WO2009077049A1 - Composite silicium/siox/carbone pour batteries ion-lithium - Google Patents
Composite silicium/siox/carbone pour batteries ion-lithium Download PDFInfo
- Publication number
- WO2009077049A1 WO2009077049A1 PCT/EP2008/009770 EP2008009770W WO2009077049A1 WO 2009077049 A1 WO2009077049 A1 WO 2009077049A1 EP 2008009770 W EP2008009770 W EP 2008009770W WO 2009077049 A1 WO2009077049 A1 WO 2009077049A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- silicon
- sio
- lithium
- carbon
- composite
- Prior art date
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Classifications
-
- 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
-
- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
-
- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
-
- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
-
- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
-
- 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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/386—Silicon or alloys based on silicon
-
- 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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
-
- 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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
-
- 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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/40—Alloys based on alkali metals
- H01M4/405—Alloys based on lithium
-
- 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
Definitions
- the invention relates to a method for producing a Si / SiO x / C composite, comprising a core of silicon and at least one shell of silicon oxide and carbon and the use of this composite as anode material in lithium-ion batteries.
- Rechargeable lithium ion batteries are key components for portable electronics and electronic devices in the world today. The rapid development of these devices also increases the demand for lithium ion batteries with high energy density and long life cycles. High energy density lithium ion batteries require a high storage capacity and coulombic efficiency electrode material. Graphite and LiCo ⁇ 2 are commonly used in such lithium ion batteries (typical Coulomb efficiency> 90%), but have relatively low capacities (respectively 372 and 145 mA hg "1).
- silicon-based thin films or silicon-metal mixtures were used, silicon dispersions in an inactive / active matrix or carbon coating, as well as various electrolyte systems.
- a variety of active / inactive mixtures have been used, with the inactive component acting as a structural buffer to minimize the mechanical stress due to the large volume changes of the active silicon. This is to prevent the wear of the electrodes.
- Recent work in this field has shown that anodes of silicon / carbon mixtures are able to combine the advantageous properties of carbon (high number of charge cycles) and silicon (high lithium storage capacity) and overall the electrochemical performance of the anode
- Anodes has.
- No. 7061-7067 describes a Si-C-core-shell powder which is produced via a resorcinol-formaldehyde (RF) microemulsion polymerization in the presence of hydrophobic Si nanoparticles and subsequent carbonization.
- RF resorcinol-formaldehyde
- Si-C nanocomposite prepared by dispersing nanocrystalline silicon in carbon airgel followed by carbonization.
- the SiC nanocomposites have a reversible lithium storage capacity of 145O mA hg '1 .
- the object of the present invention was to provide a simple and sustainable method for coating silicon nanoparticles which, moreover, leads to anode materials with improved lithium storage performance in view of high, reversible storage capacity, excellent cycle performance and high conversion rate over the conventional high-temperature processes.
- the present invention thus relates to a process for producing a Si / SiO x / C composite containing a core of silicon and at least one shell of silicon oxide SiO x and carbon, wherein a silicon particle mixed with a sugar in an aqueous medium, polymerized at elevated temperature and then one
- Carbonization is subjected (hydrothermal carbonization).
- composite generally means composite materials.
- the hydrothermal carbonization invention (HTC) is used for the production of hydrophilic carbon materials from water-soluble carbohydrates at relatively mild temperatures (180-200 0 C) in closed vessels (autoclaves) (see M. Antonietti et al. Chem. Mater. 2006, 18, 3808) , A simplified reaction mechanism for the
- Formation of carbon structures involves, in the first step, the dehydration of the hydrocarbon (eg, a sugar) and the subsequent polymerization and carbonation of the shaped organic compounds in the second step.
- the resulting droplets either form the final spherical carbon particles or they can be used for the nanocoating of other structures.
- the carbonation is carried out at temperatures between 700 and 800 0 C.
- the carbon source according to the invention is a sugar such as glucose,
- Fructose sucrose or polysaccharides such as starch used.
- the silicon source used are silicon particles, preferably nanoparticles having an average diameter of between 10 and 100 nm, preferably between 20 and 50 nm.
- the silicon particles and the sugar are used in a ratio of 2: 1.
- SiO x silicon oxide layer
- the carbonation is carried out at temperatures between 700 and 800 0 C.
- the method according to the invention thus has a way of uniformly coating silicon particles, preferably
- Nanoparticles with SiO x and carbon.
- Another object of the present invention is a Si / SiO x / C composite containing a core of silicon and at least one
- the composite of the invention has a carbon content of 20 to
- Carbon coating is amorphous.
- Carbon coating according to the invention is between 1 and 10 nm, preferably between 2 and 4 nm.
- the thickness of the complete shell consisting of silicon oxide and carbon is between 5 and 20 nm, preferably about 10 nm.
- the reversible capacitance of the Si / SiO x / C nanocomposite according to the invention is 1100 mA hg '1 at a charge density of 150 mA g -1 , wherein the capacitance does not decrease even after 60 cycles.
- Another object of the present invention is a
- Lithium ion battery (rechargeable) with a first electrode as a cathode, with a second electrode as anode, with a membrane arranged between the two electrodes as a separator, with two terminals on the electrodes, with a said housing receiving housing and with a lithium ion-containing electrolyte, with the two
- Electrodes are impregnated, wherein the second electrode contains the erfindungsgemäBe Si / SiO x / C composite.
- lithium cobalt oxide lithium nickel oxide, lithium nickel cobalt oxide (doped and undoped), lithium manganese oxide
- the separator is an ion-permeable membrane as used in the
- the separator separates the first electrode from the second electrode.
- conductive salts are, for example, lithium hexafluorophosphate, lithium hexafluoroarsenate, lithium perchlorate, lithium tetrafluoroborate, LiCF 3 SO 3 , LiN (CF 3 SO 2 ), methide, lithium borates, LiPF 6 being preferred.
- solvents cyclic carbonates, propylene carbonate, ethylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate,
- the electrolyte contains vinyl carbonate.
- Nanocomposite electrode can be achieved. This is mainly attributed to the formation of a solid electrolyte intermediate phase on the surface of active particles.
- the lithium ion battery according to the invention can be produced in all conventional forms, such as a rod battery, for example for flashlights and larger devices, so-called “Knopf'battehe, for example, watches, hearing aids and small devices, in wound or folded form, as used in capacitors is or in still other forms.
- Another object of the present invention is the use of the inventive Si / SiO x / C composite as the anode material for lithium-ion batteries.
- Electrochemical experiments were performed with a 2-electrode Swagelok TM cell.
- Si nanoparticles with particle sizes of 20-50 nm (Nanostructured and Amorphous Materials Inc.) are dispersed in 10 mL of water in a Teflon inlet of a stainless steel autoclave by sonicating. Subsequently, 0.5 g of glucose are added to the dispersion, and the mixture is hydrothermally treated at 200 ° C. for 12 hours. The resulting material is isolated by centrifugation and further carbonized 2 flow at 750 c C for 4 h under N, in order to improve the degree of structural order of the carbon coating.
- PVDF Polyvinylidene fluoride
- EC ethylene carbonate
- DMC dimethyl carbonate
- the cells were mounted in an argon-filled glove box.
- the discharge and loading measurements were performed on an Arbin MSTAT system.
- the specific capacity of the Si / SiO x / C nanocomposite was calculated by considering the total mass of Si + Si ⁇ + C.
- Electrochemical Impedance Spectroscopic measurements were taken in the frequency bandwidth of 100 kHz to 10mHz with an AC amplitude of 5mV on a Solartron 1255 impedance spectrometer.
- FIG. 2 shows galvanostatic discharge / charge curves of the Si / SiO x / C nanocomposite electrode according to the invention at various.
- FIG. 3 shows the first discharge / loading curves of the pure Si
- (1 Si / SiO x / C composite in the VC-containing electrolyte
- 2 Si / SiO x / C composite in the VC-free electrolyte
- 3 nano-Si in the VC-containing electrolyte
- 4 nano-Si im VC-free electrolyte
- Fig. 4 shows a Nyquist plot of Si / SiO x / C nanocomposite electrodes cycled in VC-free and VC-containing electrolytes.
- (1 Si / SiO x / C composite in the VC-containing electrolyte
- 2 Si / SiO x / C composite in the VC-free electrolyte
- EIS electrochemical impedance spectroscopy
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Inorganic Chemistry (AREA)
- Crystallography & Structural Chemistry (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
L'invention concerne un procédé de fabrication d'un composite Si/SiOx/C, contenant un noyau en silicium et au moins une enveloppe en oxyde de silicium et carbone, ainsi que l'utilisation de ce composite en tant que matériau d'anode dans des batteries ion-lithium.
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE102007061618.1 | 2007-12-18 | ||
DE102007061618A DE102007061618A1 (de) | 2007-12-18 | 2007-12-18 | Silizium/SiOx/Kohlenstoff-Komposit für Lithiumionenbatterien |
Publications (1)
Publication Number | Publication Date |
---|---|
WO2009077049A1 true WO2009077049A1 (fr) | 2009-06-25 |
Family
ID=40289255
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/EP2008/009770 WO2009077049A1 (fr) | 2007-12-18 | 2008-11-19 | Composite silicium/siox/carbone pour batteries ion-lithium |
Country Status (3)
Country | Link |
---|---|
DE (1) | DE102007061618A1 (fr) |
TW (1) | TW200935646A (fr) |
WO (1) | WO2009077049A1 (fr) |
Cited By (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN102237519A (zh) * | 2011-07-11 | 2011-11-09 | 三峡大学 | 锂离子电池三维多孔硅粉负极材料无氟化制备方法 |
FR2981643A1 (fr) * | 2011-10-25 | 2013-04-26 | Commissariat Energie Atomique | Procede de preparation d'un materiau composite silicium/carbone, materiau ainsi prepare, et electrode notamment electrode negative, comprenant ce materiau. |
US8773072B2 (en) | 2011-08-29 | 2014-07-08 | Aygis Ag | Refuelable storage battery |
US20160233490A1 (en) * | 2013-07-10 | 2016-08-11 | Umicore | Silicon-Based Powder and Electrode Containing the Same |
CN108336342A (zh) * | 2018-02-28 | 2018-07-27 | 宁波富理电池材料科技有限公司 | Si/SiOx/C复合负极材料、其制备方法及锂离子电池 |
CN110364699A (zh) * | 2018-04-09 | 2019-10-22 | 丰田自动车株式会社 | 锂离子二次电池及其制造方法 |
WO2022166007A1 (fr) * | 2021-02-02 | 2022-08-11 | 广东凯金新能源科技股份有限公司 | Matériau composite silicium-carbone tridimensionnel et son procédé de préparation |
Families Citing this family (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CA2773496C (fr) * | 2009-09-23 | 2015-03-03 | Umicore | Nouvelles formulations pour electrodes a base de silicium destinees a etre utilisees dans des batteries lithium-ion et procede d'obtention associe |
KR101439726B1 (ko) * | 2010-06-29 | 2014-09-12 | 유미코르 | 산소 함량이 낮은 서브마이크론 크기의 실리콘 분말 |
WO2012031719A1 (fr) | 2010-09-06 | 2012-03-15 | Arys Gmbh | Accumulateur ravitaillable |
KR102243610B1 (ko) * | 2018-12-17 | 2021-04-27 | 주식회사 티씨케이 | 음극 활물질, 그의 제조 방법 및 그를 포함하는 리튬이차전지 |
CN111326723B (zh) * | 2020-02-26 | 2021-11-05 | 博尔特新材料(银川)有限公司 | 锂离子电池用硅碳复合负极材料及其制备方法 |
CN114772606B (zh) * | 2022-03-10 | 2023-09-19 | 四川大学 | 用于电磁波吸收的碳-二氧化硅核壳复合纳米材料及其制备方法 |
Citations (4)
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---|---|---|---|---|
US20030054249A1 (en) * | 2001-03-27 | 2003-03-20 | Nec Corporation | Anode for secondary battery and secondary battery therewith |
US20030068556A1 (en) * | 1994-12-16 | 2003-04-10 | Xue Jiayu Simon | Pre-graphitic carbonaceous insertion compounds and use as anodes in rechargeable batteries |
US20050031958A1 (en) * | 2003-08-05 | 2005-02-10 | Hirofumi Fukuoka | Lithium ion secondary battery negative electrode material and its preparation |
US20070072084A1 (en) * | 2003-10-07 | 2007-03-29 | Katsushi Nishie | Nonaqueous electrolyte secondary battery |
-
2007
- 2007-12-18 DE DE102007061618A patent/DE102007061618A1/de not_active Withdrawn
-
2008
- 2008-11-19 WO PCT/EP2008/009770 patent/WO2009077049A1/fr active Application Filing
- 2008-12-16 TW TW097149063A patent/TW200935646A/zh unknown
Patent Citations (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US20030068556A1 (en) * | 1994-12-16 | 2003-04-10 | Xue Jiayu Simon | Pre-graphitic carbonaceous insertion compounds and use as anodes in rechargeable batteries |
US20030054249A1 (en) * | 2001-03-27 | 2003-03-20 | Nec Corporation | Anode for secondary battery and secondary battery therewith |
US20050031958A1 (en) * | 2003-08-05 | 2005-02-10 | Hirofumi Fukuoka | Lithium ion secondary battery negative electrode material and its preparation |
US20070072084A1 (en) * | 2003-10-07 | 2007-03-29 | Katsushi Nishie | Nonaqueous electrolyte secondary battery |
Non-Patent Citations (1)
Title |
---|
XUELIN YANG, ZHAOYIN WEN, XIUJIAN ZHU, SHAHUA HUANG: "Preparation and electrochemical properties of silicon/carbon composite electrodes", ELECTROCHEMICAL AND SOLID-STATE LETTERS, vol. 8, no. 9, 29 July 2005 (2005-07-29), on line, pages A481 - A483, XP002518671 * |
Cited By (9)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN102237519A (zh) * | 2011-07-11 | 2011-11-09 | 三峡大学 | 锂离子电池三维多孔硅粉负极材料无氟化制备方法 |
US8773072B2 (en) | 2011-08-29 | 2014-07-08 | Aygis Ag | Refuelable storage battery |
FR2981643A1 (fr) * | 2011-10-25 | 2013-04-26 | Commissariat Energie Atomique | Procede de preparation d'un materiau composite silicium/carbone, materiau ainsi prepare, et electrode notamment electrode negative, comprenant ce materiau. |
WO2013060790A1 (fr) * | 2011-10-25 | 2013-05-02 | Commissariat A L'energie Atomique Et Aux Energies Alternatives | Procede de preparation d'un materiau composite silicium/carbone, materiau ainsi prepare, et electrode notamment electrode negative, comprenant ce materiau. |
US20160233490A1 (en) * | 2013-07-10 | 2016-08-11 | Umicore | Silicon-Based Powder and Electrode Containing the Same |
CN108336342A (zh) * | 2018-02-28 | 2018-07-27 | 宁波富理电池材料科技有限公司 | Si/SiOx/C复合负极材料、其制备方法及锂离子电池 |
CN110364699A (zh) * | 2018-04-09 | 2019-10-22 | 丰田自动车株式会社 | 锂离子二次电池及其制造方法 |
CN110364699B (zh) * | 2018-04-09 | 2022-04-12 | 丰田自动车株式会社 | 锂离子二次电池及其制造方法 |
WO2022166007A1 (fr) * | 2021-02-02 | 2022-08-11 | 广东凯金新能源科技股份有限公司 | Matériau composite silicium-carbone tridimensionnel et son procédé de préparation |
Also Published As
Publication number | Publication date |
---|---|
DE102007061618A1 (de) | 2009-06-25 |
TW200935646A (en) | 2009-08-16 |
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