CN102646833B - Anodic capillary layer for beta battery and beta battery comprising same - Google Patents
Anodic capillary layer for beta battery and beta battery comprising same Download PDFInfo
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- CN102646833B CN102646833B CN201210157239.0A CN201210157239A CN102646833B CN 102646833 B CN102646833 B CN 102646833B CN 201210157239 A CN201210157239 A CN 201210157239A CN 102646833 B CN102646833 B CN 102646833B
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Abstract
The invention relates to an anodic capillary layer for a beta battery and a beta battery comprising the same. The anodic capillary layer for the beta battery is provided, wherein the beta battery comprises an anode, a solid electrolyte and a cathode; the anodic capillary layer comprises: a porous metal medium which is arranged along the surface of the solid electrolyte so as to realize good contact of the anode with the solid electrolyte on the surface of the solid electrode; and an active fluid distribution layer which is arranged between the solid electrolyte and the anode to realize effective transmission of ions and electrons. The invention also provides a beta battery comprising the anodic capillary layer.
Description
Technical field
The present invention relates to the beta batteries such as sodium-sulphur battery, more particularly, relate to a kind of anode capillary layer for beta batteries such as sodium-sulphur batteries, and the beta battery that comprises this anode capillary layer.
Background technology
Since eighties of last century the seventies, sodium-sulphur battery is as the typical beta battery of one, and high with its energy density, cycle efficieny is high, with low cost, and advantages of environment protection has caused countries in the world interest widely at the numerous areas such as electric automobile and energy storage.At present, only have a few countries such as Japan, the U.S. and China at research sodium-sulphur battery, and only have Japan by sodium-sulphur battery industrialization, and China is still among making great efforts.Final practical the faced key issue of sodium-sulphur battery is the fail safe that further reduces the internal resistance of cell and improve battery.For the anode of sodium-sulphur battery and other beta battery, improve the wetability between the solid electrolytes such as sodium and beta-aluminium oxide and ensure that the good contact between sodium and solid electrolyte is two very important problems.Taking beta-aluminium oxide as example, wetting missionary society between sodium and beta-aluminium oxide causes sodium and beta-aluminium oxide generation of interfaces seriously to polarize, make electric current finally destroy beta-aluminium oxide ceramics in a large amount of gathering of polarization place, thereby make battery failure, even produce safety problem.Therefore, do not increasing under the prerequisite of the internal resistance of cell, the wetability improving between the solid electrolytes such as sodium and beta-aluminium oxide becomes an important channel of improving beta battery safety.Meanwhile, for improving the utilance of sodium, solve the contact problems of the solid electrolytes such as sodium and beta-aluminium oxide, near the solid electrolytes such as beta-aluminium oxide, add the anode capillary layer of porous, utilize capillarity to ensure that sodium contacts with electrolytical.Research is found, does not introduce excess metal sodium, is the effective means of wetability first between the solid electrolytes such as raising sodium and beta-aluminium oxide and the solid electrolyte surfaces such as beta-aluminium oxide are modified.A lot of materials, comprise metal, oxide, carbide, nitride powder and porous nano metal etc., studied for modifying the solid electrolyte surfaces such as beta-aluminium oxide.Wherein, on the solid electrolytes such as beta-aluminium oxide, be coated the Na ion conductor amido sodium (PCT/GB 90/01584, WO 91/06133) of one deck lead or bismuth (UK Patent Application 2067005), low melting point and all reached good effect at its coated one deck porous nano metal (British patent 1530274 and 1511152) in surface etc.Porous material has larger specific area because of it, can improve more wetability compared with granular materials, can be used as anode capillary layer simultaneously, but between the solid electrolytes such as porous material and beta-aluminium oxide adhesion poor be the subject matter that always perplexs its application.For this problem, research worker before adopts physical deposition method, and as flame sputtering method and plasma sputtering etc., the surface of carrying out porous material is coated.But this class processing method technical matters is relatively complicated, cost is higher, generally need under high vacuum, operate, and can not meet the needs of practical large-scale application.Therefore, exploring the solid electrolyte surfaces such as a kind of and beta-aluminium oxide directly becomes in conjunction with the capillary transition zone of good porous the performance and the fail safe that improve Na-beta battery, reduces an important research problem of the internal resistance of cell.
Therefore, a kind of be directly combined well with the solid electrolyte such as beta-aluminium oxide in the urgent need to developing in this area, for the capillary layer of the beta galvanic anodes such as sodium sulphur, the wetability that this capillary layer can be realized between the solid electrolytes such as beta-aluminium oxide and sodium is significantly improved, ensure the good contact between sodium and solid electrolyte, under the prerequisite that does not increase the internal resistance of cell, improve interfacial polarization and the fail safe of Na-beta battery.
Summary of the invention
The invention provides a kind of novelty for the anode capillary layer of beta battery and the beta battery that comprises it, thereby solved problems of the prior art.
On the one hand, the invention provides a kind of anode capillary layer for beta battery, described beta battery comprises anode, solid electrolyte and negative electrode, and described anode capillary layer comprises:
Porous metal medium, described porous metal medium arranges along described solid electrolyte surface, to realize the good contact of described anode and described solid electrolyte on described solid electrolyte surface; And
Active fluid distribution layer, described active fluid distribution layer is arranged between described solid electrolyte and described anode, in order to realize effective transmission of ion and electronics.
One preferred embodiment in, described solid electrolyte directly contacts with described porous metal medium, to prevent that described anode capillary layer and solid electrolyte from departing from.
Another preferred embodiment in, described porous metal medium forms conductive network between described solid electrolyte and described anode.
Another preferred embodiment in, described porous metal medium is made up of nano level metallic fiber.
Another preferred embodiment in, the average cell size of described porous metal medium is greater than the molecular dimension of active fluid.
Another preferred embodiment in, described solid electrolyte is selected from sodium ion conductor pottery and sodium ion conductor glass, as beta-Al
2o
3or Na
5gdSi
4o
12.
Another preferred embodiment in, described porous metal medium is by upper reaches, described solid electrolyte surface, material that prolong, that apply or spraying forms.
Another preferred embodiment in, described porous metal medium chosen from Fe, cobalt, nickel, chromium, manganese and tungsten, and their alloy or mixture.
Another preferred embodiment in, described beta battery is selected from the Na-beta battery such as sodium-sulphur battery and sodium-chloride battery (ZEBRA battery).
On the other hand, the invention provides a kind of beta battery, it comprises above-mentioned anode capillary layer.
Brief description of the drawings
Fig. 1 is the electron scanning micrograph in the beta-aluminium oxide cross section of porous-metal nickel after coated in the embodiment of the present application 1.
Fig. 2 is the angle of wetting test picture between beta-aluminium oxide and sodium before and after coated porous metallic nickel in the application's comparative example and embodiment 1, and probe temperature is 300 DEG C.
Embodiment
The present inventor finds after having passed through extensive and deep research, in the beta batteries such as sodium-sulphur battery, at direct capillary transition zones in conjunction with good porous in solid electrolyte surface such as beta-aluminium oxide, this capillary layer comprises porous metal medium and active fluid distribution layer, the wetability that can realize between the solid electrolytes such as beta-aluminium oxide and sodium is significantly improved, and improves interfacial polarization and the fail safe of Na-beta battery under the prerequisite that does not increase the internal resistance of cell.Based on above-mentioned discovery, the present invention is accomplished.
In a first aspect of the present invention, a kind of anode capillary layer for beta batteries such as sodium-sulphur batteries is provided, described beta battery comprises solid electrolyte and the negative electrode such as anode, beta-aluminium oxide, wherein, described anode capillary layer comprises porous metal medium and active fluid distribution layer, wherein, described porous metal medium arranges along described solid electrolyte surface, to realize the good contact of described anode and described solid electrolyte on described solid electrolyte surface; Described active fluid distribution layer is arranged between described solid electrolyte and described anode, in order to realize effective transmission of ion and electronics.
In the present invention, described porous metal medium can be directly synthetic on solid electrolyte, and its thickness and even pore distribution, have good adhesion with described solid electrolyte.Described porous metal medium can improve the uniformity of described active fluid distribution layer on described solid electrolyte to a great extent, is issued to the object that reduces the beta battery interfacial polarizations such as sodium-sulphur battery in the prerequisite that does not increase the internal resistance of cell.
In the present invention, the solid electrolyte such as described beta-aluminium oxide directly contacts to prevent that with porous metal medium described capillary layer and solid electrolyte from departing from.
In the present invention, described porous metal medium forms conductive network between the solid electrolytes such as described beta-aluminium oxide and described anode.
In the present invention, described porous metal medium is made up of nano level metallic fiber.
In the present invention, the average cell size of described porous metal medium is greater than the molecular dimension of described active fluid.
In the present invention, described porous metal medium is arranged in the surf zone of described solid electrolyte, realizes being uniformly distributed of active fluid in described region.
In the present invention, described porous metal medium makes described active fluid in described solid electrolyte surface good wet, makes thus the interfacial polarization between them greatly reduce.
In the present invention, described solid electrolyte has electronic isolation and sodium ion-conductive, is selected from sodium ion conductor pottery and sodium ion conductor glass, for example beta-Al
2o
3and Na
5gdSi
4o
12.
In the present invention, described porous metal medium has good electrical conductance, metal and their alloys and mixts such as chosen from Fe, cobalt, nickel, chromium, manganese, tungsten.
In the present invention, described porous metal medium is by upper reaches, described solid electrolyte surface, material that prolong, that apply or spraying forms.
In a second aspect of the present invention, provide a kind of beta battery that comprises the above-mentioned anode capillary layer for beta batteries such as sodium-sulphur batteries.
Major advantage of the present invention is:
1) directly the adhesion of the coated solid electrolyte such as porous metal medium and beta-aluminium oxide is good, can effectively avoid decorative material contingent coming off and losing efficacy in battery operation process;
2) porous metal medium of even pore distribution can make sodium be evenly dispersed in the solid electrolyte surfaces such as beta-aluminium oxide, and can not block sodium ion-conductive passage;
3) metal medium has good conductive performance to electronics, can not increase the internal resistance of cell;
4) compared with traditional direct coating metal particles, porous metal medium of the present invention provides larger specific area, can significantly improve the wetability between sodium and electrolyte, and is conducive to keep in circulating battery process good wetability;
5) processing method is simple, and cost is low.
Embodiment
Further set forth the present invention below in conjunction with specific embodiment.But, should be understood that these embodiment only do not form limitation of the scope of the invention for the present invention is described.The test method of unreceipted actual conditions in the following example, conventionally according to normal condition, or the condition of advising according to manufacturer.Except as otherwise noted, all percentage and umber are by weight.
The solid electrolytes such as the beta-aluminium oxide using in following comparative example and embodiment provide by silicate research institute of the Chinese Academy of Sciences.
comparative example
The beta-alumina wafer polishing is repeatedly dry more than 4 hours in 80 DEG C of drying boxes after 30 minutes with absolute ethyl alcohol ultrasonic cleaning.In the glove box that is full of argon gas, test at 300 DEG C angle of wetting stable between beta-aluminium oxide and sodium.Test result as shown in Figure 2 (a) shows.From Fig. 2 (a), can find out, between the solid electrolytes such as untreated beta-aluminium oxide and sodium, angle of wetting is 151 °, almost completely nonwetting.
embodiment 1
The same comparative example of cleaning condition of Beta-aluminium oxide.The porous-metal nickel medium that is 5-10 μ m by aperture by the method applying is coated on beta-alumina surface and obtains testing the sample of angle of wetting.
According to the angle of wetting between the method test sample of comparative example and sodium, the same comparative example of test condition, test result is as shown in table 1 below.Can be found out by data in table 1, the angle of wetting between beta-alumina sample and the sodium of the coated porous metallic nickel medium that the present embodiment obtains has reduced 73.5% compared with before coated.
Fig. 1 is the cross section scanning electron photo that is coated on the porous-metal nickel medium of beta-alumina surface in the present embodiment.In figure, the thickness of porous-metal nickel medium is about 6 μ m, presents network structure.
Fig. 2 (b) be in the present embodiment the beta-aluminium oxide of porous-metal nickel medium after coated at 300 DEG C with the test photo of sodium angle of wetting.From photo, can find, after coated porous metallic nickel medium, the angle of wetting of beta-aluminium oxide and sodium is about 40 °, compares ratio, and wettability has clear improvement.
embodiment 2
The same comparative example of cleaning condition of Beta-aluminium oxide.The porous-metal nickel medium that is 4-15 μ m by aperture by the method for curtain coating is coated on beta-alumina surface and obtains testing the sample of angle of wetting.
According to the angle of wetting between the method test sample of comparative example and sodium, the same comparative example of test condition, test result is as shown in table 1 below.Can be found out by data in table 1, the angle of wetting between beta-alumina sample and the sodium of the coated porous metallic nickel medium that the present embodiment obtains has reduced 76.8% compared with before coated.
embodiment 3
The same comparative example of cleaning condition of Beta-aluminium oxide.The porous metals iron medium that is 5-10 μ m by aperture by the method applying is coated on beta-alumina surface and obtains testing the sample of angle of wetting.
According to the angle of wetting between the method test sample of comparative example and sodium, the same comparative example of test condition, test result is as shown in table 1 below.Can be found out by data in table 1, the angle of wetting between beta-alumina sample and the sodium of the coated porous metallic iron medium that the present embodiment obtains has reduced 65.6% compared with before coated.
embodiment 4
The same comparative example of cleaning condition of Beta-aluminium oxide.The porous metals iron medium that is 6-12 μ m by aperture by the method for curtain coating is coated on beta-alumina surface and obtains testing the sample of angle of wetting.
According to the angle of wetting between the method test sample of comparative example and sodium, the same comparative example of test condition, test result is as shown in table 1 below.Can be found out by data in table 1, the angle of wetting between beta-alumina sample and the sodium of the coated porous metallic iron medium that the present embodiment obtains has reduced 66.9% compared with before coated.
embodiment 5
The same comparative example of cleaning condition of Beta-aluminium oxide.By the method for curtain coating, the porous metals cobalt medium that is applied to 8-15 μ m is coated on to beta-alumina surface and obtains testing the sample of angle of wetting.
According to the angle of wetting between the method test sample of comparative example and sodium, the same comparative example of test condition, test result is as shown in table 1 below.Can be found out by data in table 1, the angle of wetting between beta-alumina sample and the sodium of the coated porous metallic cobalt medium that the present embodiment obtains has reduced 69.5% compared with before coated.
embodiment 6
The same comparative example of cleaning condition of Beta-aluminium oxide.The porous metals chromium medium that is 5-10 μ m by aperture by the method for curtain coating is coated on beta-alumina surface and obtains testing the sample of angle of wetting.
According to the angle of wetting between the method test sample of comparative example and sodium, the same comparative example of test condition, test result is as shown in table 1 below.Can be found out by data in table 1, the angle of wetting between beta-alumina sample and the sodium of the coated porous crome metal medium that the present embodiment obtains has reduced 74.8% compared with before coated.
embodiment 7
The same comparative example of cleaning condition of Beta-aluminium oxide.The porous metals tungsten medium that is 7-16 μ m by aperture by the method applying is coated on beta-alumina surface and obtains testing the sample of angle of wetting.
According to the angle of wetting between the method test sample of comparative example and sodium, the same comparative example of test condition, test result is as shown in table 1 below.Can be found out by data in table 1, the angle of wetting between beta-alumina sample and the sodium of the coated porous tungsten medium that the present embodiment obtains has reduced 70.2% compared with before coated.
embodiment 8
By Na
5gdSi
4o
12glass cleans, the same comparative example of cleaning condition.The porous-metal nickel medium that is 5-10 μ m by aperture by the method applying is coated on solid electrolyte glass surface and obtains testing the sample of angle of wetting.
According to the angle of wetting between the method test sample of comparative example and sodium, the same comparative example of test condition, test result is as shown in table 1 below.Can be found out by data in table 1, the angle of wetting between glass sample and the sodium of the coated porous metallic nickel medium that the present embodiment obtains has reduced 73% compared with before coated.
Table 1: the aperture of the corresponding experiment parameter of embodiment 1-8 and sample and film base combination degree
| Sample | Angle of wetting/(°) | Angle of wetting reduces (%) |
| Comparative example | 151 | / |
| Embodiment 1 | 40 | 73.5 |
| Embodiment 2 | 35 | 76.8 |
| Embodiment 3 | 52 | 65.6 |
| Embodiment 4 | 50 | 66.9 |
| Embodiment 5 | 46 | 69.5 |
| Embodiment 6 | 38 | 74.8 |
| Embodiment 7 | 45 | 70.2 |
| Embodiment 8 | 41 | 73 |
From upper table 1, the porous metal medium that utilizes the present invention to distribute on solid electrolyte surfaces such as beta-aluminium oxide, contacting between active fluid and described solid electrolyte can be improved significantly, can be directly as the anode capillary layer of the beta batteries such as sodium sulphur.
All documents of mentioning in the present invention are all quoted as a reference in this application, are just quoted separately as a reference as each section of document.In addition should be understood that those skilled in the art can make various changes or modifications the present invention after having read above-mentioned instruction content of the present invention, these equivalent form of values fall within the application's appended claims limited range equally.
Claims (9)
1. for an anode capillary layer for beta battery, described beta battery comprises anode, solid electrolyte and negative electrode, it is characterized in that, described anode capillary layer comprises:
Porous metal medium, described porous metal medium arranges along described solid electrolyte surface, formed by nano level metallic fiber, by forming at upper reaches, described solid electrolyte surface material that prolong or that apply, to realize the good contact of described anode and described solid electrolyte on described solid electrolyte surface; And
Active fluid distribution layer, described active fluid distribution layer is arranged between described solid electrolyte and described anode, in order to realize effective transmission of ion and electronics.
2. anode capillary layer as claimed in claim 1, is characterized in that, described solid electrolyte directly contacts with described porous metal medium, to prevent that described anode capillary layer and solid electrolyte from departing from.
3. anode capillary layer as claimed in claim 1, is characterized in that, described porous metal medium forms conductive network between described solid electrolyte and described anode.
4. anode capillary layer as claimed in claim 1, is characterized in that, the average cell size of described porous metal medium is greater than the molecular dimension of active fluid.
5. anode capillary layer as claimed in claim 1, is characterized in that, described solid electrolyte is selected from sodium ion conductor pottery and sodium ion conductor glass.
6. anode capillary layer as claimed in claim 5, is characterized in that, described solid electrolyte is beta-Al
2o
3or Na
5gdSi
4o
12.
7. anode capillary layer as claimed in claim 1, is characterized in that, described porous metal medium chosen from Fe, cobalt, nickel, chromium, manganese and tungsten, and their alloy or mixture.
8. the anode capillary layer as described in any one in claim 1-7, is characterized in that, described beta battery is selected from sodium-sulphur battery and sodium-chloride battery.
9. a beta battery, is characterized in that, it comprises the anode capillary layer described in any one in claim 1-8.
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| CN201210157239.0A CN102646833B (en) | 2012-05-17 | 2012-05-17 | Anodic capillary layer for beta battery and beta battery comprising same |
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Families Citing this family (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103117416B (en) * | 2012-12-12 | 2015-06-17 | 上海电气钠硫储能技术有限公司 | Sodium injection method for negative electrode of sodium-sulphur battery |
| CN104282953B (en) * | 2013-07-09 | 2016-09-07 | 中国科学院上海硅酸盐研究所 | Comprise sode cell of asymmetric decorative layer and preparation method thereof |
| CN104282938B (en) * | 2013-07-09 | 2016-08-10 | 中国科学院上海硅酸盐研究所 | Interplantation preparation is for the method for the solid electrolyte comprising rich metal-modified layer of sode cell |
| CN106711517B (en) * | 2015-11-16 | 2019-03-22 | 上海奥能瑞拉能源科技有限公司 | Improve the method and tubular type na chloride battery of tubular type na chloride cell power density |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB1511152A (en) * | 1975-04-24 | 1978-05-17 | Chloride Silent Power Ltd | Alkali metal-sulphur cells |
| CN2445452Y (en) * | 2000-08-28 | 2001-08-29 | 陈会林 | Sodium sulfur high-energy battery |
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2012
- 2012-05-17 CN CN201210157239.0A patent/CN102646833B/en active Active
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB1511152A (en) * | 1975-04-24 | 1978-05-17 | Chloride Silent Power Ltd | Alkali metal-sulphur cells |
| CN2445452Y (en) * | 2000-08-28 | 2001-08-29 | 陈会林 | Sodium sulfur high-energy battery |
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