EP3560022A1 - Lithium ion solid-state battery and method for producing the same - Google Patents
Lithium ion solid-state battery and method for producing the sameInfo
- Publication number
- EP3560022A1 EP3560022A1 EP17811831.1A EP17811831A EP3560022A1 EP 3560022 A1 EP3560022 A1 EP 3560022A1 EP 17811831 A EP17811831 A EP 17811831A EP 3560022 A1 EP3560022 A1 EP 3560022A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- electrolyte
- lithium
- solid
- layer
- sintered
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Classifications
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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
- 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
- H01M4/04—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
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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
- 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
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0562—Solid materials
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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
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0407—Methods of deposition of the material by coating on an electrolyte layer
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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
- H01M4/04—Processes of manufacture in general
- H01M4/043—Processes of manufacture in general involving compressing or compaction
-
- 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
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
- H01M50/461—Separators, membranes or diaphragms characterised by their combination with electrodes with adhesive layers between electrodes and separators
-
- 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
- H01M2300/0065—Solid electrolytes
- H01M2300/0068—Solid electrolytes inorganic
- H01M2300/0071—Oxides
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
-
- 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
Definitions
- Lithium-ion solid-state accumulator and method for producing the same
- the invention relates to the field of battery technology, in particular the lithium-ion solid-state batteries or accumulators and in particular to their method of preparation.
- battery technology in particular the lithium-ion solid-state batteries or accumulators and in particular to their method of preparation.
- Rechargeable lithium-ion batteries also referred to below as Li-ion batteries
- Li-ion batteries have been on the rise in recent years.
- the solid state batteries or solid electrolyte batteries are very interesting. This applies equally to the corresponding accumulators.
- an ion-conducting solid is used instead of the normally liquid or polymer-stabilized (gel) electrolyte.
- This solid electrolyte is usually inorganic (ceramics, glasses, etc.) designed.
- Decisive for the functionality of a solid-state electrolyte are the low electronic conductivity with simultaneous high ionic conductivity and a sufficiently high electrochemical stability compared to the anode and cathode material.
- the high conductivity for ions advantageously minimizes the internal electrical resistance of the accumulator and results in a high power density, while at the same time the high electrical resistance minimizes the self-discharge rate of the accumulator, thereby prolonging its life or shelf life.
- rechargeable solid-state batteries so far generally have a low power density compared to accumulators with liquid electrolytes. However, they ensure safe and environmentally friendly operation since no liquids can escape from the cell. The potential problems with liquid electrolytes, such as leakage, overheating, burn-up and toxicity, can thus be advantageously overcome. This property usually also leads to a particularly long life.
- a lithium-containing positive electrode and porous graphite or amorphous silicon are used as the negative electrode.
- the solid electrolyte and the electrodes are often layers comprising a polymer-ceramic composite material, on the one hand improve the charge transfer to the anode and on the other hand connect the cathode to the solid electrolyte. In addition, they regularly reduce the resistance.
- the previously well-functioning lithium-ion batteries typically have a thin film electrolyte.
- the task of the electrolyte is to conduct lithium ions from the anode to the cathode during discharge and to simultaneously electrically insulate the two poles.
- Suitable solid-state materials have vacancies in their atomic lattice structure. Lithium ions can occupy them and move from blank to blank through the solid.
- this mechanism is somewhat slower than the diffusion processes within a liquid electrolyte.
- This disadvantage can be compensated in principle by the execution of the electrolyte as a thin layer.
- the disadvantage is that the capacity of such thin-film accumulators is only poorly scalable due to their limited layer thickness.
- PVD physical vapor deposition
- a commercial solid-state thin-film cell based on lithium is marketed for example by the company "Infinite Power Solutions” under the name “Thinergy ® MEC200”.
- Thininergy ® MEC200 Each component of the cell is produced by a complex gas phase process. In this way, however, only thin electrodes can be realized, which in turn severely impairs the total capacity of the cell.
- layer thicknesses between typically 10 and 50 ⁇ m are regarded as thin layers.
- the object of the invention is to provide an effective and inexpensive lithium-ion solid-state accumulator, which overcomes the previous disadvantages of the prior art.
- the objects of the invention are achieved by a method for producing a lithium-ion-solid-state battery having the features of the main claim, and by a method for producing such a lithium-ion solid-state battery having the features of the independent claim.
- the production of a solid-state accumulator and in particular the production of a lithium-ion solid-state accumulator, can advantageously be based on a solid electrolyte and not on one of the electrode sides, as hitherto.
- the solid electrolyte thus assumes the mechanical load-bearing role in the production of the electrochemical cell.
- the term accumulator for rechargeable batteries is used below.
- first corresponding powder material is pressed into a dense electrolyte layer and then sintered.
- the electrolyte is then present as a nearly dense sintered electrolyte.
- close to density it is meant that the electrolyte has a density greater than 85% of the theoretical density.
- the electrolyte should have a porosity of not more than 20% by volume, preferably not more than 15% by volume. So that he has the necessary mechanical stability, the electrolyte layer according to the invention has a layer thickness of at least 100 ⁇ .
- the electrolyte according to the invention can be prepared both by a liquid-phase synthesis (solgel or hydrothermal) and by a so-called "solid oxide” synthesis In the "solid oxide” synthesis, the oxidic precursors are intimately ground and subsequently calcined. The electrolyte is then pre-pressed uniaxially in the form of an electrolyte pellet at more than 10 kN and then isostatically compressed and sintered at more than 1200 kN.
- Electrolyte powders suitable for this purpose include on the one hand compounds such as oxides, phosphates or even silicates, on the other hand, however, phosphorus sulfides. It can be used both individual of these compounds or phosphorus sulfides and mixtures of various such compounds or phosphorus sulfides. Some concrete compounds are listed below by way of example which are suitable as electrolyte powder in the aforementioned sense, without being limited to these:
- Lithium lanthanum zirconate wherein dopants of tantalum, aluminum and iron can additionally be used,
- a mixture of different phosphate compounds is preferably used in the process according to the invention.
- a particularly advantageous powder mixture for the production of the solid electrolyte according to the invention comprises, for example, lithium vanadium phosphate (LVP), lithium aluminum titanium phosphate (LATP) and lithium titanium phosphate (LTP). Because LATP is the actual ion conducting electrolyte material, it is present in excess and is usually added to both the anode and the cathode to achieve better conductivities.
- LVP lithium vanadium phosphate
- LATP lithium aluminum titanium phosphate
- LTP lithium titanium phosphate
- the ratio of LVP to LTP in this preferred electrolyte powder is, for example, 1.2: 1. It is a cathodically limited cell in which the cathode has more lithium than the active component than the anode can accommodate.
- the powder for producing the solid electrolyte should have an average particle size between 100 nm and 800 nm, preferably between 200 nm and 650 nm in order to allow a density of at least 85% of the theoretical density after densification and sintering.
- a bimodal or broad distribution of the particle sizes of the electrolyte powder used over the aforementioned relevant range has proven to be advantageous and promising for achieving high theoretical densities. Too low densities are less conducive to a solid state electrolyte because the limiting factor for ion conduction is the grain boundary conductivity.
- the average particle size (d 50 ) of the powder used was determined on the one hand by means of a scanning electron microscope (SEM) and on the other hand also by the method of measuring the static light scattering.
- the combination LTP and LVP can be mentioned, which exploits the electrochemical stability window of the electrolyte in a special way.
- a relatively low cell voltage to light days since the voltage of the anode (LTP) against Li / Li * at 2.5 V and thus the high voltage of the cathode can not be used regularly to achieve high energy densities regularly.
- the solid electrolyte produced in this way preferably has, after a sintering step, a layer thickness of between 100 ⁇ m and 800 ⁇ m, preferably between 200 ⁇ m and 500 ⁇ m, and particularly advantageously between 200 ⁇ m and 300 ⁇ m. Layer thicknesses of more than 500 ⁇ can already lead to a limitation of the internal resistance of the cell.
- the lower limit of 100 ⁇ regularly indicates the lower limit in which the layer can be present in its function as a mechanically stable carrier.
- individual electrode layers can be applied directly on both sides to the previously sintered electrolyte layer.
- the screen printing should be mentioned.
- all printing methods such as offset, roll to roll, dipping bed or ink jet printing are suitable for the system.
- all standard electrode materials can be used, wherein the electrode material used should align with the stability window of the electrolyte.
- oxidic electrode materials are suitable for example for the cathode:
- anode for example, the following materials are suitable:
- the accumulator produced according to the invention has as a special feature the uniform structure of the polyanions (PO 4 ) 3 " across the anode, electrolyte and cathode This structural feature also occurs with the use of phosphates, phosphorus sulfides and silicates
- the stability of the solid-state accumulator produced according to the invention becomes The structural integrity of the system is ensured by a matching, in their crystal structure and volume expansion matched electrodes and electrolyte combination.
- An advantageous embodiment of the invention provides that at least one interface between an electrode and the previously prepared solid electrolyte is additionally adapted in particular by a micro- and / or nanostructuring.
- composite layers of electrolyte and anode material or electrolyte and cathode material can optionally be used as "adhesion-promoting layers.”
- nanostructured anode or anode electrodes are also used Contain cathode particles as active components.
- the intermediate layers are usually applied with layer thicknesses of between 1 and 10 ⁇ m and in particular between 1 and 5 ⁇ m on the solid-state electrolyte.
- the nanostructuring can be achieved, for example, by the use of the solvothermal synthesis with the addition of suitable surfactants, eg. B. TritonXlOO ® can be achieved. As a result, a compensation of the intrinsic roughness and a good connection of the materials of both layers to each other can be ensured.
- suitable surfactants eg. B. TritonXlOO ®
- the processing of all further layers of the solid-state accumulator can advantageously be carried out using common standard printing processes, such as, for example, screen printing, offset printing or ink-jet.
- FIG. 1 flowchart of an advantageous embodiment of the invention
- Electrolyte-based process for producing a solid-state battery Electrolyte-based process for producing a solid-state battery.
- FIG. 2 Flowchart of a particular embodiment of the invention
- Electrolyte-based process for producing a solid state battery with intermediate layers Electrolyte-based process for producing a solid state battery with intermediate layers.
- FIG. 3 Schematic structure of solid-state accumulators according to the invention
- Li aluminum titanium phosphate (LATP) powder is crushed after milling in a ball mill (mean particle size after milling, d 50 ⁇ 1 pm) in a uniaxial piston press to a pellet of 1 1 mm diameter (40 kN). Subsequently, the pellet is polished on the surface and sintered at 1100 ° C (heating rate 2 K / min), holding time for 30 h in the powder bed.
- the sintered electrolyte pellet has a density of about 90% of the theoretical density and a thickness of about 400 ⁇ . The diameter shrinks regularly only minimally to about 11, 5 mm.
- the dried anode layer has a layer thickness of 60 ⁇ m (equivalent to three coatings) to account for the capacitances and the cathode layer has a thickness of 90 ⁇ m (corresponds to five coatings).
- the accumulator is then measured in a battery housing under a contact pressure of about 1 t.
Abstract
Description
Claims
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE102016015191.9A DE102016015191B3 (en) | 2016-12-21 | 2016-12-21 | Lithium-ion solid-state accumulator and method for producing the same |
PCT/DE2017/000391 WO2018113807A1 (en) | 2016-12-21 | 2017-11-18 | Lithium ion solid-state battery and method for producing the same |
Publications (1)
Publication Number | Publication Date |
---|---|
EP3560022A1 true EP3560022A1 (en) | 2019-10-30 |
Family
ID=60654572
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP17811831.1A Pending EP3560022A1 (en) | 2016-12-21 | 2017-11-18 | Lithium ion solid-state battery and method for producing the same |
Country Status (6)
Country | Link |
---|---|
US (1) | US11258053B2 (en) |
EP (1) | EP3560022A1 (en) |
JP (1) | JP7181866B2 (en) |
CN (1) | CN110235295B (en) |
DE (1) | DE102016015191B3 (en) |
WO (1) | WO2018113807A1 (en) |
Families Citing this family (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US11955595B2 (en) * | 2019-04-22 | 2024-04-09 | Bioenno Tech LLC | High-ionic conductivity ceramic-polymer nanocomposite solid state electrolyte |
US11223088B2 (en) * | 2019-10-07 | 2022-01-11 | Bioenno Tech LLC | Low-temperature ceramic-polymer nanocomposite solid state electrolyte |
CN112537958B (en) * | 2020-11-19 | 2022-04-05 | 哈尔滨工业大学 | Lanthanum lithium zirconate solid electrolyte and preparation method thereof |
US11735768B2 (en) | 2021-02-09 | 2023-08-22 | GM Global Technology Operations LLC | Gel electrolyte for solid-state battery |
CN116666728A (en) | 2022-02-21 | 2023-08-29 | 通用汽车环球科技运作有限责任公司 | Solid state intermediate layer for solid state battery |
Family Cites Families (18)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2001126758A (en) * | 1999-10-28 | 2001-05-11 | Kyocera Corp | Lithium battery |
JP5211526B2 (en) | 2007-03-29 | 2013-06-12 | Tdk株式会社 | All-solid lithium ion secondary battery and method for producing the same |
WO2008143027A1 (en) * | 2007-05-11 | 2008-11-27 | Namics Corporation | Lithium ion rechargeable battery and process for producing the lithium ion rechargeable battery |
JP5299860B2 (en) * | 2007-11-12 | 2013-09-25 | 国立大学法人九州大学 | All solid battery |
JP5358825B2 (en) * | 2008-02-22 | 2013-12-04 | 国立大学法人九州大学 | All solid battery |
JP2010272494A (en) | 2008-08-18 | 2010-12-02 | Sumitomo Electric Ind Ltd | Nonaqueous electrolyte secondary battery and method for producing the same |
JP4728385B2 (en) * | 2008-12-10 | 2011-07-20 | ナミックス株式会社 | Lithium ion secondary battery and manufacturing method thereof |
JP5269665B2 (en) | 2009-03-23 | 2013-08-21 | 日本碍子株式会社 | All solid state battery and manufacturing method thereof |
FR2956523B1 (en) * | 2010-02-18 | 2012-04-27 | Centre Nat Rech Scient | PROCESS FOR PREPARING A MONOLITHIC BATTERY BY PULSE CURRENT SINTING |
JP5715003B2 (en) | 2011-08-02 | 2015-05-07 | 日本特殊陶業株式会社 | All-solid battery and method for producing all-solid battery |
DE102011121236A1 (en) | 2011-12-12 | 2013-06-13 | Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. | Solid electrolyte for use in lithium-air or lithium-water storage batteries |
EP2683005B1 (en) * | 2012-07-06 | 2016-06-01 | Samsung Electronics Co., Ltd | Solid ionic conductor, solid electrolyte including the same, lithium battery including said solid electrolyte, and method of manufacturing said lithium battery |
US8821771B2 (en) * | 2012-09-26 | 2014-09-02 | Corning Incorporated | Flame spray pyrolysis method for forming nanoscale lithium metal phosphate powders |
JP6242620B2 (en) | 2013-07-30 | 2017-12-06 | 日本特殊陶業株式会社 | All solid battery |
JP6524775B2 (en) * | 2014-05-19 | 2019-06-05 | Tdk株式会社 | Lithium ion secondary battery |
JP2016119257A (en) | 2014-12-22 | 2016-06-30 | 株式会社日立製作所 | Solid electrolyte, all-solid battery using the same and method for producing solid electrolyte |
US9991556B2 (en) | 2015-03-10 | 2018-06-05 | Tdk Corporation | Garnet-type li-ion conductive oxide |
CN106876668A (en) | 2016-11-21 | 2017-06-20 | 蔚来汽车有限公司 | Combination electrode material of solid state lithium battery and preparation method thereof |
-
2016
- 2016-12-21 DE DE102016015191.9A patent/DE102016015191B3/en active Active
-
2017
- 2017-11-18 EP EP17811831.1A patent/EP3560022A1/en active Pending
- 2017-11-18 US US16/462,248 patent/US11258053B2/en active Active
- 2017-11-18 CN CN201780071920.4A patent/CN110235295B/en active Active
- 2017-11-18 JP JP2019527197A patent/JP7181866B2/en active Active
- 2017-11-18 WO PCT/DE2017/000391 patent/WO2018113807A1/en active Search and Examination
Also Published As
Publication number | Publication date |
---|---|
US11258053B2 (en) | 2022-02-22 |
WO2018113807A1 (en) | 2018-06-28 |
DE102016015191B3 (en) | 2018-06-14 |
CN110235295B (en) | 2023-12-19 |
CN110235295A (en) | 2019-09-13 |
JP7181866B2 (en) | 2022-12-01 |
US20190341597A1 (en) | 2019-11-07 |
JP2020514948A (en) | 2020-05-21 |
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Inventor name: MERTENS, ANDREAS Inventor name: SCHIERHOLZ, ROLAND Inventor name: GAO, XIN Inventor name: EICHEL, RUEDIGER-A. Inventor name: MERTENS, JOSEPH Inventor name: DE HAART, LAMBERTUS G. J. Inventor name: YU, SHICHENG Inventor name: KUNGL, HANS Inventor name: TEMPEL, HERMANN |
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