CN114335634B - Illumination hydrogen evolution water system battery and preparation method and application thereof - Google Patents
Illumination hydrogen evolution water system battery and preparation method and application thereof Download PDFInfo
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- CN114335634B CN114335634B CN202111622347.6A CN202111622347A CN114335634B CN 114335634 B CN114335634 B CN 114335634B CN 202111622347 A CN202111622347 A CN 202111622347A CN 114335634 B CN114335634 B CN 114335634B
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- 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
- Y02E60/10—Energy storage using batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- 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
- Y02E60/50—Fuel cells
Abstract
The invention discloses an illumination hydrogen evolution water system battery and a preparation method and application thereof. The photocatalytic material is used as the positive electrode, the positive electrode material after hydrogen production activates the battery to discharge, the positive electrode of the battery can be repaired after recharging, the photocatalytic activity is realized again, and the whole process can be circularly carried out. The oxidized catalytic material provides capacity for the anode of the battery, can improve the discharge specific capacity of the anode, and can store hydrogen energy. The invention can convert light energy to generate hydrogen and improve the battery performance. The cell has wide application prospect in the field of energy storage and hydrogen evolution, and can be used as a cell for hydrogen evolution and energy storage and a fuel cell photocatalysis range extender.
Description
Technical Field
The invention relates to the field of new energy batteries, in particular to an illumination hydrogen evolution water system battery and a preparation method and application thereof.
Background
Energy is an important support and motive force for the development of human economy and social progress, and with the development of world economy, the demand of human beings for energy is increasing. The energy source mainly used today is still a traditional fossil energy source. On the one hand, the waste gas generated by the combustion of fossil energy causes environmental pollution and climate change, which has serious influence on the living environment of human beings. On the other hand, fossil energy is non-renewable energy, and with continuous exploitation and use, fossil energy is exhausted, and humans face energy crisis.
In order to get rid of the energy crisis, clean energy such as wind energy, water energy, solar energy, tidal energy and the like has been widely studied in recent years. These clean energy sources are often utilized in the form of electrical energy. However, these new energy sources are often affected by weather, geographical locations, etc., and cannot continuously and stably supply energy sources with volatility. Therefore, it is important to develop a controllable, safe and inexpensive energy storage system to regulate and control the stable output of energy. The electrochemical energy storage has the characteristics of high energy density, long cycle life, no pollution in operation, low maintenance cost, flexible applicability to various energy storage scenes and the like, and is an important research direction of the energy storage system at present.
On one hand, the water-based zinc ion battery has been widely concerned because of the advantages of low cost, safety, environmental protection and higher energy density, and the improvement of the dynamic characteristics of the positive electrode material has important significance for developing large-scale water-based zinc ion battery energy storage by improving the cycle life and the specific charge-discharge capacity of the water-based zinc ion battery; on the other hand, solar energy is also an important component in the future energy structure, and its efficient utilization is also an object of interest, and in recent years, the development of photocatalytic hydrogen production is considered as an energy source with development potential, and among photocatalytic hydrogen production materials, there is a cheap visible light absorbing material such as Cu 2 O、Cu 2 When S is used for catalytic hydrogen production, a sacrificial agent such as methanol is usually added, otherwise, the valence state of the catalyst is changed, and the catalyst loses the hydrogen production activity.
In addition, hydrogen and oxygen fuel cells are also an important new energy cell relative to solar cells and zinc ion cells. Compared with the traditional battery in which active substances are placed in the battery in advance, the active substances of the hydrogen-oxygen fuel battery can be continuously input while reacting, and the battery capacity is far higher than that of a common battery. But the hydrogen-oxygen fuel cell has high cost, complex system, excessive construction investment of hydrogen-adding station and limited application in global scope.
Disclosure of Invention
Aiming at the prior art problems, the first aim of the invention is to provide an illumination hydrogen evolution water system battery, which uses a photocatalysis material as a battery anode, generates hydrogen under illumination condition and activates the water system battery, the anode material can be repaired after being charged, and the process can be circularly carried out. The zinc ion battery prepared by adopting the photocatalytic material as the positive electrode has excellent capacity retention rate, and the charge-discharge efficiency is higher than 100%.
In order to achieve the technical purpose, the invention adopts the following technical scheme;
an illumination hydrogen evolution water system battery takes a photocatalytic material as an anode, and activates the battery to discharge when illumination catalyzes hydrogen evolution, and the battery is charged again to recover the illumination catalytic hydrogen evolution activity.
When the battery is in illumination, the charge and discharge efficiency of the illumination hydrogen evolution water system battery is more than 100%.
According to the invention, after the photocatalysis process is coupled with the water-based zinc ion battery, the performance of the battery under the condition of illumination can be obviously improved, and the reason is that: the anode material under illumination is in an electron-hole separation state, ions can rapidly and directionally move under the action of an electric field, so that the electron ion exchange is accelerated, the battery has a higher discharge platform and better rate capability, and in addition, the charging platform can be reduced; the reason why the charge and discharge efficiency of the battery is more than 100% is that high-valence oxidation products are generated by illumination, so that the extra positive electrode capacity is improved; at the same time, the failed anode photocatalytic material can be repaired.
Furthermore, the wavelength of light absorbed by the photocatalytic material is mainly in the range of 300-790nm, and hydrogen can be generated under the irradiation of sunlight to activate the battery. Specifically Cu 2 O、CuS、CuI 2 、CdS、MoS 2 、WO 3 、AgNbO 3 、Ag 3 VO 4 At least one of them.
As a preferable technical scheme, the photocatalysis material is Cu 2 O. Under the illumination condition, no sacrificial agent is needed to be added, and the water in the cuprous oxide photocatalytic solution generates hydrogen, and the reaction equation in the process is as follows: cu (Cu) 2 O+H 2 O→2CuO+H 2 After the reaction is finished, cuprous oxide is converted into cupric oxide, so that the zinc ion battery is activated, the cupric oxide can be used as a positive electrode material of the zinc ion battery, basic zinc sulfate and copper can be generated after discharging, and the reaction equation of the process is as follows: cuo+zn+2h 2 O+ZnSO 4 →Cu+ZnSO 4 [Zn(OH) 2 ] 3 H 2 After recharging the battery, the O can change copper into cuprous oxide again, and the reaction equation of the process is as follows:
the second object of the invention is to provide a preparation method of the illumination hydrogen evolution water system battery, which is simple and easy to operate, and has longer service life and higher permittivity compared with the traditional solar battery.
A preparation method of a lighting hydrogen evolution water system battery comprises the steps of loading a photocatalysis material on a current collector, and assembling the photocatalysis material with a zinc cathode material and electrolyte; the photocatalytic material is exposed to a light source.
The photocatalytic material may be exposed to the light source during the entire charge-discharge process, or only during photocatalytic hydrogen evolution upon illumination.
Further, the loading mode is at least one of in-situ growth, rolling and coating.
As a preferable technical scheme, the electrolyte is at least one of zinc acetate, zinc sulfate, zinc triflate, naOH and ZnO in KOH solution.
As a preferred technical solution, a method for manufacturing a semiconductor device,
the manner in which the photocatalytic material is exposed to the light source includes: a transparent battery shell is adopted, or a controllable light source is arranged in the shell.
The battery case includes a hydrogen discharge port. Because hydrogen is generated, a hydrogen discharge port is required to be arranged to ensure the normal internal pressure of the battery, and in addition, water is consumed in the hydrogen evolution reaction and a water filling port is required to be arranged.
The third object of the present invention is to provide an application of the illumination hydrogen evolution water system battery as a battery cell for hydrogen evolution and energy storage or a range extender of an oxyhydrogen fuel cell.
The battery monomer for hydrogen evolution and energy storage can generate hydrogen while storing energy, and greatly improves the energy storage capacity of the battery through the conversion of light energy, so that the battery can store energy and the inside of the battery, can store the energy in a hydrogen energy form, and is also suitable for large-scale energy storage.
The illumination hydrogen evolution water system battery can also be used as a hydrogen-oxygen fuel cell range extender, particularly, after the illumination water system battery is communicated with the hydrogen-oxygen fuel cell, hydrogen generated after illumination can be directly used as a reaction raw material to be supplied to the hydrogen-oxygen fuel cell, after electric energy generated after the reaction of the illumination hydrogen evolution battery is output, the hydrogen-oxygen fuel cell is charged to activate the anode of the illumination hydrogen evolution battery to produce hydrogen again, and water generated by the hydrogen-oxygen fuel cell can be directly used as a consumable to be connected into the illumination hydrogen evolution water system battery, the process mainly utilizes light energy to increase Cheng Nengyuan, and the reaction can be circularly carried out.
Compared with the prior art, the invention has the following advantages:
1) The photocatalytic material is used as the battery anode, a sacrificial agent is not required to be added, the electrochemical charging process is used for repairing the photocatalytic material deactivated for the first time, the method is initial, simple and efficient, can be repeatedly performed, and the practical application of the catalytic material which needs the sacrificial agent to participate is greatly promoted.
2) The invention discovers that the polarization of the positive electrode of the zinc ion battery in the reaction process can be obviously reduced by illumination, so as to realize the high-rate charge and discharge process of the zinc ion battery. The illumination can also provide extra capacity for the positive electrode of the zinc ion battery, so that the charge and discharge efficiency of the positive electrode of the battery is more than 100%, and the phenomenon is discovered for the first time, and the overall energy density of the battery is improved.
3) The method for combining the energy conversion and the large-scale energy storage process has wide application prospect in the field of new energy.
Drawings
FIG. 1 is an adsorption mechanism of a photocatalytic cuprous oxide material;
FIG. 2 is an XRD and SEM of the nano-cuprous oxide material prepared in example 2;
in fig. 2, a and b are SEM pictures of nano cuprous oxide, c is XRD pattern, and d is light absorption of cuprous oxide at different wavelengths.
FIG. 3 is XPS spectrum of cuprous oxide before and after illumination of example 2;
FIG. 4 is an electrochemical impedance spectrum of cuprous oxide in both light and non-light conditions in example 2;
FIG. 5 is a cyclic voltammogram of cuprous oxide in example 2 under both light and non-light conditions;
FIG. 6 is a graph showing the cycle times and specific discharge capacity of cuprous oxide in example 2 under both light and non-light conditions;
figure 7 is an XRD pattern of example 2 before and after cuprous oxide cycling;
FIG. 8 is an XRD pattern of the cuprous oxide of example 2 after discharge;
FIG. 9 is a graph of cycle times and specific discharge capacity versus coulombic efficiency curve for example 3 for cuprous sulfide, and the capacity voltage for the test at different current densities;
in fig. 9, a is the rate performance of the battery, and b is the cyclic charge and discharge performance of the battery;
fig. 10 is an impedance spectrum of a zinc ion cell assembled by growing cuprous oxide positive electrode on a copper mesh in example 4.
Detailed Description
The following embodiments are provided to further illustrate the technical scheme of the present invention, but not to limit the technical scheme, and all modifications and equivalent substitutions are included in the scope of the present invention without departing from the spirit and scope of the technical scheme.
Example 1.
Testing hydrogen evolution rates of various photocatalytic nanomaterials before and after repair (using 465nm, 100nW/cm -2 Light source test of (c) are shown in table 1, intended to illustrate the efficiency of electrochemical repair according to the invention.
TABLE 1
Example 2.
Preparing the nano cuprous oxide material. 20mL of a 0.5mol/L copper sulfate solution and 0.1g of polyethylene glycol 2000 were added to a 250mL single-neck flask, and under magnetic stirring, 0.5 mol/L40 mL of a sodium hydroxide solution was added to the above solution, and after stirring for 30min, 50mL of a 0.1mol/L ascorbic acid solution was added, and stirring was continued for 30min. And after the reaction is finished, carrying out centrifugal separation to obtain cuprous oxide, washing with deionized water and absolute ethyl alcohol for a plurality of times, and then placing in an oven for drying at 80 ℃ for 2 hours. XRD and SEM characterization of the dried material can be seen from figure 2, and the nano cuprous oxide material is successfully synthesized.
The synthesized cuprous oxide, superconducting carbon black and polytetrafluoroethylene binder are mixed according to the following ratio of 7:2:1, rolling the mixture onto a stainless steel mesh after preparing a sheet, and then drying at 60 ℃ for 6 hours, wherein the loading amount of the final active substances is 2mg/cm -2 . Then testing the photocatalytic hydrogen production capacity of the pole piece, wherein the electrolyte is 2mol/L zinc sulfate solution, the wavelength of the used light source is 465nm, and the light intensity is 100nW/cm -2 The hydrogen evolution rate obtained by the test is 18 mu mol/h, but after the test is carried out for 4h, the pole piece loses the photocatalytic activity. The illuminated pole piece was then subjected to an X-ray photoelectron spectroscopy test, and it can be seen from the XPS spectrum that most of the cuprous ions have been converted into copper ions, successfully confirming the conversion process from cuprous oxide to cupric oxide (fig. 3).
In a square electrolytic tank, a pole piece with photocatalysis performance is used as an anode, 2mol/L zinc sulfate is used as electrolyte, zinc foil is used as a cathode, a 465nm light source is used for irradiating the anode piece, and the light intensity is 100nW/cm -2 The photocatalytic coupled aqueous zinc ion battery was assembled and first tested for electrochemical impedance spectroscopy, as shown in fig. 4, with extremely fast ion transmission resistance compared to the illuminated and non-illuminated cuprous oxide anodes. Further, cyclic voltammetry of the cell was performed using this device, and as can be seen from fig. 5, the illuminated cuprous oxide positive electrode had higher electrochemical reactivity and lower electrochemical polarization. The battery system is subjected to battery charge and discharge tests, and as can be seen from fig. 6, the cuprous oxide positive electrode under illumination has higher capacity and better capacity retention rate, and the remarkable effect of illumination on the improvement of the positive electrode performance of the zinc ion battery is fully proved. Finally, the cuprous oxide positive plate after 10 times of charge repair is subjected to photocatalysis hydrogen production test, the hydrogen evolution rate obtained by the test is 100 mu mol/h, which fully shows that the charging process can effectively repair the photocatalysis material, the main phase in the pole piece is also the cuprous oxide material with photocatalytic activity as seen in pole piece XRD (figure 7) of 10 times of charge repair, and the Cu of the pole piece after discharge is seen from figure 8 2 And finally, performing constant current charge and discharge test by using the current density of 600mAh/g to obtain a discharge platform of 0.8v and a discharge specific capacity of 200mAh/g of the battery.
Example 3
Nano Cu to be commercially produced 2 S material, superconducting carbon black and polytetrafluoroethylene binder according to the following weight ratio of 8:1:1, rolling the mixture to a stainless steel net after preparing slices, then drying at 60 ℃ for 6 hours, cu 2 S loading was 1.8mg/cm -2 . Cutting the pole piece into 2cm pieces 2 As an anode material of the aqueous zinc-ion battery, a zinc foil was used as a cathode material, 2mol/L zinc sulfate was used as an electrolyte, and an open aqueous zinc-ion battery was assembled in a square electrolytic tank, and a zinc foil having a wavelength of 465nm and a luminous intensity of 100nW/cm was used -2 The positive plate is irradiated by a monochromatic cold light source to perform electrochemical circularityIt can be tested that constant current charge and discharge tests are carried out by using the current density of 600mAh/g, and as can be found from fig. 9, the illuminated positive electrode shows high specific discharge capacity and charge and discharge efficiency of more than 100%, and a higher discharge platform.
Example 4
The copper mesh (CM, mesh=400) was degreased by washing with 5% sulfuric acid solution and washed with deionized water. A copper mesh was used as a working electrode and a platinum mesh was used as a counter electrode in an aqueous solution containing 1mol/L NaOH. At 2mA/cm -2 The current density constant-current discharge of the electrode is 1h, a copper mesh modified by a copper oxide material on the surface is obtained, then the copper mesh is soaked in an ascorbic acid solution of 0.1mol/L for 2h, copper oxide is reduced into cuprous oxide, then a pole piece is dried, the pole piece is used as the positive electrode of a zinc ion battery, the structure can obtain a large enough specific surface area, light can be fully absorbed and electrolyte can be contacted, and finally the material is tested in zinc sulfate of 2mol/L to obtain the light hydrogen evolution rate of 24 mu mol/h. The light source has wavelength of 465nm and light intensity of 100nW/cm -2 The light hydrogen evolution rate after the charging repair can still reach 21 mu mol/h after the light inactivation, and the AC impedance test is carried out by using the light hydrogen evolution rate as an anode assembled zinc ion full battery, so that the structure can realize rapid ion transmission under the light as can be seen from fig. 10.
Comparative example 1
Using commercialized nano-V 2 O 5 As the positive electrode material of the water-based zinc ion battery, the test mode is the same as that of the example 2, the discharge specific capacity of the corresponding battery is 150mAh/g, the discharge platform is 0.7V, and the discharge specific capacity is lower than that of the illumination Cu in the example 2 2 And in the O zinc ion battery system, no hydrogen is generated in the battery charging and discharging process under illumination. In addition, these vanadium-based materials are expensive and are not suitable for large-scale energy storage batteries.
Comparative example 2
Using commercial nano NH 4 V 4 O 10 As the positive electrode material of the water-based zinc ion battery, the test mode is exactly the same as that of the embodiment 2, the discharge specific capacity of the corresponding battery is 160mAh/g, the discharge platform is 0.65V, and no hydrogen is generated in the charging and discharging process of the battery under illumination, so that the water-based zinc ion battery is not suitable for large-scale energy storage batteries.
Example 5
After the illumination water system battery prepared in the embodiment 2 of the invention is communicated with the oxyhydrogen fuel cell, hydrogen generated after illumination is directly used as a reaction raw material to be supplied to the oxyhydrogen fuel cell, after electric energy generated after the reaction of the illumination hydrogen evolution battery is output, the oxyhydrogen fuel cell is charged to activate the anode of the illumination hydrogen evolution battery to generate hydrogen again, and water generated by the oxyhydrogen fuel cell is directly used as consumable material to be connected into the illumination hydrogen evolution water system battery, wherein the process mainly uses light energy as Cheng Nengyuan, and the reaction can be circularly carried out.
Claims (5)
1. An illumination hydrogen evolution water system battery which is characterized in that: taking a photocatalytic material as an anode, activating a battery to discharge while carrying out photocatalytic hydrogen evolution, and recharging to recover the photocatalytic hydrogen evolution activity;
the photocatalytic material is Cu 2 O、Cu 2 S、CdS、MoS 2 、WO 3 、AgNbO 3 、Ag 3 VO 4 At least one of (a) and (b);
the preparation method of the water-based battery comprises the following steps: loading a photocatalysis material on a current collector, and assembling the photocatalysis material with a zinc metal cathode and electrolyte; the photocatalytic material is exposed to a light source;
the electrolyte is at least one of zinc acetate, zinc sulfate, zinc triflate, naOH and KOH solution containing ZnO.
2. The illuminated hydrogen-generating aqueous battery according to claim 1, wherein: the photocatalytic material is Cu 2 O。
3. The method for producing an illumination hydrogen evolution aqueous battery according to claim 1, wherein: the photocatalytic material is supported in at least one of in-situ growth, rolling and coating.
4. The use of the illuminated hydrogen-evolving aqueous battery according to claim 1 or 2, characterized in that: the device is used for hydrogen evolution and/or energy storage or used as a fuel cell photocatalytic range extender.
5. The use according to claim 4, characterized in that: the hydrogen generated after illumination of the illumination hydrogen evolution battery is used as a reaction raw material to be supplied to the hydrogen-oxygen fuel battery as the fuel battery photocatalysis range extender, and after electric energy generated after the reaction of the illumination hydrogen evolution battery is output, the hydrogen-oxygen fuel battery is charged to activate the anode of the illumination hydrogen evolution battery to generate hydrogen again, and water generated by the hydrogen-oxygen fuel battery is used as consumable material to be connected into the illumination hydrogen evolution battery.
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