the open-circuit voltage is 1.03V, and the maximum discharge current density is 50mA multiplied by cm-2。
Example 5
Immersing an industrial pure iron metal plate into a degassed potassium chloride solution of 3mol/L to obtain a negative electrode of the battery;
immersing a graphite plate electrode into 1mol/L acidic ferric sulfate solution to obtain a positive electrode of the battery;
the negative electrolyte and the positive electrolyte are separated by a sodium polyacrylate ion semipermeable membrane;
one end of the vent pipe is immersed in the anode electrolyte, and the other end of the vent pipe is connected with an air pump to form the metal air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction.
The discharge performance of the battery is tested, the open-circuit voltage is 1.05V, and the maximum discharge current density is 58mA multiplied by cm-2。
Example 6
Immersing an industrial pure iron metal plate into a degassed 2mol/L potassium chloride solution to obtain a cathode of the battery;
immersing a graphite plate electrode into 2mol/L acidic ferric chloride solution to obtain a positive electrode of the battery;
the negative electrolyte and the positive electrolyte are separated by a sodium polyacrylate ion semipermeable membrane;
one end of the vent pipe is immersed in the anode electrolyte, and the other end of the vent pipe is connected with an air pump to form the metal air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction.
The discharge performance of the battery is tested, the open-circuit voltage is 1.12V, and the maximum discharge current density is 40mA multiplied by cm-2。
The above-described embodiments are merely illustrative of the preferred embodiments of the present invention, and do not limit the scope of the present invention, and various modifications and improvements of the technical solutions of the present invention can be made by those skilled in the art without departing from the spirit of the present invention, and the technical solutions of the present invention are within the scope of the present invention defined by the claims.
Claims (6)
1. A metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction is characterized by comprising a negative electrode electrolyte (1), a positive electrode electrolyte (2), a negative electrode metal plate (3), an ion semipermeable membrane (4), a graphite electrode (5), a vent pipe (6) and an air pump (7);
the negative electrode metal plate (3) is immersed in the negative electrode electrolyte (1);
the graphite electrode (5) is immersed in the anode electrolyte (2);
the negative electrolyte (1) and the positive electrolyte (2) are separated by an ion semipermeable membrane (4);
one end of the vent pipe (6) is immersed in the anode electrolyte (2), and the other end of the vent pipe is connected with the air pump (7);
the negative electrode electrolyte is one of degassed sodium chloride or potassium chloride solution;
the concentration of the negative electrode electrolyte (1) is 1mol/L to saturation;
the positive electrolyte (2) is soluble Fe with pH less than 33+An ionic solution;
the concentration of the positive electrode electrolyte (2) is 0.5mol/L to saturation.
2. A metal-air battery based on Fe (ii)/Fe (iii) chemical oxidation and electrochemical reduction according to claim 1, characterized in that the positive electrolyte (2) is one or several of ferric nitrate, ferric chloride or ferric sulfate.
3. The metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction of claim 1, wherein the material of the negative electrode metal plate (3) is one of magnesium, aluminum, zinc and iron.
4. The metal-air battery based on Fe (II)/Fe (III) chemical oxidation and electrochemical reduction according to claim 1, wherein the ionic semipermeable membrane (4) is one of an anionic semipermeable membrane, a cationic semipermeable membrane, and a mixed type semipermeable membrane.
5. A metal-air cell based on Fe (ii)/Fe (iii) chemical oxidation and electrochemical reduction according to claim 1, characterized in that the graphite electrode (5) is one of a carbon plate or carbon felt electrode.
6. The metal-air cell based on Fe (ii)/Fe (iii) chemical oxidation and electrochemical reduction of claim 1, wherein the breather tube does not react with an acid or base.
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| EP3291361A1 (en) * | 2016-09-02 | 2018-03-07 | Helmholtz-Zentrum Geesthacht Zentrum für Material- und Küstenforschung GmbH | Electrolyte additives for magnesium air batteries |
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| JPS544332A (en) * | 1977-06-13 | 1979-01-13 | Matsushita Electric Ind Co Ltd | Alkaline cell |
| CN101714680A (en) * | 2008-10-07 | 2010-05-26 | 中国人民解放军63971部队 | Rechargeable metal-air redox flow battery combining electrochemical preparation |
| CN102881961B (en) * | 2012-09-27 | 2014-08-06 | 合肥工业大学 | Method of using single-chamber fuel cell for treatment of sulfur containing wastewater, recovery of elemental sulfur and co-production of electric energy |
| JP5755624B2 (en) * | 2012-10-15 | 2015-07-29 | トヨタ自動車株式会社 | Air electrode for air battery and air battery |
| JP5828336B2 (en) * | 2013-11-19 | 2015-12-02 | トヨタ自動車株式会社 | Iron-air battery pack and method of using the same |
| CN106532195B (en) * | 2017-01-03 | 2018-09-04 | 湖南科技大学 | A kind of ferrous ion/air cell and preparation method thereof |
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