CN111769291A - Sodium-carbon dioxide battery, anode used on sodium-based battery and preparation method thereof - Google Patents
Sodium-carbon dioxide battery, anode used on sodium-based battery and preparation method thereof Download PDFInfo
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- H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
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- H01M4/00—Electrodes
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Abstract
The invention relates to a sodium-carbon dioxide battery, an anode used on the sodium-based battery and a preparation method thereof. The anode comprises metal sodium, biphenyl, supporting electrolyte, ether solvent and conductive carbon; the preparation method comprises the steps of dissolving a supporting electrolyte in an ether solvent to obtain an electrolyte, dissolving biphenyl and metal sodium in the electrolyte to obtain an alkali solution, and then mixing the alkali solution with conductive carbon to obtain the conductive carbon; the concentration of the supporting electrolyte in the electrolyte is 0.1-1 mol/L; the concentration of the sodium biphenyl in the alkali solution is 0.1-1 mol/L. The method comprises the steps of dissolving a supporting electrolyte in an ether solvent to prepare an electrolyte with the concentration of 0.1-1 mol/L; dissolving biphenyl and metal sodium in electrolyte to prepare an alkali solution with the sodium concentration of 0.1-1 mol/L; and adding conductive carbon into the alkali solution to obtain the anode. The invention also includes a sodium carbon dioxide battery having the anode described above. The anode is safe and has stable electrochemical performance.
Description
Technical Field
The invention relates to the field of new energy materials, in particular to a sodium-carbon dioxide battery, an anode used on the sodium-based battery and a preparation method thereof.
Background
Although the research of sodium-carbon dioxide batteries has made a major breakthrough in recent years, the typical sodium-carbon dioxide battery is composed of solid metal sodium as a negative electrode and liquid electrolyte, and the metal sodium has the problems of dendrite, self-corrosion and the like in stripping and electroplating processes. These problems eventually lead to internal short circuits, creating serious safety issues.
In order to solve these problems, one solution is to replace the organic liquid electrolyte with a highly conductive, non-flammable solid ceramic electrolyte, however, the interface between solid sodium metal and the solid electrolyte has a huge contact interface resistance, resulting in a metal carbon dioxide battery that has never been a major breakthrough. In addition, the electrochemical performance of the metal carbon dioxide battery is unstable.
Disclosure of Invention
The technical problem to be solved by the invention is as follows: how to provide an anode which has stable and safe electrochemical performance and is used on a sodium-based battery. On the basis, the problem of how to provide a sodium-carbon dioxide battery with stable electrochemical performance and safety is further solved.
In order to solve the technical problems, the invention provides a sodium-carbon dioxide battery, an anode used on the sodium-based battery and a preparation method thereof.
The invention provides an anode for a sodium-based battery, which comprises: metal sodium, biphenyl, supporting electrolyte, ether solvent and conductive carbon; dissolving the supporting electrolyte in the ether solvent to obtain an electrolyte, dissolving the biphenyl and the metal sodium in the electrolyte to obtain an alkali solution, and mixing the alkali solution with the conductive carbon to obtain the anode; the supporting electrolyte comprises one or more of sodium perchlorate, sodium trifluoromethanesulfonate, sodium bistrifluoromethanesulfonylimide and sodium hexafluorophosphate, and the concentration of the supporting electrolyte in the electrolyte is 0.1-1 mol/L; the concentration of the metal sodium in the alkali solution is 0.1-1 mol/L.
Preferably, the ether solvent includes one or more of ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, triethylene glycol dimethyl ether and tetraethylene glycol dimethyl ether.
Preferably, the mass fraction of the conductive carbon in the alkali solution is 0.1-5%.
Preferably, the metal sodium and the biphenyl are dissolved in the electrolyte according to a molar ratio of 1:1 to obtain the alkali solution.
The invention also provides a preparation method of the anode for the sodium-based battery, which comprises the following steps:
s1, dissolving the supporting electrolyte in an ether solvent to prepare an electrolyte with the concentration of 0.1-1 mol/L; the supporting electrolyte comprises one or more of sodium perchlorate, sodium trifluoromethanesulfonate, sodium bistrifluoromethanesulfonylimide and sodium hexafluorophosphate;
s2, dissolving biphenyl and metal sodium in the electrolyte obtained in the step S1 to obtain an alkali solution with the sodium concentration of 0.1-1 mol/L;
s3, adding conductive carbon into the alkali solution prepared in the step S2 to obtain the anode.
Further, the conductive carbon is added into the alkali solution prepared in the step S2 and stirred for 2-3h to obtain the anode.
Preferably, in step S3, the conductive carbon is added to the alkaline solution prepared in step S2 in an amount of 0.1 to 5% by mass of the alkaline solution to obtain the anode.
In addition, the invention also provides a sodium-carbon dioxide battery, which sequentially comprises the anode or the anode prepared by the preparation method, a solid electrolyte, an aqueous electrolyte and a carbon dioxide positive electrode from top to bottom, wherein the aqueous electrolyte is a NaCl solution.
Compared with the prior art, the invention has the advantages that: the metal sodium and the biphenyl are dissolved in the electrolyte to form an alkali solution, wherein the metal sodium and the biphenyl form biphenyl sodium, the metal sodium in the alkali solution exists in the form of sodium ions, water does not exist in the alkali solution, the anode does not have the problems of dendrite generation and self-corrosion of the metal sodium, the performance of the anode is safe, the concentration of the metal sodium in the alkali solution is 0.1-1 mol/L, the anode has high sodium ion conductivity, in addition, the electrolyte is prepared by dissolving a supporting electrolyte in an ether solvent, the supporting electrolyte comprises one or more sodium salts of sodium perchlorate, sodium trifluoromethanesulfonate, sodium bistrifluoromethanesulfonylimide and sodium hexafluorophosphate, the supporting electrolyte is dissolved in the ether solvent to form the electrolyte with the concentration of 0.1-1 mol/L, the supporting electrolyte in the electrolyte can also provide the sodium ions, the stable ionic strength can be maintained in the alkali solution, and the conductivity of the alkali solution is increased, in addition, the specific surface area of the conductive carbon used as the biphenyl sodium carrier is large, so that the effective current density can be reduced, the transmission rate of electrons can be effectively accelerated, and the anode has stable electrochemical performance, so that the anode is safe and has stable electrochemical performance. Further, a sodium carbon dioxide battery including the anode is safe and has stable electrochemical properties.
In addition, the sodium-carbon dioxide battery adopting the semi-liquid anode enhances the electrochemical reaction kinetics due to the rapid transmission of sodium ions and electrons, thereby reducing the charging voltage of the battery, and the charging voltage can be as low as 2.5V.
Drawings
The features and advantages of the present invention will be more clearly understood by reference to the accompanying drawings, which are illustrative and not to be construed as limiting the invention in any way, and in which:
fig. 1 is a schematic block diagram of a battery including an anode-based sodium carbon dioxide battery for use in a sodium-based battery.
Fig. 2 is a charge-discharge graph of the sodium carbon dioxide battery in example 1.
Fig. 3 is a discharge capacity graph of the sodium carbon dioxide cell in example 1.
Fig. 4 is a rate graph of the sodium carbon dioxide cell of example 1.
Fig. 5 is a charge-discharge graph of the sodium carbon dioxide battery in example 2.
Fig. 6 is a graph of the rate of expansion of the sodium carbon dioxide cell in example 2.
Fig. 7 is a charge-discharge graph of the sodium carbon dioxide battery in example 3.
Detailed Description
In order to make the aforementioned objects, features and advantages of the present invention comprehensible, embodiments accompanied with figures are described in detail below. In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present invention. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein, but rather should be construed as broadly as the present invention is capable of modification in various respects, all without departing from the spirit and scope of the present invention.
The present embodiment provides an anode for use in a sodium-based battery, comprising: metal sodium, biphenyl, supporting electrolyte, ether solvent and conductive carbon; dissolving the supporting electrolyte in the ether solvent to obtain electrolyte, dissolving the biphenyl and the metal sodium in the electrolyte according to a molar ratio of 1:1 to obtain an alkali solution, and mixing the alkali solution and the conductive carbon to obtain the anode; the supporting electrolyte comprises one or more of sodium perchlorate, sodium trifluoromethanesulfonate, sodium bistrifluoromethanesulfonylimide and sodium hexafluorophosphate, and the concentration of the supporting electrolyte in the electrolyte is 0.1-1 mol/L; the concentration of the metal sodium in the alkali solution is 0.1-1 mol/L; wherein the ether solvent comprises one or more of ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, triethylene glycol dimethyl ether and tetraethylene glycol dimethyl ether; the mass fraction of the conductive carbon in the alkali solution is 0.1-5%.
The specific embodiment further comprises the preparation method of the anode for the sodium-based battery, which comprises the following steps:
s1, dissolving the supporting electrolyte in an ether solvent to prepare an electrolyte with the concentration of 0.1-1 mol/L; the supporting electrolyte comprises one or more of sodium perchlorate, sodium trifluoromethanesulfonate, sodium bistrifluoromethanesulfonylimide and sodium hexafluorophosphate;
s2, dissolving biphenyl and metal sodium in the electrolyte obtained in the step S1 to obtain an alkali solution with the sodium concentration of 0.1-1 mol/L;
s3, adding conductive carbon which accounts for 0.1-5% of the mass fraction of the alkali solution into the alkali solution prepared in the step S2, and stirring for 2-3 hours to obtain the anode.
With reference to fig. 1, the present embodiment further includes a sodium-carbon dioxide battery, which includes the anode described above or the anode prepared by the preparation method described above, a solid electrolyte, an aqueous electrolyte and a carbon dioxide positive electrode in order from top to bottom, where the aqueous electrolyte is a NaCl solution.
Wherein the solid electrolyte comprises Na3Zr2Si2PO12The fast ion conductor of NASICON structure, β -Al2O3One of sodium aluminate fast ion conductor and sulfide fast ion conductor.
To further illustrate the anode for sodium-based batteries and the sodium carbon dioxide battery proposed in this embodiment, several more detailed examples are set forth below.
The anode according to this embodiment is added with conductive carbon, and the anode has a flow characteristic at room temperature, and is called a semi-liquid anode.
Example 1
In an inert atmosphere glove box, firstly, taking sodium perchlorate as a supporting electrolyte to dissolve in tetraethylene glycol dimethyl ether, and stirring until the supporting electrolyte is completely dissolved to obtain 0.1mol/L sodium perchlorate electrolyte; biphenyl and metal sodium are respectively weighed according to the molar ratio of 1:1, the biphenyl is firstly dissolved in the sodium perchlorate electrolyte, the metal sodium is added after the biphenyl is completely dissolved to obtain a dark green alkali solution of 0.1mol/L, 1 wt% of conductive carbon black is added after the biphenyl is completely dissolved, and the mixture is stirred for 2 hours to obtain the semi-liquid anode.
As shown in figure 1, from the negative electrode to the positive electrode, the semi-liquid anode and β -Al are sequentially arranged from bottom to top2O3The sodium carbonate battery is assembled by the sodium aluminate fast ion conductor solid electrolyte, the sodium chloride electrolyte and the carbon dioxide positive electrode.
The sodium-carbon dioxide battery assembled in the embodiment is pure CO at room temperature2The charge and discharge performance test was performed in an atmosphere, and the charge and discharge curves of the sodium-carbon dioxide battery prepared in this example are shown in fig. 2, the discharge capacity curve of the sodium-carbon dioxide battery prepared in this example is shown in fig. 3, and the rate performance curve of the sodium-carbon dioxide battery prepared in this example is shown in fig. 4. As shown in FIG. 2The battery shows a stable charging and discharging platform, and the charging and discharging voltage difference of the battery is 0.72V; as can be seen from fig. 3, the battery discharge capacity was 3.6 mAh; as can be seen from fig. 4, the battery exhibited good rate capability.
Example 2
In an inert atmosphere glove box, firstly, taking sodium perchlorate as a supporting electrolyte to dissolve in ethylene glycol dimethyl ether, and stirring until the supporting electrolyte is completely dissolved to obtain 0.1mol/L sodium perchlorate electrolyte; biphenyl and metal sodium are respectively weighed according to the molar ratio of 1:1, the biphenyl is firstly dissolved in the sodium perchlorate electrolyte, the metal sodium is added after the biphenyl is completely dissolved to obtain 1mol/L dark green alkali solution, 5 wt% of conductive carbon black is added after the biphenyl is completely dissolved, and the mixture is stirred for 2 hours to obtain the double (electronic and ionic) conductive medium semi-liquid anode.
As shown in figure 1, a sodium-carbon dioxide battery is assembled from a semi-liquid anode, a sulfide fast ion conductor solid electrolyte, a sodium chloride electrolyte and a carbon dioxide anode from bottom to top in sequence from a cathode to an anode.
The sodium-carbon dioxide battery assembled in the embodiment is pure CO at room temperature2The charge and discharge performance test was performed in an atmosphere, and the charge and discharge curves of the sodium-carbon dioxide battery prepared in this example are shown in fig. 5, and the rate performance curve of the sodium-carbon dioxide battery prepared in this example is shown in fig. 6. As can be seen from fig. 5 to 6, the battery exhibited a low charge voltage (about 2.5V), a battery charge-discharge voltage difference of 0.68V, and good rate capability.
Example 3
In an inert atmosphere glove box, firstly, dissolving sodium trifluoromethanesulfonate as a supporting electrolyte in tetraethylene glycol dimethyl ether, and stirring until the supporting electrolyte is completely dissolved to obtain 0.1mol/L sodium trifluoromethanesulfonate electrolyte; biphenyl and metal sodium are respectively weighed according to the molar ratio of 1:1, the biphenyl is firstly dissolved in the sodium perchlorate electrolyte, the metal sodium is added after the biphenyl is completely dissolved to obtain a dark green alkali solution of 0.2mol/L, after the biphenyl is completely dissolved, 3 wt% of conductive carbon black is added, and the mixture is stirred for 2 hours to obtain the semi-liquid anode.
As shown in fig. 1, the semi-liquid anode is arranged from the negative electrode to the positive electrode from bottom to top、Na3Zr2Si2PO12The NASICON structure fast ion conductor solid electrolyte, the sodium chloride electrolyte and the carbon dioxide positive electrode are assembled into the sodium-carbon dioxide battery.
The sodium-carbon dioxide battery assembled in the embodiment is pure CO at room temperature2When the charge and discharge performance test is performed in the atmosphere, the charge and discharge curve of the sodium-carbon dioxide battery prepared in this example is as shown in fig. 7, and it can be seen from the graph that the battery shows stable charge and discharge voltage and can stably operate.
Other beneficial effects are as follows:
(1) the metal sodium reacts with biphenyl to form a dark green sodium ion solution in an ether solvent, and the sodium ion solution has high sodium ion conductivity; in addition, the supporting electrolyte can provide sodium ions so as to increase the conductivity, and the conductive carbon is beneficial to accelerating the transmission rate of electrons; the semi-liquid anode has electron and ion conductive media, so that the migration of sodium ions and the interface electron transfer are effectively improved.
(2) The flowing semi-liquid anode has lower contact surface resistance with the solid electrolyte, and is beneficial to developing a high-performance carbon dioxide battery.
(3) The sodium element in the semi-liquid anode exists in a sodium ion form, so that severe reaction can not occur when the semi-liquid anode is in contact with water, and the safety of the battery is higher; in addition, the semi-liquid anode solves the problems of dendrite, self-corrosion and the like of the traditional metal sodium, and the safety of a battery system is higher.
(4) The metal sodium, the biphenyl, the supporting electrolyte and the conductive carbon have good solubility in ether solvents, and formed ions and electron conductive media have synergistic effect and are mutually promoted, so that the battery finally shows low charging voltage.
(5) Compared with a pure liquid anode, the anode is a semi-liquid anode, so that the anode is not easy to volatilize and leak.
(6) The carbon dioxide battery has a lower electrical resistance at the contact surface between the electrode anode and the solid electrolyte, and is useful for developing a long-life, high-efficiency carbon dioxide battery.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used in the description of the invention herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
Claims (8)
1. An anode for use on a sodium-based battery, comprising: metal sodium, biphenyl, supporting electrolyte, ether solvent and conductive carbon; dissolving the supporting electrolyte in the ether solvent to obtain an electrolyte, dissolving the metal sodium and the biphenyl in the electrolyte to obtain an alkali solution, and mixing the alkali solution and the conductive carbon to obtain the anode; the supporting electrolyte comprises one or more of sodium perchlorate, sodium trifluoromethanesulfonate, sodium bistrifluoromethanesulfonylimide and sodium hexafluorophosphate, and the concentration of the supporting electrolyte in the electrolyte is 0.1-1 mol/L; the concentration of the metal sodium in the alkali solution is 0.1-1 mol/L.
2. The anode of claim 1, wherein the ether solvent comprises one or more of glyme, diglyme, triglyme, and tetraglyme.
3. The anode used for the sodium-based battery as claimed in claim 1, wherein the mass fraction of the conductive carbon in the alkali solution is 0.1-5%.
4. The anode for use in a sodium-based battery as claimed in claim 1, wherein said alkali solution is obtained by dissolving said metallic sodium and said biphenyl in said electrolyte at a molar ratio of 1: 1.
5. A method of preparing an anode for use in a sodium-based battery as claimed in any one of claims 1 to 4, comprising the steps of:
s1, dissolving the supporting electrolyte in an ether solvent to prepare an electrolyte with the concentration of 0.1-1 mol/L; the supporting electrolyte comprises one or more of sodium perchlorate, sodium trifluoromethanesulfonate, sodium bistrifluoromethanesulfonylimide and sodium hexafluorophosphate;
s2, dissolving biphenyl and metal sodium in the electrolyte obtained in the step S1 to obtain an alkali solution with the sodium concentration of 0.1-1 mol/L;
s3, adding conductive carbon into the alkali solution prepared in the step S2 to obtain the anode.
6. The method according to claim 5, wherein the conductive carbon is added to the alkali solution obtained in step S2 and stirred for 2-3h to obtain the anode.
7. The method according to claim 5, wherein in step S3, the conductive carbon is added to the alkaline solution obtained in step S2 in an amount of 0.1 to 5% by mass of the alkaline solution to obtain the anode.
8. A sodium-carbon dioxide battery, which is characterized by comprising the anode according to any one of claims 1 to 4 or the anode prepared by the preparation method according to any one of claims 5 to 7, a solid electrolyte, an aqueous electrolyte and a carbon dioxide positive electrode in sequence from top to bottom, wherein the aqueous electrolyte is a NaCl solution.
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