An interface layer with high diffusion coefficient, a preparation method thereof and a battery

Abstract

The present application discloses an interface layer with high diffusion coefficient, the raw material of the interface layer includes carbon material, organic compound with thioamide group. The interface layer of the present application can effectively reduce the local current density of anode and improve the diffusion ability of Li + The interface layer of the present application can effectively prevent the accumulation of electric charge, promote the diffusion ability of anode and improve the diffusion ability of Li + The interface layer of the present application can effectively prevent the accumulation of electric charge, promote the diffusion ability of anode and improve the diffusion ability of Li The interface layer of the present application can be used in batteries to improve the electrical performance and safety performance of the batteries.

Description

Technical Field

[0001] This invention relates to the field of materials technology, specifically to an interface layer with a high diffusion coefficient, its preparation method, and a battery. Background Technology

[0002] In recent years, all-solid-state batteries with high safety have attracted widespread attention. Sulfide solid electrolytes (SSEs) have the highest ionic conductivity (1-25 mS / cm). -1 With its ideal mechanical properties and better interfacial contact with active materials, it is considered one of the most promising SSEs. It boasts the lowest redox potential (-3.04 V compared to a standard hydrogen electrode) and an ultra-high specific capacity (3860 mAh g⁻¹). -1 Lithium metal is the most promising anode for achieving high energy density all-solid-state batteries (ASSBs). Therefore, all-solid-state lithium sulfide metal batteries (ASSLMBs) using sulfide electrolytes and lithium metal anodes are the most promising for achieving high safety and high energy density.

[0003] However, the growth of lithium dendrites in the spin body has long limited the development of ASSLMBs. The growth of lithium dendrites is mainly caused by several factors. First, the low binding strength, low surface energy, and high fluidity of lithium make it prone to one-dimensional whisker growth. Second, metallic lithium tends to form voids with the spin body during exfoliation, leading to poor interfacial contact, high interfacial resistance, uneven charge distribution, and high overpotential, which exacerbates the formation of Li dendrites. To address these interfacial issues, researchers have developed numerous interfacial protective layers to improve them. ZnO, Al₄Li₉, LiF, Ag₂C, and graphite layers have been used to wet the interface and provide lithium deposition sites; however, the current density and areal capacity achievable by ASSLMBs are still insufficient for commercial applications. This is mainly because the formation of Li dendrites is also caused by Li… + The reduction rate and their replenishment around the electrodes are determined by the Li. At high current densities, due to the Li + The reduction of Li is relatively rapid, greatly increasing the chance of Li dendrite formation. If Li + Without timely replenishment, localized charge accumulation occurs, inducing the growth of Li dendrites. Lithium deposition in ASSLMBs occurs only at the anode-SSE interface, further increasing the risk of charge accumulation and thus significantly limiting the rate performance of ASSLMBs. Therefore, constructing a three-dimensional lithium metal anode, preventing lithium deposition from being confined to the anode-electrolyte interface, is an effective way to suppress lithium dendrite growth and improve battery rate performance. The main reason for lithium deposition at the electrolyte-anode interface is Li... + The low diffusion coefficient in the anode leads to Li+ They cannot be transported into the anode and directly acquire electrons at the interface. Therefore, the primary task in developing dendrite-free ASSLMB is to design lithium metal anodes with high ion diffusion coefficients and electronic conductivity. Summary of the Invention

[0004] This invention addresses the problems in the prior art by disclosing an interface layer with a high diffusion coefficient. This interface layer can effectively reduce the local current density of lithium-containing anodes and improve Li... + The diffusion capability of lithium-containing anodes prevents charge accumulation and promotes Li + It can be replenished in a timely manner, thereby preventing the growth of Li dendrites. The interface layer of this invention, when used in a battery, can improve the battery's electrical performance and safety performance.

[0005] This invention is achieved through the following technical solution:

[0006] The present invention provides an interface layer with a high diffusion coefficient, wherein the raw materials of the interface layer include carbon materials and organic compounds having thioamide groups.

[0007] In the above design of the present invention, the S and N in the thioamide group (structural formula I) are doped into the carbon material to form CN and CS bonds. The CN and CS bonds can further reduce the Li + The transmission energy barrier is reduced, thereby significantly improving the Li-1000 transmission energy barrier. + The diffusion rate of Li, therefore, + It can diffuse throughout the entire interface layer, gain electrons, and form metallic lithium. This method of depositing metallic lithium within the interface layer can effectively reduce the local current density at the anode, prevent charge accumulation, and allow Li to... + It can be replenished in a timely manner, thereby preventing the growth of Li dendrites. Therefore, the interface layer of this invention can improve the lithium-ion diffusion rate of the lithium-metal anode and reduce the formation of lithium dendrites, thereby improving the battery's electrical and safety performance.

[0008] The thioamide group has the following structural formula I:

[0009]

[0010] As a further embodiment, the mass ratio of the carbon material to the organic compound having a thioamide group is 1:(0.125-1).

[0011] As a further embodiment, the mass ratio of the carbon material to the organic compound having thioamide groups is 1:(0.5-1). This results in better electrical properties.

[0012] As a further option, the carbon material includes one or more of soft carbon and hard carbon. Soft carbon has a larger interlayer spacing, which is more conducive to Li... + The spread of.

[0013] As a further embodiment, the soft carbon includes one or more of graphite, petroleum coke, needle coke, carbon fiber, and carbon microspheres.

[0014] As a further embodiment, the hard carbon includes one or more of resin carbon, organic polymer carbon, carbon black, and biomass carbon.

[0015] As a further embodiment, the resin carbon includes one or more of phenolic resin, epoxy resin, and polyfurfuryl alcohol resin.

[0016] As a further embodiment, the organic polymer carbon includes one or more of PVA (polyvinyl alcohol), PVC (polyvinyl chloride), PVDF (polyvinylidene fluoride), and PAN (polyacrylonitrile).

[0017] As a further embodiment, the carbon black includes acetylene black prepared by CVD.

[0018] As a further embodiment, the biomass carbon includes plant residues.

[0019] As a further embodiment, the organic compound having a thioamide group includes thiourea and thioacetamide.

[0020] As a further option, the raw materials for the interface layer also include a film-forming agent.

[0021] As a further embodiment, the film-forming agent includes one or more of polytetrafluoroethylene, polyethylene, polyhexafluoropropylene, and styrene-butadiene rubber.

[0022] As a further embodiment, the interface layer has characteristic peaks at 25°, 44°, and 45° in the X-ray powder diffraction pattern represented by the diffraction angle 2θ.

[0023] As a further option, the thickness of the interface layer is 25μm-35μm.

[0024] The present invention also provides a method for preparing the interface layer, the method comprising:

[0025] The carbon material and the organic compound with thioamide groups are weighed according to the specified mass ratio, mixed, and then calcined in an inert atmosphere to obtain a composite. The composite is then mixed with a film-forming agent and dry-rolled to form a film, thus obtaining the interface layer of this invention. During calcination, the organic compound with thioamide groups generates H2S and NH3 molecules. The diameter of the NH3 molecules is slightly larger than the interlayer spacing of the carbon material; therefore, the heated NH3 molecules can further expand the interlayer spacing of the carbon material during calcination, thereby promoting the Li... + The diffusion of H2S and NH3 molecules during calcination can attack C-C bonds, increasing the defect degree of carbon materials and forming CN and CS bonds. These defects can enable Li... + The crossing between carbon layers increases transport paths, while CN and CS bonds can further reduce Li + The transmission energy barrier is reduced, thereby significantly improving the Li-1000 transmission energy barrier. + The diffusion rate of Li promotes + It can diffuse throughout the entire carbon material layer, gain electrons, and form metallic lithium. In this invention, dry roll forming is beneficial for promoting the formation of the interface layer, and those skilled in the art can adjust the roll forming pressure according to the actual situation.

[0026] As a further embodiment, the mass ratio of the composite to the film-forming agent is 100:3.

[0027] As a further embodiment, the calcination temperature is 300℃-500℃, and the calcination time is 4h-6h.

[0028] As a further option, the inert atmosphere includes one of nitrogen, argon, helium, neon, krypton, and xenon.

[0029] The present invention also provides an application method for the interface layer, wherein the application method is selected from scheme I or scheme II:

[0030] Option I:

[0031] The interface layer is disposed as a separate layer between the lithium metal anode and the electrolyte in a battery.

[0032] Option II:

[0033] The interface layer is composited with a lithium metal-containing anode to form a composite anode for use in a battery. In this invention, the lithium metal-containing anode includes a lithium metal anode and a pre-lithiated anode, specifically a pre-lithiated anode made of pre-lithiated graphite, pre-lithiated silicon-carbon, or pre-lithiated silicon-oxygen. In this art, during battery discharge, the cathode represents the positive electrode of the battery, and the anode represents the negative electrode.

[0034] The present invention also provides a lithium metal anode, cathode, or battery separator having the aforementioned interface layer. When the interface layer of the present invention is used in the cathode or battery separator of a battery, it can improve the ionic conductivity of the battery; when the interface layer is used in the lithium metal anode of a battery, it can not only improve the ion diffusion capability, but also suppress the growth of lithium dendrites.

[0035] The present invention also provides a battery or electrochemical device having the interface layer.

[0036] As a further embodiment, the battery can be used in 3C products, including but not limited to computers, tablets, mice, mobile phones, digital cameras, Walkmans, electronic dictionaries, digital audio players, smartwatches, MP3 players, MP4 players, radios, and Bluetooth headsets.

[0037] As a further embodiment, the electrochemical device can be used in end-consumer products, including but not limited to mobile phones, laptops, pen input computers, mobile computers, e-book players, portable phones, portable fax machines, portable copiers, and portable printers.

[0038] As a further embodiment, the electrochemical device can be used in electrical equipment, including large and small electrical equipment. Small electrical equipment includes consumer products, wearable electronic devices, or portable electronic devices; large electrical equipment includes transportation equipment. Transportation equipment includes, but is not limited to, vehicles such as automobiles, motorcycles, electric bicycles, buses, subways, high-speed trains, airplanes, and ships. Wearable electronic devices or portable electronic devices include, but are not limited to, headphones, video recorders, LCD TVs, portable cleaners, portable CD players, mini CDs, transceivers, electronic notebooks, calculators, memory cards, portable recorders, radios, backup power supplies, drones, motors, lighting fixtures, toys, game consoles, clocks, power tools, flashlights, cameras, large household batteries, and lithium-ion capacitors.

[0039] The features and beneficial effects of this invention are as follows: the interface layer of this invention can effectively reduce the local current density of lithium-containing anodes and improve Li... + The diffusion ability at the anode prevents charge accumulation and promotes Li + It can be replenished in a timely manner, thereby preventing the growth of Li dendrites. The interface layer of this invention, when used in a battery, can improve the battery's electrical performance and safety performance. Attached Figure Description

[0040] To more clearly illustrate the technical solutions in the embodiments of the present invention, the drawings used in the description of the embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0041] Figure 1 These are schematic diagrams and features of embodiments and comparative examples of the present invention, wherein, Figure 1 a is a schematic diagram of lithium deposition on the SC-TU-Li anode. Figure 1 b is a SEM image of the interface between the SC-TU-Li anode and LPSCl (Li6PS5Cl) at a magnification of 20 μm. Figure 1 c is a SEM image of the SC-TU-Li anode and LPSCl interface at a magnification of 10 μm. Figure 1 d is a cross-sectional scan image of the SC-TU-Li anode after lithium deposition at a magnification of 4 μm. Figure 1 e is a SEM image of the interface between the colored SC-TU-Li anode and LPSCl. Figure 1 f is a schematic diagram of lithium deposition on an SC-Li anode. Figure 1 g is a SEM image of the SC-Li anode and LPSCl interface at a magnification of 20 μm. Figure 1 h is a SEM image of the SC-Li anode and LPSCl interface at a magnification of 10 μm. Figure 1 i is a cross-sectional scan image of the SC-Li anode after lithium deposition at a magnification of 4 μm. Figure 1 j is a SEM image of the interface between the colored SC-Li anode and LPSCl.

[0042] Figure 2 This is a SEM image of the SC-TU-Li anode before lithium deposition in an embodiment of the present invention. Figure 2 a is a SEM image of the SC-TU-Li anode and LPSCl interface at a magnification of 20 μm. Figure 2 b is a SEM image of the SC-TU-Li anode and LPSCl interface at a magnification of 10 μm. Figure 2 c is a cross-sectional scan image of the SC-TU-Li anode before lithium deposition at a magnification of 5 μm.

[0043] Figure 3 For the characterization of the physical and chemical properties of the embodiments and comparative examples of the present invention, wherein Figure 3 a is an XRD pattern of an embodiment and a comparative example of the present invention. Figure 3 b is the Raman spectrum of the embodiment and comparative example of the present invention. Figure 3c represents the electronic conductivity of the embodiments and comparative examples of this invention. Figure 3 d is the XPS spectrum of C1s in an embodiment of the present invention. Figure 3 e is the XPS spectrum of N1s in embodiment N of the present invention. Figure 3 f is the XPS spectrum of embodiment S2p of the present invention. Figure 3 g is the Li in the embodiments and comparative examples of the present invention. + Diffusion coefficient, Figure 3 h is the Tafel curve of a Li-symmetric cell with different sandwich layers. Figure 3 i represents the nucleation overpotential in the embodiments and comparative examples of this invention.

[0044] Figure 4 For the electrical performance testing of all-solid-state batteries with ultra-high current density, among which Figure 4 a is at 0.25mAhcm -2 The critical current density of symmetrical lithium batteries with different sandwich layers. Figure 4 b is at a current density of 20 mA cm -2 The cycle performance of symmetric lithium batteries using SC-TU sandwich technology. Figure 4 c is at a current density of 2 mA cm -2 Cycle performance of symmetrical lithium batteries employing SC-TU sandwich and SC sandwich layers. Figure 4 d represents the ACE index of symmetrical lithium batteries using SC-TU and SC sandwich structures. Figure 4 e represents LCO (lithium cobalt oxide) / LPSCl / SC-TU-Li, LCO / LPSCl / SC-Li, and LCO / LPSCl / Li (lithium) ASSB (all-solid-state battery) at 0.5 mAh cm⁻¹. -2 speed performance, Figure 4 f is the charge-discharge curve of LCO / LPSCl / SC-TU-Li at a discharge rate of 30C. Figure 4 g is the charge-discharge curve of LCO / LPSCl / SC-Li at a discharge rate of 30C. Figure 4 h represents the cycle performance of LCO-LPSCl-SC-TU / Li ASSB at a discharge rate of 30C and at a discharge rate of 50C. Figure 4 j is a comparison of the electrical performance in the embodiments of the present invention and the references.

[0045] Figure 5 CCDs of SC and TU products in different proportions.

[0046] Figure 6 Cyclic performance of LCO-LPSCl-SC-Li ASSB at 30°C.

[0047] Figure 7 The test results are for all-solid-state batteries with high areal capacity and energy density. Figure 7 a is the rate curve of LCO / LPSCl / SC-TU-Li ASSB. Figure 7 b is an LCO / LPSCl / SC-TU-Li ASSB with an area capacity of 3mAh cm⁻¹ -2 Cyclic performance, Figure 7 c represents the charge-discharge curves of LCO / LPSCl / SC-TU-Li ASSB with different area capacities. Figure 7 d has a capacity of 15mAh cm -2 Cycling performance of LCO / LPSCl / SC-TU-Li ASSB at 0.1C rate. Figure 7 e represents a comparison of the area capacity in this work with other literature. Figure 7 f is the charge-discharge curve of LCO / LPSCl / SC-TU-Li ASSB, with an energy density of 403.0 Wh / kg. -1 , Figure 7 Charge-discharge curves of a square pouch-shaped LCO / LPSCl / SC-TU-Li battery with a side length of 2 cm. Figure 7 h is a comparison of energy density with other reported values ​​in the literature.

[0048] Figure 8 It is LCO-LPSCl-SC-Li ASSB at 2C and 3mAh cm⁻¹ -2 Cyclic performance.

[0049] Figure 9 It is LCO-LPSCl-SC-Li ASSB at 2C and 3mAh cm⁻¹ -2 The charging curve after 30 cycles. Detailed Implementation

[0050] To facilitate understanding of the high diffusion coefficient interface layer and its preparation method of the present invention, a more comprehensive description of the high diffusion coefficient interface layer and its preparation method of the present invention will be given below, and embodiments of the present invention will be provided, but this does not limit the scope of the present invention.

[0051] In this invention, graphite and thiourea in soft carbon are used as examples to illustrate the concept of the invention. The anode in this invention uses a lithium metal anode as an example to explore how the interface layer improves the electrical performance of the lithium metal anode. In this invention, SC in the following text represents the soft carbon used in the embodiments of this case; in the embodiments and comparative examples of this invention, the soft carbon is graphite.

[0052] Example 1:

[0053] SC-xTU is obtained by mixing soft carbon (SC) and thiourea (TU) at a mass ratio of 1:0.5, placing the mixture in a tube furnace, and calcining it at 400°C for 5 hours under nitrogen atmosphere. The composite is then mixed with polytetrafluoroethylene (PTFE) at a mass ratio of SC-xTU:PTFE = 100:3 to obtain the interface layer of this invention. This interface layer is then rolled to a 30 μm thickness using a roll-to-roll machine.

[0054] By placing SC-TU between the anode and the electrolyte, SC-TU can be combined with the anode for use in solid-state batteries. Alternatively, during battery fabrication, the cathode, electrolyte layer, interface layer, and anode can be placed sequentially, followed by pressing under pressure to obtain the battery, where SC-TU is combined with the anode to form an SC-TU-Li anode. In Example 1 of this invention, the soft carbon is graphite.

[0055] Example 2:

[0056] SC-xTU is obtained by mixing soft carbon (SC) and thiourea (TU) at a mass ratio of 1:0.25, placing the mixture in a tube furnace, and calcining it at 400°C for 5 hours under nitrogen atmosphere. The composite is then mixed with polytetrafluoroethylene (PTFE) at a mass ratio of SC-xTU:PTFE = 100:3 to obtain the interface layer of this invention. This interface layer is then rolled to a 30 μm thickness using a roll-to-roll machine.

[0057] By placing SC-TU between the anode and the electrolyte, SC-TU can be combined with the anode for use in solid-state batteries. Alternatively, during battery fabrication, the cathode, electrolyte layer, interface layer, and anode can be placed sequentially, followed by pressing under pressure to obtain the battery, where SC-TU is combined with the anode to form an SC-TU-Li anode. In Example 1 of this invention, the soft carbon is graphite.

[0058] Example 3:

[0059] SC-xTU is obtained by mixing soft carbon (SC) and thiourea (TU) at a mass ratio of 1:0.75, placing the mixture in a tube furnace, and calcining it at 400°C for 5 hours under nitrogen atmosphere. The composite is then mixed with polytetrafluoroethylene (PTFE) at a mass ratio of SC-xTU:PTFE = 100:3 to obtain the interface layer of this invention. This interface layer is then rolled to a 30 μm thickness using a roll-to-roll machine.

[0060] By placing SC-TU between the anode and the electrolyte, SC-TU can be combined with the anode for use in solid-state batteries. Alternatively, during battery fabrication, the cathode, electrolyte layer, interface layer, and anode can be placed sequentially, followed by pressing under pressure to obtain the battery, where SC-TU is combined with the anode to form an SC-TU-Li anode. In Example 1 of this invention, the soft carbon is graphite.

[0061] Comparative Example 1: SC-Li anode was formed using only soft carbon (SC) as the interface layer. The soft carbon in Comparative Example 1 was graphite.

[0062] Comparative Example 2: Li anode without an interface layer.

[0063] This invention will also provide an interface layer for use in batteries:

[0064] Cathode preparation: LCO cathodes are also prepared by dry rolling, with a mass ratio of LCO (lithium cobalt oxide): LPSCl (solid electrolyte): PTFE = 60:40:0.5. It is rolled to the appropriate thickness according to the required area capacity.

[0065] Preparation of Li6PS5Cl (LPSCl): Synthesized via solid-state mechanical chemical reaction. A mixture of Li2S (lithium sulfide) (99.9%, Zhejiang Fengli New Energy Technology Co., Ltd.), LiCl (lithium chloride) (99.95%, Innochem), and P2S5 (phosphorus pentasulfide) (>99%, Macklin) was milled at 600 rpm for 45 hours using a planetary ball mill. The mass ratio of the mixture to zirconia balls was 1:40. The ball-milled powder was granulated under a pressure of 2 tons (approximately 250 MPa), then sealed in a quartz tube and annealed in a muffle furnace at 550°C for 12 hours to obtain the final product. LiCoO2 (lithium cobalt oxide) (>99.5%, aldaddin) was coated with LiZrO2. Li6PS5Cl (LPSCl) is also commercially available.

[0066] Preparation of the all-solid-state battery: 80 mg of LPSCl powder was added to a Swagelok model battery and pressed at 125 MPa (1 ton) for 1 minute to form a flat surface. A prepared LCO cathode film was placed on the surface of the LPSCl layer and pressed together at 375 MPa (3 tons) for 1 minute. Other SC-TU layers were placed on the other side of the LPSCl layer. Lithium foil was placed on the surface of the SC-TU layers and pressed together at 873 MPa (7 tons) for 1 minute. Finally, the pressure was reduced to 250 MPa (2 tons). Thus, a four-layer particle battery was sandwiched between two stainless steel rods and sealed within the Swagelok model battery. Electrostatic charge-discharge was performed on a LANHE (CT2001A, LAND Electronic Co., Ltd.) battery testing system. The voltage window was set to 2.5–4.2 V, and various constant current densities were applied to evaluate the cycle stability and rate performance of the ASSB at 55°C. All battery fabrication processes were carried out in an argon-filled glove box.

[0067] Fabrication of the all-solid-state pouch cell: The LCO cathode film was also prepared by dry rolling, with a ratio of LCO:LPSCl:VGCF (carbon fiber):PTFE = 70:27:3:0.5. The electrolyte layer consisted of two layers: LIC (solid electrolyte Li3InCl6) and LPSCl. They were each mixed with 1 wt% PTFE and then dry rolled to form an 80 μm film. Aluminum foil, LCO, LIC, LPSCl, SC-TU, Li, and copper foil were then sequentially stacked and sealed in an aluminum-plastic bag. The bag cell was then pressed at 625 MPa to obtain the pouch cell.

[0068] Analysis of verification results:

[0069] Table 1 Comparison of current densities of all-solid-state batteries in the embodiments of the present invention and the references

[0070]

[0071]

[0072] Table 2 Comparison of the highest area capacity of batteries in the embodiments of the present invention and in the references.

[0073] <![CDATA[Area capacity (mAh cm -2 )]]> Battery configuration References 1 1.25 NCA / LPS / 3D anode <![CDATA[(ACS Energy Lett.)

[15] ]]> 2 1 LFP / LLZO / Li-rGO <![CDATA[(Sci.Adv.)

[16] ]]> 3 2 Li / LAGP / NCM811 <![CDATA[(Energy Storage Mater.)

[17] ]]> 4 4.2 LiIn / LPSCl / S <![CDATA[(Adv.Funct.Mater.)

[18] ]]> 5 4.9 <![CDATA[Li / Li3PS4 / CuS]]> <![CDATA[(Adv.Energy Mater)

[19] ]]> 6 6.8 Ag-C / LPSCl / NCM <![CDATA[(Nat.Energy)

[12] ]]> 7 7.46 <![CDATA[Li2S@C-LPS-AB / LPS / Li]]> <![CDATA[(Nano Lett.)

[20] ]]> 8 8.7 <![CDATA[NMC / Li6PS5Cl / Li]]> <![CDATA[(ACSAppl.Mater.Interfaces)

[21] ]]> 9 12.5 <![CDATA[SeS2 / Li 10 GeP2S 12 –Li3PS4 / Li]]> <![CDATA[(Adv.Mater.)

[22] ]]> 10 13.2 NMC622 / LABTP / PVDF-HFP / Li <![CDATA[(Energy Environ.Sci.)

[23] ]]> 11 15 This work

[0074] Table 3 Comparison of energy density of batteries in the embodiments of the present invention and in the references.

[0075] <![CDATA[Energy density (Whkg -1 )]]> Battery configuration References 1 44 <![CDATA[NCM622|Li6PS5Cl|Graphite]]> <![CDATA[(Nano Lett.)

[24] ]]> 2 73.6 NCM532|LLZTO|Li-FEC <![CDATA[(Adv.Energy Mater.)

[25] ]]> 3 110 <![CDATA[NCM622 / / PI-Li6PS5Cl 0.5 Br 0.5 / Graphite]]> <![CDATA[(ACS Energy Lett.)

[26] ]]> 4 128.4 <![CDATA[Sulfur|Li6PS5Cl|In-Li]]> <![CDATA[(Adv.Fun.Mater.)

[18] ]]> 5 151.1 <![CDATA[LiNi 0.90 Mn 0.05 Co 0.05 O2|Li6PS5Cl|Graphite]]> <![CDATA[(Energy Storage Mater.)

[27] ]]> 6 155 <![CDATA[LiNi 1 / 3 Co 1 / 3 Mn 1 / 3 O2|Li3PS4|Graphite]]> <![CDATA[(J.Electrochem.Soc.)

[28] ]]> 7 178.3 <![CDATA[NCM622|PI-Li6PS5Cl|Graphite]]> <![CDATA[(Nano Lett.)

[29] ]]> 8 280 <![CDATA[NCM811|LLZTO|Graphite+SiO x ]]> <![CDATA[(ACS Energy Lett.)

[30] ]]> 9 284.4 <![CDATA[Co3S4|polydopamine-coated Li6PS5Cl|Li]]> <![CDATA[(Energy Storage Mater.)

[31] ]]> 10 305 This work

[0076] We successfully obtained an interface layer using the preparation method of this invention. After sintering carbon materials and organic compounds with thioamide groups, the organic compounds with thioamide groups generate H2S and NH3 molecules during calcination. The diameter of the NH3 molecules is slightly larger than the interlayer spacing of the carbon materials. Therefore, the heated NH3 molecules can further expand the interlayer spacing of the carbon materials during calcination, thereby promoting the Li... + The diffusion of H2S and NH3 molecules during calcination can attack C-C bonds, increasing the defect degree of carbon materials and forming CN and CS bonds. These defects can enable Li... + The crossing between carbon layers increases transport paths, while CN and CS bonds can further reduce Li + The transmission energy barrier is reduced, thereby significantly improving the Li-1000 transmission energy barrier. + The diffusion rate of Li promotes + It can diffuse throughout the entire carbon material layer, gain electrons, and form metallic lithium. Therefore, the method of this invention successfully achieves an interface layer that enhances the Li content of the anode. + It improves diffusion rate and can also suppress the growth of lithium dendrites.

[0077] To verify our experimental design, a current density of 4 mA cm⁻¹ was used. -2 3mAh cm -2 After removing lithium metal, the morphology of the SC (soft carbon) and SC-TU (soft carbon-thiourea) interlayers (where the mass ratio of SC to TU is 1:0.5) was observed using SEM. Figure 1 a) The SC-TU interface layer of this invention promotes uniform lithium deposition and suppresses the formation of lithium dendrites. Figure 1 f is a comparative example of its application in batteries, where lithium deposition uniformity is poor and lithium dendrites are also formed. From Figure 1 b- Figure 1 c and Figure 1 g- Figure 1 In the cross-sectional image of h, we can clearly see the electrolyte layer, the interface layer, and the lithium metal layer. The thickness of the interface layer between SC and SC-TU is approximately 30 μm. For easier observation, we will... Figure 1 c and Figure 1 h coloring, such as Figure 1 As shown in e and 1j, the blue and yellow parts represent the anode (lithium metal layer and interface layer) and the electrolyte, respectively. Figure 1 As shown in image e, the SC-TU anode after Li deposition is very dense, with no interparticle voids observed. From the magnified image... Figure 1 As can be seen from d, metallic lithium is deposited on the surface of the SC-TU particles, and the spaces between the particles are also filled with metallic lithium. As for the SC-TU layer before deposition (…), Figure 2 As shown in the diagram, we can observe a large number of voids, indicating that lithium metal is deposited in the voids of the SC-TU anode. The deposition of lithium metal in the voids can significantly increase the deposition sites, thereby effectively reducing the local current density and suppressing the formation of lithium dendrites. Conversely, the unmodified SC has a very low diffusion coefficient, thus... + They tend to gain electrons directly at the interface between the SC layer and the electrolyte layer, forming Li dendrites that pierce the electrolyte (e.g., Figure 1 g- Figure 1 (as shown in j). From Figure 1 g- Figure 1 It can be clearly seen that a large number of Li dendrites have penetrated the electrolyte. Figure 1 Image i is a cross-sectional SEM image of the SC intermediate layer, showing numerous voids without metallic lithium inside the SC anode. This indicates a large amount of Li. + Instead of diffusing into the interior of the SC anode, the lithium dendrites directly gain electrons at the interface between the SC and SSE, forming Li dendrites. Therefore, the interface layer of this invention can reduce the formation of lithium dendrites.

[0078] Building upon this, we further investigate how the interface layer in this invention enhances the Li content of the anode. + Diffusion coefficient. Figure 3 XRD in a shows that, compared to SC, the peak position of SC-TU shifted 0.6° to the left, indicating that the interlayer spacing of soft carbon widened due to calcination of thiourea. Simultaneously, the full width at half maximum (FWHM) increased from 7.9 to 9.9, suggesting a reduction in grain size, which may be due to the formation of defects. Figure 3 Raman in b further proves this point. It's easy to see that the ratio of ID to IG increased from 1.10 to 1.33 (as shown in figure b). Figure 3 As shown in b), this indicates an increase in disordered structure, which also means that the graphite structure is disrupted, resulting in defects. The generation of defects contributes to the formation of Li + Achieve inter-layer transmission, thereby improving Li + The transmission rate. Simultaneously, defects form electron wave scattering centers on the carbon surface, causing a decrease in the electronic conductivity of soft carbon. Figure 3 c). Figure 3 d- Figure 3 f shows the XPS spectrum of the SC-TU film. The carbon spectrum can be divided into four peaks: CC (284.6 eV), CS (286.0 eV), CN (288.5 eV), and CF (292.4 eV). CF is derived from the PTFE used for film formation, while the nitrogen spectrum can be divided into pyridine N (399.1 eV), pyrrole N (400.9 eV), and NO (404.8 eV). The sulfur spectrum can be divided into CS (163.2 eV), SO42-, and CS2-. 2- (167.4 eV). Therefore, we can infer that the calcination process of thiourea breaks some C-C bonds, forming C-S and CN bonds. This demonstrates that S- and N-doped C can effectively reduce Li... + The energy barrier for transmission. Furthermore, increasing the interlayer spacing can promote Li... + The transmission speed of SC-TU will be faster, so SC-TU will have faster Li + Its transmission capacity. Figure 3 g shows the Li values ​​of SC and SC-TU in the voltage range of 0V-0.1V. + The diffusion coefficient, measured using PITT, is readily apparent. It is not difficult to observe that the Li in SC-TU... + The diffusion coefficient is 2-3 times higher than that of SC. Therefore, the SC-TU-Li anode also achieves a higher exchange current density. Figure 3 h) and smaller overpotentials ( Figure 3 i) This is beneficial for the uniform deposition of metallic lithium. Figure 3 The Tafel curves in h show that the SC-TU-Li anode exhibits a 10-fold higher exchange current density than the SC-Li anode. This demonstrates that the interface layer of this invention can enhance the Li-to-Li exchange current density of the anode. + The diffusion coefficient is improved, and the anode also achieves a higher exchange current density and a smaller overpotential, which is beneficial for the uniform deposition of lithium metal.

[0079] We further investigated the improvement in the critical current density of the anode obtained by adjusting the mass ratio of soft carbon to thiourea in this invention. Figure 5 As can be seen, it uses an area capacity of 0.25mAh cm⁻¹ -2 Using a constant capacity testing method, we found that the critical current density (CCD) of the anode increases with the addition of thiourea. When the ratio exceeds 1:0.5, the CCD decreases slightly but remains higher than that below 1:0.5. We believe this is likely due to the increased amount of impurities remaining after calcination of thiourea. The high CCD demonstrates its better suppression of lithium dendrites; therefore, the SC-0.5TU anode achieves higher current density, rate performance, areal capacity, and energy density compared to anodes with other ratios. We further optimized the mass ratio of carbon material to organic compounds with thioamide groups to be 1:(0.5-1). Next, we conducted further research using a mass ratio of soft carbon and thiourea of ​​1:0.5 (Example 1) as an example.

[0080] We further investigated the electrochemical performance of batteries with the interface layer of this invention. Figure 4 a shows the critical current density (CCD) of SC-TU-Li, SC-Li, and Li anodes, using an areal capacity of 0.25 mAh cm⁻¹. -2 The constant capacity test method, in Figure 4 In a, it can be observed that the SC-TU-Li anode exhibits the highest CCD (up to 36 mA cm⁻¹). -2 While the CCD of SC-Li and Li anodes only reached 12 mA cm⁻¹. -2 and 4mA cm -2 Furthermore, SC-TU-Li symmetric cells can operate at a current density of 20 mA / cm². -2 The surface area capacity is 0.5mAh cm⁻¹ -2 (like Figure 4 Under the conditions shown in b), it stably cycled for over 18,000 times (900 hours). Figure 4 In c, SC-Li in a Li-symmetric cell at a current density of 2 mA cm⁻¹ -2 The surface area capacity is 2mAh cm -2 It short-circuits immediately after 35 cycles, which we believe is caused by the growth of Li dendrites, while the SC-TU-Li symmetric cell exhibits short circuits at 2 mA cm⁻¹. -2 (2mAh cm -2 Under these conditions, it can be cycled more than 750 times (1500 hours). Figure 4 d shows the coulombic efficiency (ACE) of SC-TU and SC anodes, where 3 mAh cm⁻¹ -2The lithium was first deposited onto a lithium-free anode, and then completely stripped after 50 cycles, resulting in an areal capacity of 0.5 mAh cm⁻¹. -2 It can be seen that the overpotential of the SC anode begins to increase after 35 cycles, indicating that the active lithium metal has been completely stripped and lithium in LiC6 (lithium hexacarbonide) has begun to be removed. Therefore, the ACE value of the SC-TU anode is 98%, while the ACE value of the SC anode is only 94%.

[0081] Because SC-TU has a higher exchange current density, it will have better rate performance, such as Figure 4 As shown in Figure e, the SC-TU anode exhibits the best rate performance. Surprisingly, the LCO / LPSCl / SC-TU-Li ASSB shows a rate performance of 15 mA / cm². -2 Ultra-high current density, with a capacity of 70mAh g -1 It also boasts an exceptionally long cycle life of 12,000 cycles with a capacity retention of 95%. Figure 4 h). Conversely, as Figure 6 As shown, the capacity of LCO / LPSCl / SC-Li ASSB decays to 0 after 2000 cycles. Figure 4 f- Figure 4 The charge-discharge curves in g show that the LCO / LPSCl / SC-Li ASSB exhibits high polarization and severe micro-short circuit problems during cycling, with an ACE of only 40%-60%. We believe this is due to the growth of lithium dendrites leading to increased interfacial side reactions and the formation of dead lithium, thus continuously increasing battery polarization and causing capacity decay. Furthermore, the LCO / LPSCl / SC-TU-Li ASSB (all-solid-state battery) can also achieve 50C (25mA cm⁻¹) -2 ) Repeat the cycle 18000 times (e.g.) Figure 4 i). exist Figure 4 Table 1 summarizes and compares the current densities of ASSBs in the literature, with the SC-TU-Li anode exhibiting an unprecedented current density, far exceeding the current highest level of ASSBs. This is attributed to S and N doping and the increased interlayer spacing, which broadens and increases the current density of Li. + The transmission channel greatly enhances Li's... + The spread of.

[0082] We further discovered that the SC-TU-Li anode not only exhibits ultra-high rate performance and ultra-high current density, but also ultra-high areal capacity. For example... Figure 7 a- Figure 7 As shown in b, the LCO / LPSCl / SC-TU-Li ASSB also exhibits good rate performance and cycling performance at high surface capacities, achieving a speed of up to 3 mAh cm⁻¹. -2Area capacity and 6mA cm -2 After 200 cycles at high current density, the capacity retention reached 93.8%. Notably, at 6mA cm⁻¹... -2 It is an ASSLMBs (all-solid-state lithium metal battery) with a high area capacity (>1mAh cm⁻¹). -2 The highest value under these conditions. However, LCO / LPSCl / SC-Li ASSB begins to exhibit micro-short circuits at 2C (e.g., Figure 8 and Figure 9 As shown in the diagram, this micro-short circuit significantly increases charging time, as lithium dendrites continuously penetrate the electrolyte, leading to rapid lithium depletion and capacity decay. Furthermore, the SC-TU-Li anode of this invention can also operate at ultra-high regional capacity (5 mAh cm⁻¹). -2 15mAh cm -2 and 20mAh cm -2 ),like Figure 7 As shown in c; LCO / LPSCl / SC-TU-LiASSB exhibits approximately 130 mAh g at 0.1C. -1 Specific capacity. To our knowledge, 20mAh cm⁻¹ -2 Far exceeding the highest area capacity of current all-solid-state, semi-solid-state, and polymer solid-state lithium metal batteries (e.g.) Figure 7 (as shown in e and Table 2), when the area capacity is 15mAh cm⁻¹ -2 LCO / LPSCl / SC-TU-Li ASSB can also be cycled 50 times at 0.1C (e.g.) Figure 7 d).

[0083] To demonstrate the practical application potential of this solid-state lithium metal battery system, the cathode and SE films were dry-rolled to 380 μm and 180 μm, respectively, using PTFE binder. Charge / discharge curves are shown... Figure 7 f, The percentage of active material in the cathode is 80%, and the areal loading of the active material is 60 mg / cm². -2 Its specific discharge capacity in the first cycle is 183.0 mAh g. -1 It provides an energy density of up to 403Wh / kg. -1 In addition, a square pouch-shaped battery with sides of 2 cm was assembled (e.g., Figure 7 (as shown in g), wherein the active material ratio of the cathode is 70%, and the areal loading of the active material is 39 mg / cm². -2 Its first-cycle discharge capacity is 173.0 mAh g. -1 It provides an energy density of 305Wh / kg. -1 This is the highest value of ASSLMB reported to date. Figure 7(as shown in h and Table 3). If the thickness of the SE film is reduced to <50 μm, the energy density can be further increased to >380 Wh kg. -1 .

[0084] In summary, a high-Li content was invented using soft carbon calcined with thiourea. + The high diffusion coefficient of the lithium metal anode promotes uniform deposition of lithium metal within the anode, thereby suppressing the growth of Li dendrites at ultra-high current densities. Thiourea produces NH3 and H2S during calcination; the hot gas molecules can widen the interlayer spacing of soft carbon, promoting Li... + The transport of NH3 and H2S can also attack C-C bonds, increasing the defectivity of soft carbon and forming C-S and CN bonds. The formation of defects makes Li... + Crossing between carbon layers increases transport paths, while CN and CS bonds can further reduce Li... + The transmission energy barrier, thus greatly increasing the Li + The diffusion rate of Li. + It can rapidly diffuse throughout the anode and deposit across the entire region, thereby reducing local current density and replenishing Li in a timely manner. + To prevent the growth of Li tree branches. Therefore, at 0.25 mAh cm⁻¹ -2 The area capacity of the lithium-ion symmetric battery is 36 mA cm⁻¹. -2 The ultra-high critical current density. The ASSB with SC-TU-Li anode and LCO cathode exhibited a high capacity retention of 95% (15 mA cm⁻¹) after 13,000 cycles at 30°C. -2 The current density and cycle life both break the records for the highest levels of solid-state batteries reported in the literature to date (8.6 mA cm⁻¹). -2 (and 10,000 cycles). 6mA cm -2 It is a high-capacity ASSLMB (>1mAh cm⁻¹) -2 It also boasts the highest value for 15mAh cm⁻¹. -2 The ultra-high areal capacity allows for cycling, enabling ASSB's device-level energy density to reach 403Wh / kg. -1 (like Figure 7 As shown in g), the assembled pouch battery has an energy density as high as 305 Wh / kg. -1 (like Figure 7 As shown in h), the areal capacity and energy density here also break the current record for solid-state lithium metal batteries (e.g., Figure 7(as shown in i). Last but not least, the SC-TU-Li anode presented in this work is composed of a low-cost composite material, making it readily adaptable to large-scale mass production. Therefore, these encouraging results demonstrate the enormous practical application potential of the SC-TU-Li anode reported in this work and may represent one of the most important breakthroughs in the development of ASSB.

[0085] It should be noted that the above description is only a preferred embodiment of the present invention and is not intended to limit the present invention. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the protection scope of the present invention.

[0086] References in Tables 1-3: Tables 1 and 3... Figure 4 The references for j are consistent, and Table 2 is consistent with them. Figure 7 The references for e are consistent, and Table 3 is consistent with them. Figure 7 The references for h are consistent.

[0087] [1]Xu R,Han F,Ji X,et al.Interface engineering of sulfideelectrolytes for all-solid-state lithium batteries[J].Nano Energy,2018,53:958-966.

[0088] [2]Ji X, Hou S, Wang P, et al. Solid-State Electrolyte Design for LithiumDendriteSuppression[J]. Advanced Materials, 2020, 32(46):e2002741.

[0089] [3]Chen Y, Li W, Sun C, et al. Sustained release-driven formationofultrastable sei betweenLi6PS5Cl and lithium anode for sulfide-based solid-state batteries[J]. Advanced EnergyMaterials, 2021,11(4):2002545.

[0090] [4]Cheng Z,Pan H,Li F,et al.Achieving long cycle life for all-solid-state rechargeable Li-I2battery by a confined dissolution strategy[J].Naturecommunications,2022,13(1):1-9.

[0091] [5]Liang J,Li X,Zhao Y,et al.In Situ Li3PS4 Solid-State ElectrolyteProtection Layers forSuperior Long-Life and High-Rate Lithium-Metal Anodes[J].Advanced Materials,2018,30(45):1804684.

[0092] [6]Kim C,Kim J,Park J,et al.Ion-Conducting Channel Implanted AnodeMatrix for All-Solid-State Batteries with High Rate Capability and StableAnode / Solid ElectrolyteInterface[J].Advanced Energy Materials,2021,11(40):2102045.

[0093] [7]Lee K,Han S,Lee J,et al.Multifunctional Interface for High-Rateand Long-DurableGarnet-Type Solid Electrolyte in Lithium Metal Batteries[J].ACS Energy Letters,2021,7(1):381-389.

[0094] [8]Wan H,Zhang J,Xia J,et al.F and N Rich Solid Electrolyte forStable All-Solid-StateBattery[J].Advanced Functional Materials,2022,32(15):2110876.

[0095] [9]Zhou L,Zuo T-T,Kwok C Y,et al.High areal capacity,long cycle life4V ceramicall-solid-state Li-ion batteries enabled by chloride solidelectrolytes[J].Nat Energy,2022,7(1):83-93.

[0096]

[10] Peng L,Yu C,Zhang Z,et al.Chlorine-rich lithium argyroditeenabling solid-statebatteries with capabilities of high voltage,high rate,low-temperature and ultralongcyclability[J].Chem Eng J,2022,430.

[0097]

[11] Tan D H,Chen Y-T,Yang H,et al.Carbon-free high-loading siliconanodes enabled bysulfide solid electrolytes[J].Science,2021,373(6562):1494-1499.

[0098]

[12] Lee Y-G,Fujiki S,Jung C,et al.High-energy long-cycling all-solid-state lithium metalbatteries enabled by silver–carbon composite anodes[J].Nature Energy,2020,5(4):299-308.

[13] Kim D H,Oh D Y,Park K H,etal.Infiltration of solution-processable solid electrolytesinto conventionalLi-ion-battery electrodes for all-solid-state Li-ion batteries[J].Nanoletters,2017,17(5):3013-3020.

[0099]

[14] Ye L,Li X.A dynamic stability design strategy for lithium metalsolid state batteries[J].Nature,2021,593(7858):218-222.

[0100]

[15] Xing X,Li Y,Wang S,et al.Graphite-Based Lithium-Free 3D HybridAnodes for HighEnergy Density All-Solid-State Batteries[J].ACS Energy Lett,2021,6(5):1831-1838.

[0101]

[16] Liu Y,Lin D,Jin Y,et al.Transforming from planar to three-dimensional lithium withflowable interphase for solid lithium metal batteries[J].Science advances,2017,3(10):eaao0713.

[0102]

[17] Zhang Z,Chen S,Yao X,et al.Enabling high-areal-capacity all-solid-state lithium-metalbatteries by tri-layer electrolyte architectures[J].Energy Storage Mater,2020,24:714-718.

[0103]

[18] Zhu G L,Zhao C Z,Peng H J,et al.A Self-Limited Free-StandingSulfide ElectrolyteThin Film for All-Solid-State Lithium Metal Batteries[J].Adv Funct Mater,2021,31(32).

[0104]

[19] Santhosha A L,Nazer N,Koerver R,et al.Macroscopic DisplacementReaction ofCopperSulfide in Lithium Solid-State Batteries[J].Adv EnergyMater,2020,10(41).

[0105]

[20] Yan H,Wang H,Wang D,et al.In Situ Generated Li(2)S-CNanocomposite forHigh-Capacity and Long-Life All-Solid-State Lithium SulfurBatteries with Ultrahigh ArealMass Loading[J].Nano Lett,2019,19(5):3280-3287.

[0106]

[21] Doerrer C,Capone I,Narayanan S,et al.High Energy Density Single-CrystalNMC / Li(6)PS(5)Cl Cathodes for All-Solid-State Lithium-Metal Batteries[J].ACS Appl MaterInterfaces,2021,13(31):37809-37815.

[0107]

[22] Li X,Liang J,Luo J,et al.High-Performance Li-SeS(x)All-Solid-State LithiumBatteries[J].Adv Mater,2019,31(17):e1808100.

[0108]

[23] Han X,Wang S,Xu Y,et al.All solid thick oxide cathodes based onlow temperaturesintering for high energy solidbatteries[J].Energy EnvironSci,2021,14(9):5044-5056.

[0109]

[24] Nam Y J,Cho S J,Oh D Y,et al.Bendable and thin sulfide solidelectrolyte film:a newelectrolyte opportunity for free-standing and stackablehigh-energy all-solid-state lithium-ionbatteries[J].Nano Lett,2015,15(5):3317-23.

[0110]

[25] Jiang T,He P,Wang G,et al.Solvent-Free Synthesis of Thin,Flexible,NonflammableGarnet-Based Composite Solid Electrolyte for All-Solid-State Lithium Batteries[J].AdvEnergy Mater,2020,10(12).

[0111]

[26] Kim D H,Lee Y-H,Song Y B,et al.Thin and Flexible SolidElectrolyte Membranes withUltrahigh Thermal Stability Derived from Solution-Processable Li Argyrodites forAll-Solid-State Li-Ion Batteries[J].ACS EnergyLett,2020,5(3):718-727.

[0112]

[27] Hippauf F,Schumm B,Doerfler S,et al.Overcoming binder limitationsof sheet-typesolid-state cathodes using a solvent-free dry-film approach[J].Energy Storage Mater,2019,21:390-398.

[0113]

[28] Sakuda A,Kuratani K,Yamamoto M,et al.All-Solid-State BatteryElectrode SheetsPrepared by a Slurry Coating Process[J].J Electrochem Soc,2017,164(12):A2474-A2478.

[0114]

[29] Zhang Z,Wu L,Zhou D,et al.Flexible Sulfide Electrolyte ThinMembrane withUltrahigh Ionic Conductivity for All-Solid-State LithiumBatteries[J].Nano Lett,2021,21(12):5233-5239.

[0115]

[30] Wang C,Yu R,Duan H,et al.Solvent-Free Approach for InterweavingFreestanding andUltrathin Inorganic Solid Electrolyte Membranes[J].ACS EnergyLett,2021,7(1):410-416.

[0116]

[31] Liu G,Shi J,Zhu M,et al.Ultra-thin free-standing sulfide solidelectrolyte film forcell-level high energy density all-solid-state lithiumbatteries[J].Energy Storage Mater,2021,38:249-254.

Claims

1. An interface layer with a high diffusion coefficient, characterized in that, The interface layer has characteristic peaks at 25°, 44°, and 45° in the X-ray powder diffraction pattern expressed as a diffraction angle of 2θ. The raw materials for the interface layer include carbon materials, organic compounds with thioamide groups, and film-forming agents; The thioamide group has structural formula I: (Structure I).

2. The interface layer with a high diffusion coefficient according to claim 1, characterized in that, The mass ratio of the carbon material to the organic compound having thioamide groups is 1:(0.125-1).

3. The interface layer with a high diffusion coefficient according to claim 1, characterized in that, The mass ratio of the carbon material to the organic compound having thioamide groups is 1:(0.5-1).

4. The interface layer with a high diffusion coefficient according to claim 1, characterized in that, The carbon material includes one or more of soft carbon and hard carbon; the organic compound having a thioamide group includes one or more of thiourea and thioacetamide; the film-forming agent includes one or more of polytetrafluoroethylene, polyethylene, polyhexafluoropropylene, and styrene-butadiene rubber.

5. The interface layer with a high diffusion coefficient according to claim 4, characterized in that, The soft carbon includes one or more of graphite, petroleum coke, needle coke, carbon fiber, and carbon microspheres; the hard carbon includes one or more of resin carbon, organic polymer carbon, carbon black, and biomass carbon.

6. The interface layer with a high diffusion coefficient according to claim 1, characterized in that, The thickness of the interface layer is 25μm-35μm.

7. The method for preparing the interface layer according to any one of claims 1-6, characterized in that, The preparation method includes: Weigh the carbon material and the organic compound with thioamide groups according to the mass ratio, mix them, and calcine the mixed carbon material and the organic compound with thioamide groups in an inert atmosphere to obtain a composite. The composite is then mixed with a film-forming agent and dry-rolled to form a film to obtain an interface layer.

8. The preparation method according to claim 7, characterized in that, The mass ratio of the composite to the film-forming agent is 100:3; The calcination temperature is 300℃-500℃, and the calcination time is 4h-6h; The inert atmosphere includes one of nitrogen, argon, helium, neon, krypton, and xenon.

9. A lithium metal anode comprising the interface layer according to any one of claims 1-6.

10. A cathode comprising the interface layer according to any one of claims 1-6.

11. A membrane comprising the interface layer according to any one of claims 1-6.

12. The lithium-containing anode according to claim 9, characterized in that, The lithium metal-containing anode including the interface layer has an areal capacity of 5 mAh cm⁻¹. -2 above.

13. The lithium-containing anode according to claim 9, characterized in that, The lithium metal-containing anode including the interface layer has an areal capacity of 15 mAh cm⁻¹. -2 above.

14. The lithium-containing anode according to claim 9, characterized in that, The lithium metal-containing anode including the interface layer has an areal capacity of 20 mAh cm⁻¹. -2 above.

15. A battery, characterized in that, The battery includes the interface layer as described in any one of claims 1-6.

16. The battery according to claim 15, characterized in that, The battery includes a sulfide all-solid-state lithium metal battery.

17. An electrochemical device, characterized in that, The electrochemical device comprises the interface layer as described in any one of claims 1-6.

Images