CN109273287A - A kind of self-healing hydrogel polyelectrolyte and its preparation and application - Google Patents
A kind of self-healing hydrogel polyelectrolyte and its preparation and application Download PDFInfo
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/54—Electrolytes
- H01G11/56—Solid electrolytes, e.g. gels; Additives therein
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F220/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
- C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
- C08F220/52—Amides or imides
- C08F220/54—Amides, e.g. N,N-dimethylacrylamide or N-isopropylacrylamide
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F220/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
- C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
- C08F220/52—Amides or imides
- C08F220/54—Amides, e.g. N,N-dimethylacrylamide or N-isopropylacrylamide
- C08F220/58—Amides, e.g. N,N-dimethylacrylamide or N-isopropylacrylamide containing oxygen in addition to the carbonamido oxygen, e.g. N-methylolacrylamide, N-(meth)acryloylmorpholine
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/02—Elements
- C08K3/04—Carbon
- C08K3/042—Graphene or derivatives, e.g. graphene oxides
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/34—Silicon-containing compounds
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08F220/00—Copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and only one being terminated by only one carboxyl radical or a salt, anhydride ester, amide, imide or nitrile thereof
- C08F220/02—Monocarboxylic acids having less than ten carbon atoms; Derivatives thereof
- C08F220/52—Amides or imides
- C08F220/54—Amides, e.g. N,N-dimethylacrylamide or N-isopropylacrylamide
- C08F220/58—Amides, e.g. N,N-dimethylacrylamide or N-isopropylacrylamide containing oxygen in addition to the carbonamido oxygen, e.g. N-methylolacrylamide, N-(meth)acryloylmorpholine
- C08F220/585—Amides, e.g. N,N-dimethylacrylamide or N-isopropylacrylamide containing oxygen in addition to the carbonamido oxygen, e.g. N-methylolacrylamide, N-(meth)acryloylmorpholine and containing other heteroatoms, e.g. 2-acrylamido-2-methylpropane sulfonic acid [AMPS]
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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
- Y02E60/13—Energy storage using capacitors
Abstract
The present invention relates to a kind of self-healing hydrogel polyelectrolyte and its preparation and application, which is by being prepared with 2- acrylamide-2-methyl propane sulfonic and the copolymerization of N,N-DMAA monomer, lithium diatomaceous earth and graphene oxide for dual crosslinking agent.Compared with prior art, the present invention not only tensile strength with higher, and excellent and repeatable self-healing performance is shown under heating or Infrared irradiation.Using the hydrogel simultaneously as electrolyte and diaphragm, and accordion electrode is constructed by the method for pre-stretching, prepared supercapacitor has the tensility (1000%) and excellent self-healing performance of superelevation.Also, the supercapacitor after healing still maintains 900% or so tensility.The structure and preparation process of self-healing, high stretch supercapacitor in the present invention are all relatively simple, have broad application prospects in terms of Portable flexible, wearable device.
Description
Technical field
The present invention relates to supercapacitor technologies fields, and in particular to a kind of self-healing hydrogel polyelectrolyte and its preparation
With application.
Background technique
In recent years, there is intelligent self-healing, the flexibility of stretch-proof, wearable electronic product to get more and more people's extensive concerning,
For the energy requirement for preferably meeting above-mentioned electronic product, there is an urgent need to develop matched selfreparing, resistance to mechanical power
The energy storage device of destruction.Due to its power density is high, have extended cycle life, manufacture craft is simple the features such as, people are by setting
Meter new structure electrode material and electrolyte deeply grind the flexible super capacitor with selfreparing or tensile property
Study carefully.Although thering are some stretchable supercapacitors with self-healing properties to be reported at present, their self-healing properties
It is often poor, and usually fracture/reparation cycle-index is less.Therefore, while realizing that efficient self-repairability and superelevation can be drawn
The supercapacitor for stretching performance is still a huge challenge.
Self-healing or stretchable substrate or electrolyte are the key that the self-healing or stretchable function for realizing supercapacitor
Place.But that neither there are inherent self-healing properties also not have is very high for the polyvinyl alcohol base electrolyte generallyd use at present
Tensile property, and three-dimensional network crosslinking polyalcohol hydrogel can by functionalization, and ionic conductivity with higher,
Self-healing and tensile property, to obtain Multi-function super capacitor.But it currently, is used about novel hydrogels polyelectrolyte
It is seldom in the report with selfreparing and stretchable flexible super capacitor.
Summary of the invention
It is an object of the present invention to overcome the above-mentioned drawbacks of the prior art and provide a kind of self-healing hydrogels
Polyelectrolyte and its preparation and application.
The purpose of the present invention can be achieved through the following technical solutions: a kind of self-healing hydrogel polyelectrolyte, the water
Gel polyelectrolyte is 2- acrylamide-2-methyl propane sulfonic monomer and N, and the reaction of N- dimethacrylamide monomers generates poly-
Object hydrogel is closed, the polymer is using graphene oxide and lithium diatomaceous earth as crosslinking agent, wherein the 2- acrylamide -2- first
Base propane sulfonic acid, N, N- dimethacrylamide, graphene oxide, lithium diatomaceous earth and water mass ratio be (0.028~0.08):
(0.0125~0.018): (0~0.025): (0.01~0.05): 1, and the amount of graphene oxide is not 0.
Inorganic matter graphene oxide and lithium diatomaceous earth interact in the polymer matrix can be enhanced hydrogel mechanical performance.
In addition, the inorganic nano material graphene oxide and lithium diatomaceous earth of different structure are made with polymer chain again by interacting between the two
It uses or both respectively with polymer chain using the secondary or physical bonds such as hydrogen bond or coordinate bond interaction crosslinking as multi-functional crosslinking agent.
On the other hand, polymer chain under conditions of heating or infrared light after the diffusion on the interface of fracture position with lithium diatomaceous earth or/
It is acted on again with graphene oxide and forms new crosslinking points and assign hydrogel self-healing performance.In addition, as infrared absorbing agents, GO
Sheet material promptly can convert thermal energy for the luminous energy of absorption, so that the diffusion and crosslinked action of polymer chain is greatly facilitated, it is real
Quick self-healing behavior is showed.
A kind of preparation method of self-healing hydrogel polyelectrolyte as described above, comprising the following steps:
(1) in deionized water by graphene oxide dispersion, stirring, ultrasound obtain dispersion liquid, and lithium diatomaceous earth is then added, stirs
It mixes to obtain mixed liquor；
(2) 2- acrylamide-2-methyl propane sulfonic monomer and N, N- dimethyl propylene is added in the mixed liquor obtained by step (1)
Acrylamide monomer, then sequentially adds initiator and catalyst, is stood after mixing to get the poly- electricity of the self-healing hydrogel
Solve plasma membrane.
In uniform graphene oxide and lithium diatomaceous earth mixed dispersion liquid is made, potassium peroxydisulfate decomposes free radical, causes 2-
Free radicals copolymerization reaction in situ occurs for acrylamide-2-methyl propane sulfonic monomer and N,N-DMAA monomer, in oxygen
Crosslinked polymer is carried out in the presence of graphite alkene and lithium diatomaceous earth, so that it may obtain the hydrogel dielectric film.
Preferably, after the graphene oxide is add to deionized water, mixing time is 10~60min, stirring speed
Rate is 100~2000rpm, and ultrasonic time is 20~60min, and supersonic frequency is 10~60kHz.
Preferably, the mixing time being added after the lithium diatomaceous earth is 10~60min, stirring rate is 100~
2000rpm。
Preferably, it is both needed to after 2- acrylamide-2-methyl propane sulfonic monomer and N,N-DMAA monomer being added
It stirs evenly, the rate of stirring is 100~2000rpm, and mixing time is 10~60min.
Preferably, the initiator is potassium peroxydisulfate, and the additive amount of the potassium peroxydisulfate and the addition mass ratio of water are
(0.0006~0.00375): 1, after initiator is added, stir 10~50min.
Preferably, the catalyst is tetramethylethylenediamine, the additive amount of the tetramethylethylenediamine and potassium peroxydisulfate
Adding mass ratio is (0.13~0.775): 1, after catalyst is added, stir 5~30min.
Preferably, the temperature of the standing is room temperature, and the time of standing is 12~48h.
A kind of application of self-healing hydrogel polyelectrolyte as described above, which comprises the following steps: described
For hydrogel polyelectrolyte for the electrolyte as supercapacitor, the supercapacitor includes being covered on the poly- electrolysis of hydrogel
The film of matter formation and the membrane electrode for being covered on film two sides, the end of the membrane electrode pass through the fixed copper wire of elargol.
Preferably, the material of the membrane electrode is carbon nano-tube film or carbon nano-tube/poly aniline film.Wherein, carbon
The size of nano-tube film is about 2mm × 15mm, when needs are when carbon nano-tube film surface deposits polyaniline, using electrochemistry
Sedimentation, specific as follows: using the sulfuric acid solution of aniline as electrolyte, carbon nano-tube film is working electrode, saturated calomel electrode
For reference electrode, platinized platinum is to carry out cyclic voltammetry scan, the parameter of the cyclic voltammetry scan is that scanning speed is to electrode
0.1V/s, scanning range are -0.1-0.8V, and circle number is 1~160 circle.
Compared with prior art, the beneficial effects of the present invention are embodied in following several respects:
(1) the hydrogel polyelectrolyte not only tensile property with higher prepared by the present invention, but also can heat
Or excellent repeatable self-healing performance is shown under the conditions of infrared light photograph；
(2) supercapacitor constructed by the present invention has flexible and repeatable bendability well, by introducing counterfeit electricity
Capacity materials significantly improve the capacitance of supercapacitor；
(3) supercapacitor constructed by the present invention shows tensile property and the self-healing of superelevation (1000%)
Energy；
(4) supercapacitor prepared by the present invention still maintains 900% tensility energy after self-healing.
Detailed description of the invention
Fig. 1 hydrogel respectively high temperature and infrared laser irradiation under mechanical strength variation diagram；
Capacity and resistance variations figure under the differently curved angle of Fig. 2 supercapacitor；
Fig. 3 supercapacitor is bent the capacity and resistance variations figure of 120 degree of different numbers；
Fig. 4 carbon nano-tube/poly aniline membrane electrode based super capacitor charging and discharging curve figure；
Charging and discharging curve figure under Fig. 5 supercapacitor different stretch state；
Fig. 6 supercapacitor respectively high temperature and infrared laser irradiation under cycle-index figure；
Capacity retention ratio curve graph under Fig. 7 self-healing supercapacitor different stretch state.
Specific embodiment
It elaborates below to the embodiment of the present invention, the present embodiment carries out under the premise of the technical scheme of the present invention
Implement, the detailed implementation method and specific operation process are given, but protection scope of the present invention is not limited to following implementation
Example.
Embodiment 1
It is a kind of with self-healing and tensility can hydrogel polyelectrolyte and its apply in flexible super capacitor
Preparation method, specific steps are as follows:
Step 1: taking 0.38g 2.5wt% graphene oxide to be dispersed in the deionized water of 7.8ml, persistently stir 16 points
Clock, it is then 40 minutes ultrasonic.
Step 2: 0.2g lithium diatomaceous earth being added in the graphene oxide dispersion of step 1, is persistently stirred 20 minutes.
Step 3: by monomer 0.42g 2- acrylamide-2-methyl propane sulfonic and monomer 1.3ml N, N- dimethyl allene acyl
Amine is added sequentially in the mixed liquor of step 2, is stirred 20 minutes respectively.
Step 4: initiator 0.015g potassium peroxydisulfate is then added, stirs 10 minutes.8 μ L of catalyst mixing is eventually adding to stir
It mixes 8 minutes.
Step 5: the copolymer that step 4 is obtained, which is placed in, can be obtained dual Nanometer composite hydrogel in 18 hours at room temperature.
Step 6: after hydrogel cutting in step 5, testing hydrogel before and after the processing after heating or Infrared irradiation
Tensile property.
Step 7: it is 2mm × 15mm elongate in shape that carbon nanotube thin film, which is cut into size, and end connects copper wire with elargol.In step 5
In the two sides of obtained aquagel membrane respectively cover a piece of carbon nanotube thin film electrode for having permeated pre-polymerization liquid and obtain supercapacitor.
Step 8: supercapacitor in step 7 being tested into chemical property under differently curved angle and is repeated its is curved
Chemical property under song to 120 degree.
By above step, have and polyvinyl alcohol electrolyte by the dual Nanometer composite hydrogel that in-situ polymerization obtains
Comparable conductivity (5mS/cm) and draftability, additionally show self-healing performance, and the fracture of hydrogel is stretched after being cut off
Before long rate can be restored to fracture after the irradiation of high temperature and infrared laser and intensity improves (Fig. 1), hydrogel
Self-healing property can be attributed to polymer chain under conditions of heating or infrared light after the diffusion on the interface of fracture position with
Lithium diatomaceous earth or/and graphene oxide act on again forms new crosslinking points.On the other hand, in entire agglutination, not only disconnected
Position is split, crosslinked action again also has occurred in entire gel, the mechanical strength for resulting in hydrogel after healing enhances.In addition,
As infrared absorbing agents, GO sheet material promptly can convert thermal energy for the luminous energy of absorption, so that polymer chain be greatly facilitated
Diffusion and crosslinked action, realize quick self-healing behavior.Meanwhile the supercapacitor assembled be flexible to any angle and
Capacitance and resistance all do not change significantly (Fig. 2), or even can pass through 5000 bend cycles (Fig. 3), illustrate super electricity
Container has excellent flexibility and stability.
Embodiment 2
It is a kind of with self-healing and tensility can hydrogel polyelectrolyte and its apply in flexible super capacitor
Preparation method, specific steps are as follows:
Step 1: it takes 0.4g 2.5wt% graphene oxide to be dispersed in the deionized water of 7.8ml, persistently stirs 10 minutes,
Then ultrasound 20 minutes.
Step 2: 0.2g lithium diatomaceous earth being added in the graphene oxide dispersion of step 1, is persistently stirred 20 minutes.
Step 3: by monomer 0.4g 2- acrylamide-2-methyl propane sulfonic and monomer 0.8ml N, N- dimethyl allene acyl
Amine is added sequentially in the mixed liquor of step 2, is stirred 30 minutes respectively.
Step 4: initiator 0.02g potassium peroxydisulfate is then added, stirs 20 minutes.13 μ L of catalyst mixing is eventually adding to stir
It mixes 10 minutes.
Step 5: the copolymer that step 4 is obtained, which is placed in, can be obtained dual Nanometer composite hydrogel in 15 hours at room temperature.
Step 6: polyaniline by the method for electrochemical deposition method it is compound in carbon nanotube thin film, comprising the following steps: with aniline
Sulfuric acid solution be electrolyte, carbon nano-tube film is working electrode, and saturated calomel electrode is reference electrode, and platinized platinum is to electricity
Pole carries out cyclic voltammetry scan, and it is 0.1V/s that the parameter of the cyclic voltammetry scan, which is scanning speed, and scanning range is-
0.1-0.8V, circle number are 120 circles.
Step 7: it is 2.5mm × 12mm strip that carbon nano-tube/poly aniline film obtained in step 6, which is cut into size,
Shape, end connect copper wire with elargol.The two sides of obtained aquagel membrane respectively covers a piece of pre-polymerization liquid of having permeated in steps of 5
Carbon nano-tube/poly aniline membrane electrode obtains supercapacitor.
By above step, by introducing fake capacitance material polyaniline, the performance of the supercapacitor prepared can be by
9mF/cm2It improves to 180mF/cm2(Fig. 4).
Embodiment 3
It is a kind of with self-healing and tensility can hydrogel polyelectrolyte and its apply in flexible super capacitor
Preparation method, specific steps are as follows:
Step 1: taking 0.32g 2.5wt% graphene oxide to be dispersed in the deionized water of 7.8ml, persistently stir 20 points
Clock, it is then 30 minutes ultrasonic.
Step 2: 0.16g lithium diatomaceous earth being added in the graphene oxide dispersion of step 1, is persistently stirred 15 minutes.
Step 3: by monomer 0.38g 2- acrylamide-2-methyl propane sulfonic and monomer 1.05mol N, N- dimethyl allene
Amide is added sequentially in the mixed liquor of step 2, is stirred 15 minutes respectively.
Step 4: initiator 0.01g potassium peroxydisulfate is then added, stirs 15 minutes.10 μ L of catalyst mixing is eventually adding to stir
It mixes 5 minutes.
Step 5: the copolymer that step 4 is obtained, which is placed in, can be obtained dual Nanometer composite hydrogel in 24 hours at room temperature.
Step 6: it is 2mm × 15mm elongate in shape that carbon nanotube thin film, which is cut into size, and end connects copper wire with elargol.In step 5
In the two sides of obtained aquagel membrane respectively cover a piece of carbon nanotube thin film electrode for having permeated pre-polymerization liquid and obtain supercapacitor.
Step 7: after supercapacitor cutting in step 6, testing supercapacitor under heating or Infrared irradiation
Chemical property.
Step 8: supercapacitor in step 6 being stretched under differently strained length, the electrochemistry of supercapacitor is tested
Performance.
By above step, the supercapacitor prepared not only tensile property with higher can be stretched to 100%
Preferable chemical property (Fig. 5) is still kept, and shows preferable self-healing repetitive cycling performance (Fig. 6), can be weighed
Repair 15 times again or more.Meanwhile to by processing to obtain supercapacitor progress different stretch degree under heating or Infrared irradiation
Under electrochemical property test, it is known that self-healing supercapacitor still can be stretched to 900% (Fig. 7), supercapacitor
Capacity can still keep 85% compared with initial capacity.
Claims (10)
1. a kind of self-healing hydrogel polyelectrolyte, which is characterized in that the hydrogel polyelectrolyte is 2- acrylamide -2- methyl
The polyalcohol hydrogel that sulphonic acid monomer and N,N-DMAA monomer reaction generate, the polymer is with graphite oxide
Alkene and lithium diatomaceous earth are as crosslinking agent, wherein the 2- acrylamide-2-methyl propane sulfonic, N,N-DMAA, oxidation
The mass ratio of graphene, lithium diatomaceous earth and water is (0.028~0.08): (0.0125~0.018): (0~0.025): (0.01~
0.05): 1, and the amount of graphene oxide is not 0.
2. a kind of preparation method of self-healing hydrogel polyelectrolyte as described in claim 1, which is characterized in that including following
Step:
(1) in deionized water by graphene oxide dispersion, stirring, ultrasound obtain dispersion liquid, and lithium diatomaceous earth is then added, stirs
To mixed liquor；
(2) 2- acrylamide-2-methyl propane sulfonic monomer and N, N- dimethyl allene acyl is added in the mixed liquor obtained by step (1)
Amine monomers, then sequentially add initiator and catalyst, are stood after mixing to get the self-healing hydrogel polyelectrolyte
Film.
3. a kind of preparation method of self-healing hydrogel polyelectrolyte according to claim 2, which is characterized in that described
After graphene oxide is add to deionized water, mixing time is 10~60min, and stirring rate is 100~2000rpm, ultrasound
Time is 20~60min, and supersonic frequency is 10~60kHz.
4. a kind of preparation method of self-healing hydrogel polyelectrolyte according to claim 2, which is characterized in that institute is added
Stating the mixing time after lithium diatomaceous earth is 10~60min, and stirring rate is 100~2000rpm.
5. a kind of preparation method of self-healing hydrogel polyelectrolyte according to claim 2, which is characterized in that 2- is added
It is both needed to stir evenly after acrylamide-2-methyl propane sulfonic monomer and N,N-DMAA monomer, the rate of stirring is
100~2000rpm, mixing time are 10~60min.
6. a kind of preparation method of self-healing hydrogel polyelectrolyte according to claim 2, which is characterized in that described to draw
Hair agent is potassium peroxydisulfate, and the additive amount of the potassium peroxydisulfate and the addition mass ratio of water are (0.0006~0.00375): 1, add
After entering initiator, 10~50min is stirred.
7. a kind of preparation method of self-healing hydrogel polyelectrolyte according to claim 2, which is characterized in that described to urge
Agent is tetramethylethylenediamine, the addition mass ratio of the additive amount of the tetramethylethylenediamine and potassium peroxydisulfate be (0.13~
0.775): 1, after catalyst is added, stir 5~30min.
8. a kind of preparation method of self-healing hydrogel polyelectrolyte according to claim 2, which is characterized in that described quiet
The temperature set is room temperature, and the time of standing is 12~48h.
9. a kind of application of self-healing hydrogel polyelectrolyte as described in claim 1, which is characterized in that including following step
Rapid: for the hydrogel polyelectrolyte for the electrolyte as supercapacitor, the supercapacitor includes being covered on water-setting
The film of glue polyelectrolyte formation and the membrane electrode for being covered on film two sides, the end of the membrane electrode pass through elargol fixed copper
Line.
10. a kind of application of self-healing hydrogel polyelectrolyte according to claim 9, which is characterized in that the film
The material of electrode is carbon nano-tube film or carbon nano-tube/poly aniline film.
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| CN113745675A (en) * | 2021-09-07 | 2021-12-03 | 中新国际联合研究院 | Zinc electrode protected by negative electricity skeleton hydrogel as modification layer and preparation method thereof |
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