CN102044659B - Electrode including ring catch - Google Patents

Electrode including ring catch Download PDF

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Publication number
CN102044659B
CN102044659B CN201010519800.6A CN201010519800A CN102044659B CN 102044659 B CN102044659 B CN 102044659B CN 201010519800 A CN201010519800 A CN 201010519800A CN 102044659 B CN102044659 B CN 102044659B
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silk
interlayer
support
donor
ring
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CN102044659A (en
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罗纳德·安东尼·罗杰斯基
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Priority claimed from US12/904,113 external-priority patent/US8481214B2/en
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0471—Processes of manufacture in general involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0421—Methods of deposition of the material involving vapour deposition
    • H01M4/0423—Physical vapour deposition
    • H01M4/0426—Sputtering
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0421—Methods of deposition of the material involving vapour deposition
    • H01M4/0428—Chemical vapour deposition
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Abstract

A kind of electrode including ring catch, including configuration for preventing the interlayer structure from electrode separation and/or configuration for creating the structure with the region that less concentration sandwiches material on electrode.This electrode includes supporting silk, arranges interlayer on support silk.Support that silk has nano-grade size alternatively.

Description

Electrode including ring catch
The cross reference of related application
This application claims that submit on October 22nd, 2009, name and be called the rights and interests of U.S. Provisional Patent Application No.61/254,090 and the priority of " ElectrodesIncludingCollarStop "；And the application on February 25th, 2009 submit to, name is called the U.S. Patent application No.12/392 of " HighCapacityElectrodes ", the part continuation application of 525, this U.S. Patent No. 12/392,525 require in the U.S. Provisional Patent Application 61/067 that on February 25th, 2008 submits to, 018 and the priority of U.S. Provisional Patent Application 61/130,679 submitted on June 2nd, 2008 and rights and interests.All above-mentioned interim and non-provisional it is incorporated by reference at this.
Technical field
The invention belongs to electrode technology field.
Summary of the invention
The various embodiments of the present invention include a kind of electrode, and this electrode includes: substrate；It coupled to the support silk (filament) of substrate；Including the interlayer of donor-acceptor material, the configuration of this donor-acceptor material is for receiving the reactant (such as, ion, electronics, electric charge donor and/or charge receptor) of electrochemical reaction, and donor-acceptor material is arranged along the length direction supporting silk；And the sandwiched area close to substrate, and relative to the sandwiched area away from substrate, it includes less amount of donor-acceptor material.
The various embodiments of the present invention include a kind of method producing electrode, and the method includes: receive substrate；Growth coupled to the first area of the support silk of substrate；Away from the terminal growth ring catch of substrate in the first area supporting silk, the configuration of this ring catch is for reducing the amount of the donor-acceptor material arriving first area；Support the second area of silk from ring catch growth, the second area of ring catch has the diameter less than ring catch；And by donor-acceptor materials application to supporting silk, so that relative to the donor-acceptor material depositing larger thickness in the first area supporting silk in the second area supporting silk.
The various embodiments of the present invention include a kind of battery, and this battery includes the first electrode and the second electrode, and the second electrode includes: substrate；It coupled to the support silk of this substrate；Configuration is for receiving the interlayer of the reactant of electrochemical reaction, and this interlayer is arranged on support silk；And for device that create the sandwiched area close to substrate, include less amount of donor-acceptor material relative to the sandwiched area away from substrate.
Accompanying drawing explanation
Fig. 1 illustrates the support cap electrode design according to the various embodiment of the present invention.
Fig. 2 illustrates the support ring electrode design according to the various embodiment of the present invention.
Fig. 3 illustrates the ring catch electrode design according to the various embodiment of the present invention.
Fig. 4 illustrates the support cap according to the various embodiment of the present invention and supports ring electrode design.
Fig. 5 illustrates the support cap according to the various embodiment of the present invention and ring catch electrode design.
Fig. 6 illustrates the support ring according to the various embodiment of the present invention and ring catch electrode design.
Fig. 7 A, Fig. 7 B and Fig. 7 C illustrate the electrode including sandwiching material according to the various embodiment of the present invention.
Fig. 8 illustrates the method creating electrode extension according to the various embodiment of the present invention.
Fig. 9 A, Fig. 9 B illustrate the measured charge capacity according to the various embodiment of the present invention and the relation sandwiching material thickness.
Figure 10 illustrates the battery cycle life according to the various embodiment of the present invention and the relation sandwiching material thickness.
Figure 11 illustrates a kind of battery according to the various embodiment of the present invention.
Figure 12 A and Figure 12 B illustrates the carbon nano-fiber of growth in copper substrate according to the various embodiment of the present invention.
Figure 13 A and Figure 13 B illustrate according to the various embodiment of the present invention be coated with sandwich material, in copper substrate growth carbon nano-fiber.
Figure 14 illustrates the sectional view of the electrode without interlayer 750 for collecting the data for Fig. 9 A, Fig. 9 B and Figure 10 according to the various embodiment of the present invention.
Detailed description of the invention
Fig. 1 illustrates the electrode including supporting silk 110.Support that silk 110 includes supporting cap 150.Support that cap 150 is the extension supporting silk 110 alternatively, and have more than supporting filament diameter 112 about 1%, 2.5%, 10%, 25%, 40% or the support cap width 157 up to 60%.Support that silk height 114 includes supporting cap height 155.In some embodiments, support that cap height 155 is at least 250 nanometers, 500 nanometers, 2000 nanometers or 5000 nanometers.In other embodiments, support that cap height 155 is at least percent the 1 of silk height 114,5,20,30 or 50.Support that cap width 157 can be at least percent the 1 of starting point separation distance 126,5,15,40 or 75.Starting point is to start growth in Seed Layer 122 to support the position of silk.The shape of cross section of support cap 150 (as shown in Figure 1) can be rectangle, triangle, square, circular or rhombus.Other shapes are also possible.Support cap 150 can configure be used for preventing interlayer 750 (Fig. 7) skid off support silk 110 be not connected with end.
Support that silk 110 can be CNT (CNT), carbon nano-fiber (CNF) or nano wire (NW), or other nanoscale structures.Material including CNT is usually carbon, and can include other materials, metal, quasiconductor and the insulator such as inputted in feed gas during the growth of CNT.It addition, CNT can be single wall or many walls.Material including CNF is usually carbon, and can include other materials, metal, quasiconductor and the insulator such as inputted in feed gas during the growth of CNF.CNT is commonly described as the diameter with at least 2nm, 5nm, 10nm, 30nm or 50nm.CNF is commonly described as the diameter with at least 30nm, 50nm, 150nm, 250nm, 500nm or 750nm.Nano wire (NW) can include metal (such as gold, copper or stannum) or quasiconductor (such as silicon, germanium, Inp, GaN, GaP, ZnO) or oxide, such as MnO2, indium tin oxide, ZnO, SnO2、Fe2O3、In2O3Or Ga2O3.Other materials is also possible.
Fig. 2 illustrates an electrode including supporting silk 110, and this support silk 110 includes supporting ring 210.Supporting that ring 210 is the extension supporting silk 110 alternatively, it has more than the diameter supporting filament diameter 112 at least 1%, 2.5%, 10%, 25%, 40% or 60%.In some embodiments, support that ring height 214 is at least 100,250,500,2000 or 5000 nanometers, it is possible to bigger, and can be as small as 50 nanometers, it is possible to be less.In some embodiments, support that ring height 214 is at least supporting percent the 1 of silk height 114,5,15,40 or 75.Support that ring width 212 can be at least the 1% of starting point separation distance 126,5%, 15%, 40% or 75%.Support the shape of ring 210 can be rectangle, square, circular, triangle, annular, rhombus, bending etc..Other shapes are also possible.Support that ring fundamental distance 216 is at least supporting the half of silk height 114 alternatively.Ring fundamental distance 216 is to support that the 10% of silk height 114,30% or 75% is possible.Fundamental distance 216 can extend at least 500,1000,2500,5000 or 12500 nanometers from starting point 120.Additionally, fundamental distance 216 extends end in some microns of most advanced and sophisticated 152 at silk is possible.
Fig. 3 illustrates an electrode including supporting silk 110, and this support silk 110 includes ring catch 310.Ring catch 310 is by a region of the support silk 110 characterized more than the diameter of other regional diameters supporting silk 110.In some embodiments, the diameter of ring catch 310 at least above percent 1 of support silk 110 diameter (such as, support filament diameter 112) in other regions one or more supporting silk 110,2.5,10,25,40 or 60.The diameter and the ring catch interval 312 that control ring catch 310 create trunk 350.This trunk 350 will result in the region that donor-acceptor material (DAM) reduces.It is wherein there is sandwiching material but being not necessarily entirely without the region sandwiching material of minimizing amount relative to other regions supporting silk that DAM reduces region.Such as, in various embodiments, DAM region can include relative to supporting other regions of silk 110 less than percent 75,50,25,10 or 5 (supporting the weight of the per unit area of silk 110) sandwich material.(for purposes of illustration, sandwich material be defined as supply or accept electric charge to complete the material of the external circuit of electrode.Sandwich material configuration for the exchange of electrolyte electric charge carrier of surrounding, electric charge donor and/or electric charge receiving body.Sandwich material and can permeate these materials alternatively).Ring catch interval 312 can close to 0, or percent the 10 of the distance being at least between starting point 126,50,75 or 95.Ring catch 310 can grow the optional position in the length supporting silk 110, for instance, in some embodiments, ring catch 310 can be arranged in the 10000 of starting point 120,5000,2000,1000,750,250,100,25 or 5 nanometers.
The method creating ring catch 310 is generally similar to create the method supported ring 210 or support cap 150.Control to support ring 210, support that the method for the diameter of cap 150 and/or ring catch 310 can include changing the temperature of feed gas, substrate or reative cell (or combination of three), or change the flow velocity of various feed gas.Such as, the composition changing feed gas during supporting the growth of silk 110 can also control these diameters.Control supports that the other method of the diameter of silk 110, ring catch 310, support ring 210 and/or support cap 150 is to apply static state or dynamic electric field, applies static state or dynamic magnetic field or the combination in applying electric field and magnetic field.Those of ordinary skill in the art will be clear to by the additive method controlling these diameters.
Ring catch 310, support ring 210 and support cap 150 alternatively with support that silk 110 is identical material, but be depending on the concrete technology realized, it is possible to use other materials and ratio thereof.Such as, different feed gas can use in the different process time, such as utilizes acetylene, ethylene or ethanol to replace methane (when CNT/CNF grows).It addition, different process gas can use in the different time.Such as, argon can utilize the process gas of such as ammonia, nitrogen or hydrogen etc to replace.Different gas can be used to mix according to desired effect.CNT/CNF grows those of skill in the art and is appreciated that, it is possible to use other feed gas and process gas.
Ring catch thickness 314 will typically be less than some microns, but can be support percent the 1 of silk height 114,5,10,26,50 or 75.In some embodiments, ring catch thickness 314 is less than supporting percent the 40 of silk height 114,20,5,2 or 0.25.According to the growth rate supporting silk 110, the cross section of the ring catch 310 as shown in the plane of Fig. 3 can be oval, rhombus or square.Other shape of cross sections are possible.Support cap 150 and support that ring 210 and ring catch 310 have these shape and size alternatively.
Ring catch diameter 316 is controlled for the process creating ring catch 310 by selection.Such as, during the growth of ring catch 310, thus it is possible to vary the temperature of reative cell, to accelerate or to slow down to create the reaction supporting silk 110, thus creates the diameter region more than the support silk 110 in other regions supporting silk 110.Such as, support that silk 110 can include the relatively narrow diameter region separated by the ring catch 310 with considerable larger diameter.Alternatively, support that silk can include the region (ring catch 310 can less than or close to the same diameter in this region) with relatively large diameter between substrate 124 and ring catch 310 and the region with small diameter away from substrate 124.Support that filament diameter 112 is defined as along the minimum diameter supporting silk.
Ring catch interval 312 is controlled by starting point interval 126 and ring catch diameter 316.Being sized to of ring catch 310 so that relative to the region of the support silk 110 away from substrate 124, occurs the DAM reduced to add between ring catch 310 and substrate 124.Single support silk 110 can include more than one ring catch 310 and/or more than one supports ring 210.
In the embodiment as shown, trunk 350 is substantially will not have DAM material or relative to supporting that silk 110 part (away from substrate 124) on ring catch 310 has the region of the DAM material of minimizing amount.This will have been selected by ring catch diameter 316 and the suitable of ring catch interval 312.Such as, ring catch interval 312 and ring catch diameter 316 can be chosen as so that specific ring catch 310 has just contacted its immediate adjacent annular block piece, effectively to create the ring catch interval 312 equal to 0.Alternatively, ring catch interval 312 can more than 0.Ring catch 310 is formed and decreases the barrier layer arriving the DAM amount supporting the silk 110 region between ring catch 310 and substrate 124 relative to other parts supporting silk 110.
Fig. 4 illustrates the various embodiments of the present invention, wherein supports that silk 110 has support cap 150 and supports ring 210, but does not have ring catch 310.
Fig. 5 illustrates the various embodiments of the present invention, wherein supports that silk 110 has support cap 150 and ring catch 310, but does not have support ring 210.
Fig. 6 illustrates the various embodiments of the present invention, wherein supports that silk 110 has support ring 210 and ring catch 310, but does not have support cap 150.Fig. 4-Fig. 6 illustrates and supports the support cap 150 that can include on silk 110, the combination in any supporting ring 210 and ring catch 310.These combinations can include in these elements one, two, three or more.Single support silk 110 can include more than one ring catch 310 and/or more than one supports ring 210.The position supporting ring 210 and ring catch 310 upwardly or downwardly can change relative to the position shown in figure in the length supporting silk 110.Ring catch 310 and support ring 210 are generally around the longitudinal axis Cylindrical symmetry supporting silk 110.
Fig. 7 A illustrates and includes the interlayer 750 of DAM, ring catch 310, support cap 150 and support ring 210.This diagram has been represented graphically the basic function on ring catch 310, such as, interlayer 750 is deposition/growth on support silk 110 top supporting between cap 150 and ring catch 310 substantially, and do not deposit in ring catch 310 area below (or less)/grow, thus create sandwich material relatively fewer or be substantially free of sandwich material DAM reduce region 720.By suitably selecting ring catch diameter 316 and ring catch interval 312, create mask so that minimum (or less) sandwiches material and arrive substrate 124.
It is the region supporting to prevent interlayer 750 from depositing on silk 110 that DAM reduces region 720.Generally, DAM reduces the contiguous Seed Layer 122 in region 720.
Fig. 7 A also show and supports cap 150 and support the use of ring 210.Support cap 150 and support that ring 210 is all characterized by the diameter of the diameter 112 more than other parts supporting silk 110.In some embodiments, it is assumed that interlayer 750 expands during Electrode Operation, then interlayer will separate with the diameter supporting silk 110.In some embodiments, as long as supporting ring width 212 and/or supporting the diameter internal diameter sandwiching material more than expansion of cap width 157, interlayer 750 just will mechanically be constrained to support silk 110, therefore ensure that sandwiching material will not separate with support silk 110.
Ring catch 310 is similar with supporting ring 210 size and/or shape alternatively.A difference between ring catch 310 and support ring 210 is in that to support that on certain position that ring 210 is arranged in support silk 110, (or being otherwise configured to) makes its support interlayer 750 be attached on support silk 110.Such as, support ring 210 configuration for prevent interlayer 750 skid off support silk 110 be not connected with end.On the contrary, ring catch 310 arranges that (or otherwise configuration) is in certain position supporting silk 110 so that its region producing in support silk 110 region between ring catch 310 and substrate 124 to have the interlayer 750 of minimizing relative to other parts supporting silk 110.In lesser extent, support that ring 210 can also produce the region of the interlayer 750 slightly reduced.
Freely sandwiching material 710 is the material not stoped by ring catch 310 during the deposition/growth of interlayer 750.Material source for the deposition/growth of interlayer 750 generally regards as on self-supporting silk 110 (above the page), as shown in Fig. 7 A-Fig. 7 C.
Fig. 7 C illustrates the alternate embodiment supporting silk 110.These embodiments include the example with the support silk that more than one supports ring and taper.The various different examples of the support silk 110 shown in Fig. 7 B and Fig. 7 C are not generally on identical electrode.One electrode generally includes a type of support silk 110, supports ring 210, supports cap 150 and ring catch 310, because all of support silk generates together.The purpose that variant shown here is merely cited for.The thickness of the interlayer 750 shown in Fig. 7 A-Fig. 7 C has been also only descriptive purpose.In typical embodiment, interlayer 750 ratio significantly supports that silk 110 is thick.Along with charged matter is absorbed and discharges, the thickness of interlayer 750 also will change.It is also important to note that interlayer 750 thickness described here is for the situation not having charged matter to be absorbed by interlayer 750 or discharge.
Fig. 8 illustrates the method for manufacturing the support silk with interlayer 750.First step 801 is to receive substrate 124.Substrate 124 is copper alternatively when anode, or is aluminum alternatively when negative electrode.According to desired application, substrate can be other materials.For example, it is possible to rustless steel or graphite are used as substrate.According to desired application, battery design those skilled in the art can also specify other materials.
Optional second step 803 is cleaning substrate.The purpose clearing up 803 substrates is in that subsequent deposition and growth for the material in processing step subsequently and preparing substrate.This means other pollutant removed any Organic substance, oxide and be present on current colelctor electrode.The scope clearing up the method for substrate can include (the use solvent of (such as use and grind to remove the material thin-layer being exposed to pollutant) of physics, chemistry, such as acetone, isopropanol, TCE or methanol) and/or chemical etching (citric acid immersion/rinse, in a case of copper, it has dissolved part actual substrate), or the combination in any of physics and chemical method, thus the processing step being follow-up prepares surface.
Third step 805 is optional seed layer deposition.Seed layer deposition 805 is to create the processing step for the basic unit supporting silk 110 to grow or Seed Layer 122.This processing step can be realized by gas phase (physics or chemistry) deposition/growth, liquid deposition/growth or solid precipitation/growth or its combination in any.
Physical gas phase deposition technology (material wherein deposited is delivered to substrate with gas phase from source) may include that thermal evaporation, electron beam evaporation, DC sputtering, DC magnetron sputtering, RF sputtering, pulsed laser deposition, cathodic arc deposition etc..It is also possible for using reaction physical vapor deposition and following methods, and the method is passed through to be injected in room by " dusty gas " during growth technique, thus along with himself is incorporated in layer by its growth.
Chemical vapour deposition technique (wherein chemical precursor with gas-phase transport to surface, and subsequently then surface experience chemical reaction) can include low-pressure chemical vapor deposition, plasma enhanced chemical vapor deposition, Atmospheric pressure chemical vapor deposition, metalorganic chemical vapor deposition, hot line chemical vapor deposition, very high frequency plasma enhancing chemical vapor deposition, microwave plasma enhanced chemical vapor deposition etc..
The liquid-phase deposition technique creating Seed Layer 122 can include plating, plating or chemical solution deposition etc..Solid precipitation technology can include focused ion beam deposition.Another possibility is that of deposition comprises liquid and the solution of the appropriately sized particle that suspends, and it is sprayed on current colelctor electrode, and substrate " solidification " subsequently then so that carrier solution is removed, and particle is intactly stayed on the surface of a substrate.
The combination in any of process above step may be used for creating suitable Seed Layer 122, for the starting point created for supporting silk 110 to grow.
The 4th step 815 in technique is to create starting point.This step depends on the selected method for creating Seed Layer 122.Such as, starting point separation distance 126 can be determined by the selected thickness for seed layer deposition 805 and material.Such as, the Seed Layer of 3000 angstroms of nickel/300 angstrom chromium will produce every square centimeter of certain number of starting point.If the thickness of nickel reduces to 2000 angstroms, then the starting point number of every square centimeter is by different from the nickel of 3000 angstroms of thickness.If selecting another material, such as ferrum replaces nickel, then the starting point of produced every square centimeter is also by difference.Step 815 is a part for step 805 alternatively.
Solid precipitation technology can allow to control the starting point of every square centimeter.This can be focused ion beam deposition, wherein starting point/cm2Directly controlled by the position of its material of focused ion beam deposition；Or can be that nanoparticle suspends, wherein starting point/cm2Controlled by the number of the nanoparticle comprised in given suspension volume.The number of starting point can also be controlled by the size etc. of nanoparticle in the size of focused ion beam deposition point or solution.
The reactant generally manufacturing electrode wherein arrives and the applicable reaction temperature of the feed gas stream being suitable for, and when feed gas starts catalysis Seed Layer 122, creates starting point.Thus create starting point, and started to support that silk 110 grows.
5th step 820 is that silk 110 is supported in growth.Growth supports that silk 110 exists numerous available growth technique.Such as, chemical vapor deposition, heat chemistry gas deposition, vapour phase-liquid-solid growth (a kind of type of CVD) and plasma enhanced chemical vapor deposition are can to realize, by it, the technique that CNT (CNT), carbon nano-fiber (CNF) and nano wire (NW) grow.It will be recognized that there is other available growing methods in silk growth those skilled in the art.
May be used for the example of the feed gas of growth CNT/CNF is carbon monoxide, methane, ethane, ethylene, acetylene etc..Using other Hydrocarbon or inorganic compound is also possible for growth technique.
Interested is plasma enhanced chemical vapor deposition (CVD) method, owing to supporting that the growth of silk 110 is directed at the electric field of plasma, so allowing to produce vertically aligned support silk 110.Under specific process conditions, hot CVD can also produce vertically aligned support silk 110.It addition, water assisted CVD makes the perpendicular alignmnet with very high aspect ratio support that silk (length/diameter is approximately equal to 1,000,000) is possibly realized, it is allowed to produce very high support silk.
It also shows that the antibacterial suitably changed and virus have been grown to nano thread structure.This type of technology may be used for creating supports silk 110.
By properly selecting material, some technology once can be used together.Such as, when applying electric field, antibacterial/virus may be used for growth CNT/CNF/NW, in order to produce vertically aligned support silk.Supporting that the other method that silk 110 grows is to apply electric field and/or magnetic field during VLS grows, to control the track of growth CNT/CNF/NW, this controls the 3D shape of support silk 110.Another technology is to utilize the reactant of operation in PECVD pattern to support the growth of silk 110 to start CNT/CNF/NW；After at the appointed time, reactant may switch to hot CVD pattern；And then again at the appointed time after, reactant converts back PECVD pattern.CNT/CNF/NW grows those of skill will appreciate that of field, there are other possible combinations and allows to support the suitable Growth Control of silk 110.
The height 114 supporting silk 110 is generally determined by the persistent period of growth technique.The combination of the temperature of reactant, the feed gas used and the electric field applied and magnetic field (or it is absent from) and intensity can affect speed and the amount of silk growth.
If nanoparticle suspension process is selected for establishment Seed Layer 122, then support the diameter 112 of silk 110 generally by the thickness of Seed Layer 122 or be included in the size of nanoparticle in suspension and determine, if or focused ion beam deposition is selected for establishment Seed Layer 122, then being determined the diameter 112 supporting silk 110 by the size of ion beam.The combination of the temperature of reactant, the feed gas used and the electric field applied and magnetic field (or it is absent from) and intensity can also affect the diameter supporting silk 110.
During supporting the growth step 820 of silk 110, it is possible to realize sub-step 820a, wherein growth ring catch 310.This direction and intensity that can pass through to change the temperature of reactant, the feed gas used and relative composition and flow rate and the electric field applied and magnetic field (or it is absent from) realizes.The persistent period implicit expression changed determines ring catch thickness 314 and ring catch diameter 316.Ring catch interval is changed the persistent period to ready state (and changing the persistent period of self) by above-mentioned parameter and controls, and is controlled by starting point spacing distance 126.Sub-step 820a can be repeated.
During supporting the growth step 820 of silk 110, it is possible to realize sub-step 820b, wherein ring 210 is supported in growth；If step 820b occurs, then this will occur after step 820a.Sub-step 820b is by changing the temperature of reactant, changing the feed gas that uses and composition and change combination and the intensity of electric field and magnetic field (or it is absent from) applied and realize relatively thereof.Support that the diameter of ring 210, thickness and going up highly largely is controlled by the change of above-mentioned parameter.
During supporting the growth step 820 of silk 110, it is possible to realize sub-step 820c, wherein cap 150 is supported in growth；If step 820c occurs, then this will occur after step 820b.This temperature that can pass through to change reactant, changes the feed gas that uses and relatively forms, and changes the electric field applied and the combination of magnetic field (or it is absent from), direction and intensity realize.Support the diameter of cap 150, thickness and controlled by the change of above-mentioned parameter highly alternatively.
Can realizing the arbitrary steps in three step 820a, 820b and 820c, no matter other step 820a, 820b and 820c exist or are absent from.For example, it is possible to perform step 820a and do not perform step 820b or step 820c.It is alternatively possible to perform step 820a and 820c, and do not perform step 820b, or may decide that execution step 820b, and do not perform step 820a or 820c.It is alternatively possible to determine any step not realizing in sub-step 820a, 820b and 820c, thus create and there is support silk 110 along its length that minimize diameter change.
6th step 825 is to create DAM to reduce region 720, it is noted that DAM reduces region 720 corresponding to trunk 350.(reason of the difference between element 350 and 370 is in that DAM reduces region 720 and creates during the deposition of interlayer 750, and trunk 350 and the shape common definition supporting silk 110.When adding interlayer 750, trunk 350 will become DAM and reduce region 720.Specifically, trunk 350 is the part supporting silk 110, and DAM reduces region 720 and refers to the region wherein reducing or being absent to sandwich material 750).DAM region is created processing step 825 and can be realized by some methods, includes but not limited to use ring catch 310.The example of this type of method includes, in growth and orientated deposition (such as evaporation or the ion beam depositing) period sandwiching material, controlling to support the aspect ratio of silk 110.Additional method includes electro-deposition and the electroless deposition at bottom place, to isolate trunk 350.Being likely to perform the sputtering/photoengraving of mask layer, to open support silk 110 to interlayer 750 grown/deposited, or it is alternatively possible to amendment supports that the growth parameter(s) of silk 110 is to realize useful aspect ratio (such as tree).This can be undertaken by the composition of the feed used between change trophophase and process gas.Another possible method is to create DAM minimizing region 720, to perform to sandwich the deposition of material and directed eat-back (such as reactive ion etching), supports that silk 110 is covered by interlayer 750 to exempt.DAM reduces the establishment in region 729 and depends on selecting the method and structure for CNT/CNF/NW growth, and is selected for the method and structure of interlayer deposition.Such as, after deposition interlayer 750, for instance it can be possible for creating DAM minimizing region 720 via applicable directed etching (such as reactive ion etching or sense coupling).
8th processing step 830 is deposition/growth interlayer 750.(noting, DAM refers to the material supplying or accepting ion during battery charging and discharging, and wherein interlayer 750 includes DAM and can provide other layers of attachment, or can provide the layer increasing absorption, or can improve the layer of electric conductivity.Other purposes of layer are possible.These extra plays can deposition DAM on or under).
The growth of interlayer 750 can be realized by gas phase (physics or chemistry) deposition/growth, liquid deposition/growth or solid precipitation/growth or its combination in any.
Physical gas phase deposition technology (material wherein deposited is delivered to substrate with gas phase from source) may include that thermal evaporation, electron beam evaporation, DC sputtering, DC magnetron sputtering, RF sputtering, pulsed laser deposition, cathodic arc deposition etc..It is also possible for using reaction physical vapor deposition and following methods, and the method is passed through to be injected in room by " dusty gas " during growth technique, thus along with himself is incorporated in layer by its growth.
Chemical vapour deposition technique (wherein chemical precursor with gas-phase transport to surface, and subsequently then surface experience chemical reaction) can include low-pressure chemical vapor deposition, plasma enhanced chemical vapor deposition, Atmospheric pressure chemical vapor deposition, metalorganic chemical vapor deposition, hot line chemical vapor deposition, very high frequency plasma enhancing chemical vapor deposition, microwave plasma enhanced chemical vapor deposition etc..
Note, in any depositional phase, it is possible to deposition more than one material simultaneously.For example, it is possible to simultaneously two kinds of (or more kinds of) different types of metals of deposition/growth, such as stannum (Sn) and golden (Au)；Can two kinds of (or more kinds of) different types of quasiconductors of deposition/growth, such as silicon (Si) and germanium (Ge)；Can two kinds of (or more kinds of) different types of oxides of grown/deposited, such as iron lithium phosphate (LiFePO4) and lithium nickel cobalt manganese oxide (Li (NiCoMn) O2).Additionally, it is possible to material type is mixed, such as metal and quasiconductor, or quasiconductor and oxide, or metal and oxide, or metal, quasiconductor and oxide.Example includes silicon (Si) and lithium (Li) codeposition, silicon (Si) and LiO2(or SiO2) codeposition, and silicon (Si), lithium (Li) and LiO2(or SiO2) codeposition.Codeposition insulant can also be expected, such as silicon dioxide (SiO2) or silicon nitride (Si3N4).Alternatively, it is also possible to expect coprecipitated carbon distribution (C).
Interlayer 750 is created by liquid phase process alternatively, liquid phase process such as electroless deposition or plating.Comprised the material (such as silicon (Si) or stannum (Sn)) that sandwiches being suspended in adhesive solvent substrate by utilization and be coated with support silk thus it is also possible for creating interlayer.After appropriate processing, outside solvent is evicted out of substrate, only retain binding agent and sandwich material, thus creating and include supporting silk 110 and sandwiching the electrode of material.This technology can also be applied to negative electrode.Interlayer can include aeroge.When interlayer 750 generates according to liquid process, DAM is reduced region 720 and can be generated by the material that includes repelling this liquid at trunk 350 alternatively.Such as, if using water, then hydrophobic substance can include in the region of trunk 350.These materials can be incorporated to be supported silk 110 or is coated on the surface supporting silk 110.
In some embodiments, the electric conductivity of interlayer 750 is controlled with growing technology by properly selecting deposition.Such as, when sputtering, use the silicon of heavy doping p+ or n+ relative to using the silicon that undopes will to create the body interlayer silicon (such as, highly doped silicon is 10 ' sohm-cm, and pure silicon is 10000 ' sohm-cm) of facing conductive.When using the CVD siliceous deposits of silane, interpolation hydrogen phosphide or arsenic hydride can be used alternatively to increase the electric conductivity of the silicon of deposition/growth.In various embodiments, adulterant includes boron (B), gallium (Ga), arsenic (As), phosphorus (P), antimony (Sb), indium (In), thallium (Th) and/or bismuth (Bi).Other adulterants are possible.
In some embodiments, by depositing metal (such as, but not limited to gold (Au), stannum (Sn), silver (Ag), lithium (Li) or aluminum (Al)) when deposition/growth silicon, it is possible to increase the electric conductivity of interlayer 750.In some embodiments, the electric conductivity of interlayer 750 controls via ion implanting.These methods use and select the other materials (such as germanium (Ge)) for interlayer 750 is also possible.In various embodiments, the resistivity of produced interlayer 750 is less than 1ohm-cm, less than 10ohm-cm, less than 500ohm-cm, less than 2000ohm-cm, or less than 12000ohm-cm.In other embodiments, resistivity is more than 12000ohm-cm.
In some embodiments, step 830 includes the post processing of the interlayer 750 to deposition.This post processing can change the crystal structure of interlayer 750.Such as, in some embodiments, non-crystalline silicon is deposited as interlayer 750, and non-crystalline silicon is carried out suitable annealing by subsequent process steps, thus creates layer and/or the surface of polysilicon on interlayer 750.The structure produced can include the polysilicon layer on outer surface and the amorphous silicon layer between polysilicon layer and support silk 110.Two silicon layers are all considered as a part for interlayer 750.This annealing process can by using superpower laser or some other quick high-temp thermal source to realize.After annealing method after this deposition can apply to negative electrode and/or anode material alternatively.
In some embodiments, the interlayer 750 of deposition is passivation.In case of silicon, passivation can be realized by the annealing that other places in this article are discussed, or realizes by depositing the oxide, nitride and/or the carbide lamella that approximately be less than 5,10,40,100 or 250 nanometers.This oxide, carbide or nitride layer are considered a part for interlayer 750, and can support that a part for silk step 820 generates as growth.Oxide or nitride can be grown by heat treatment method and standard CVD and PECVD technique or deposit.Such as, surface passivation can be realized by growth carbide on the surface of interlayer 750 alternatively.By execution seed layer deposition step 805, establishment starting point step 815 and growth, this growth can support that silk step 820 realizes, wherein carbide, oxide and/nitride grow in step 820.In some embodiments, on interlayer 750, the CNT/CNF/NW of growth is highly maximum is several microns, and is typically smaller than 250nm.
Owing to supporting silk 110, ring catch 310, support ring 210 and support the shape of cap 150, different amounts of sandwich material along the length supporting silk 110 in various location deposition.Deposition/growth method for creating interlayer 750 optionally depends on the surface reaction for initial and continued growth process.If decreasing the reactant flow to the surface supporting silk 110, then the deposition/growth speed of interlayer 750 will reduce accordingly.
By way of example, and with reference to Fig. 7 A-Fig. 7 C, if ring catch interval 312 is 0, then there is no or only minimal amount of reactant supports the silk 110 surface under ring catch 310 by arriving, this generates DAM and reduce region 720, compared with other parts supporting silk 110, it has relatively little interlayer 750.
Ensure to depend on along the another way of the different amounts of interlayer 750 of length deposition/growth supporting silk 110 to support that silk height 114 separates the relatively wide aspect ratio of 126 with starting point.The magnitude of this aspect ratio can be similar to 5: 1,10: 1,100: 1,1000: 1,10000: 1 or height to 1000000: 1, it is possible to bigger.Because bigger aspect ratio means along with reactant moves to substrate 124, the lateral surfaces supporting silk has less solid angle inconspicuous, reduce accordingly along the increment supporting silk, thereby produce and have seldom or do not have the DAM of interlayer 750 to reduce region 720.Producing DAM minimizing region 720 by this way need not ring catch 310.
In step 840, it is possible to complete electrode manufacture.Electrode is optionally included in battery.
Fig. 9 A and Fig. 9 B illustrates the measurement capacity of the anode using technique described here to create, and wherein supports that silk 110 is carbon nano-fiber, and interlayer 750 is silicon.Fig. 9 A illustrates the capacity of the electrode increased with the thickness of interlayer 750.In figures 9 b and 9, line 910 illustrates the calculating capacity of only equadag coating, and line 920 illustrates the experimental result of the mixture using amorphous and polysilicon.Measure to arrange in (half-cellsetup) at half-cell and carry out.Fig. 9 B illustrates compared with the anode of pure graphite-based, the improvement of have 5 to 7 times of charge storage capacity.The amount improved depends on thickness and the material type of interlayer 750.
Figure 10 illustrates compared with industrial standard electrode, uses the cycle life of battery of the anode utilizing technique described here to create and the relation of the temperature of interlayer and thickness.Support that silk 110 is carbon nano-fiber, and interlayer 750 is silicon.Measurement can arrange in (full-cellsetup) at full battery and carry out at two different temperature, and performs circulation with C/2 speed.Data show, relative to prior art, have the cycle life being obviously enhanced at an elevated temperature.
Figure 11 illustrates the battery 1100 of the various embodiments according to the present invention.Battery 1100 includes such as the first electrode 1110 shown in Fig. 1-Fig. 8 herein and the second electrode 1120.Second electrode 1120 can include or can not include the feature shown in Fig. 1-Fig. 8.Battery 1100 also includes conductor (not shown), and its configuration is used for coupling the first electrode 1110 and the second electrode 1120 in the circuit being configured to provide electrical power to load.Those skilled in the art will appreciate that and how can configure these conductors.Battery 1100 usually rechargeable battery.First electrode can configure for as anode or cathode operation.
Figure 12 A is the height 114 of support silk 110 is the diagram of the electrode of 3.5 microns.Figure 12 B is the height 114 of support silk 110 is the diagram of the electrode of 17.5 microns.These in Figure 12 A and Figure 12 B support that silk does not include sandwiching material.
Figure 13 A is the height 114 of support silk 110 is the diagram of the electrode that siliceous deposits is interlayer 750 of 3.5 microns and 0.25 micron.Data indicate, and support that silk 110 has low-down cycle life (10 circulations of <) for 3.5 microns of the interlayer 750 (silicon) being coated with 0.25 micron.
Figure 13 B is the height 114 of support silk 110 is the diagram of the electrode that siliceous deposits is interlayer 750 of 17.5 microns and 0.25 micron.Data indicate, and support that silk 110 has very good cycle life (30 circulations of >, the capacity attenuation of < 20%) for 17.5 microns that are coated with 0.25 micron of interlayer 750 (silicon).The various embodiments of the present invention include having height 114 and are at least 17.5 microns of (17.5x10-6Rice) and there is the support silk 110 of interlayer 750 of at least 0.1,0.25,0.35,0.5 or 0.75 micron.
Figure 14 supports that the height 114 of silk is 10 microns and is absent from the cross section of electrode of interlayer.This electrode design (has the sandwich material deposit thickness of 0.5 micron of linear measurement, 1.5 microns and 4.0 microns) and has be carried out test, and creates Fig. 9 A, Fig. 9 B and Figure 10 data presented.This result indicates, and has the capacity of enhancing and the cycle life (during at 60 degrees Celsius, circulating for 300 times, 40% capacity attenuation, C/2 speed) of improvement at the temperature place improved.The various embodiments of the present invention include having at least 10 microns of (10.0x10-6Rice) the support silk 110 of interlayer 750 of height 114 and at least 0.1,0.25,0.35,0.5 or 0.75 micron.
Specifically illustrate at this and/or describe some embodiments.It is to be appreciated, however, that when without departing from the spirit and scope of claims, amendment and variant are covered by teachings above, and in scope of the claimed.Such as, electrode described here can use in equipment beyond battery.
Embodiment described here is the example of the present invention.Because describe these embodiments of the present invention with reference to example, so the various amendments of described method and/or ad hoc structure and adjustment can become apparent to those skilled in the art.Rely on the teachings of the present invention and these instruction on Push Technology all this type of amendment, adjust or variant be considered as within the spirit and scope of the present invention.Therefore, these describe and are not construed as ways to restrain with accompanying drawing, it should be understood that the present invention is by no means limited to shown embodiment.

Claims (45)

1. an electrode, including:
Substrate；
It coupled to the support silk of described substrate；
Interlayer, including the donor-acceptor material of the reactant configured for receiving electrochemical reaction, described donor-acceptor material is arranged along the length of described support silk, and the thickness of described interlayer is less than the length of described support silk；
Close to the sandwiched area of described substrate, relative to the sandwiched area away from described substrate, it includes less amount of donor-acceptor material；And
Along the ring catch that the length of described support silk is arranged, the configuration of described ring catch is for generating the sandwiched area including less amount of described donor-acceptor material.
2. electrode according to claim 1, wherein said support silk includes CNT or carbon nano-fiber or nano wire.
3. electrode according to claim 1, wherein said interlayer includes silicon, stannum or germanium.
4. electrode according to claim 1, wherein according to the weight supporting silk per unit area, the amount sandwiching material in the sandwiched area comprising less amount of donor-acceptor includes the described donor-acceptor material in the region away from described substrate less than 75%.
5. electrode according to claim 1, wherein according to the weight supporting silk per unit area, the amount sandwiching material in the sandwiched area comprising less amount of donor-acceptor includes away from described donor-acceptor material less than 50% in described substrate area.
6. electrode according to claim 1, also includes supporting ring, its configuration is used for preventing described interlayer from separating with described support silk.
7. electrode according to claim 1, also includes supporting cap, its configuration is used for preventing described interlayer from separating with described support silk.
8. electrode according to claim 1, wherein said interlayer is p+ or n+ doping.
9. electrode according to claim 1, also includes the Seed Layer being arranged between described substrate and described support silk, and the configuration of described Seed Layer is for coupleding to described substrate by described support silk.
10. electrode according to claim 1, wherein said support silk includes more than one support ring.
11. electrode according to claim 1, it is additionally included in the carbide lamella on the surface of described interlayer, oxide skin(coating) or nitride layer.
12. electrode according to claim 1, wherein said interlayer includes metal.
13. electrode according to claim 1, the surface of wherein said interlayer is passivation.
14. electrode according to claim 1, wherein said support silk includes CNT or carbon nano-fiber.
15. electrode according to claim 1, also including supporting ring, described support ring is configured to support to be attached to described interlayer described support silk.
16. electrode according to claim 12, wherein said metal is selected to increase the electric conductivity of described interlayer.
17. electrode according to claim 15, wherein said support ring is configured to generate the region along described support silk with different amounts of interlayer.
18. electrode according to claim 15, wherein said support ring has cone or triangular-section.
19. electrode according to claim 15, wherein said support ring has conical by its shape.
20. electrode according to claim 1, wherein said interlayer includes metal and oxide.
21. electrode according to claim 1, also including the support ring arranged along the length of described support silk, described support ring is characterised by the diameter diameter more than the other parts of described support silk.
22. electrode according to claim 1, wherein said support silk includes multi-walled carbon nano-tubes.
23. the method producing electrode, described method includes:
Receive substrate；
The first area of silk is supported in growth, and it coupled to described substrate；
At the terminal growth ring catch away from described substrate of the first area of described support silk, the configuration of described ring catch is for reducing the amount of the donor-acceptor material arriving described first area；
Grow the second area of described support silk from described ring catch, the second area of described support silk has the diameter less than described ring catch；And
To described support silk application donor-acceptor material so that support the donor-acceptor material of the first area greater thicknesses of silk in the second area of described support silk described in deposition rate.
24. method according to claim 23, wherein the diameter increase of described support silk is made to grow described ring catch by change growth conditions.
25. method according to claim 23, wherein said donor-acceptor material includes silicon, stannum or germanium, and described support silk includes CNT, carbon nano-fiber and nano wire.
26. method according to claim 23, also include growth support cap, its configuration for prevent described donor-acceptor material skid off described support silk be not connected with end.
27. method according to claim 23, also include growth support ring, its configuration for prevent described donor-acceptor material skid off described support silk be not connected with end.
28. method according to claim 23, also including described substrate application Seed Layer, the configuration of described Seed Layer is used for growing support silk.
29. method according to claim 23, also include adding oxide, carbide or nitride layer to the surface of described donor-acceptor material.
30. method according to claim 23, also include the material adding n+ or p+ doping to described donor-acceptor material.
31. method according to claim 23, also include adding metal to described donor-acceptor material.
32. method according to claim 23, it is additionally included in and applies after described donor-acceptor material to described support silk, heat described donor-acceptor material, in order to change the crystal structure of described donor-acceptor material.
33. method according to claim 23, it is additionally included in and applies after described donor-acceptor material to described support silk, be passivated described donor-acceptor material.
34. method according to claim 23, wherein said support silk includes multi-walled carbon nano-tubes.
35. a battery, including:
First electrode；And
Second electrode, including:
Substrate,
It coupled to the support silk of described substrate,
Interlayer, configuration is for receiving the reactant of electrochemical reaction, and described interlayer is arranged on described support silk and has the deposit thickness less than or equal to 4 microns, and
Along the ring catch that the length of described support silk is arranged, the configuration of described ring catch is for generating relative to the region away from described substrate close to described substrate and the sandwiched area including less amount of donor-acceptor material.
36. battery according to claim 35, wherein said second electrode configures as anode operation.
37. battery according to claim 35, also include for preventing described interlayer from skidding off the device of described support silk.
38. battery according to claim 35, also include the device of electric conductivity for increasing described interlayer.
39. battery according to claim 35, wherein said support silk includes multi-walled carbon nano-tubes.
40. battery according to claim 35, wherein said interlayer includes metal and oxide.
41. battery according to claim 35, wherein said interlayer includes silicon.
42. battery according to claim 35, wherein said interlayer includes silicon, metal and oxide.
43. battery according to claim 35, wherein said ring catch is configured to generate the region along described support silk with different thickness of interlayer.
44. battery according to claim 35, wherein said ring catch is configured to support to be attached to described interlayer described support silk.
45. battery according to claim 35, wherein said support silk includes multi-walled carbon nano-tubes.
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