Application of astaxanthin as electronic switch in three-phase interface regulation and control of all-solid-state lithium-sulfur battery

By introducing astaxanthin as an electronic switch into the all-solid-state lithium-sulfur battery, the problem of three-phase interface instability is solved, the initial capacity, cycle stability and high-rate performance of the battery are improved, and wide temperature range adaptability and mechanical stability are achieved.

CN121688052APending Publication Date: 2026-03-17Wenzhou University Carbon Materials and Hydrogen Energy Industry Technology Research Institute +1
View PDF 0 Cites 0 Cited by

Patent Information

Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-12-19
Publication Date
2026-03-17

AI Technical Summary

Technical Problem

In all-solid-state lithium-sulfur batteries, the instability of the three-phase interface leads to a decline in battery performance, including slow sulfur redox reaction kinetics, hindered charge transport, and electrochemical-mechanical failure, which are particularly evident under high load and wide temperature range.

Method used

Astaxanthin was introduced as an electronic switch to regulate the decomposition pathway of sulfide solid electrolytes through the electronic pocket effect, promote the generation of Li2S active materials, construct low-potential channels to promote Li+ transport, and serve as a flexible molecular scaffold to alleviate volume expansion and maintain interfacial contact stability.

Benefits of technology

It significantly improves the initial capacity and cycle stability of the battery, enhances high-rate performance and wide-temperature adaptability, achieves high capacity output and mechanical stability, and solves the technical bottleneck of unstable three-phase interface.

✦ Generated by Eureka AI based on patent content.

Smart Images

  • Figure CN121688052A_ABST
    Figure CN121688052A_ABST
Patent Text Reader

Abstract

The invention provides application of astaxanthin as an electronic switch in three-phase interface regulation and control of an all-solid-state lithium-sulfur battery, belongs to the technical field of battery materials, and aims to solve the problems that a three-phase interface formed by a sulfur active material, a conductive carbon material and a sulfide solid electrolyte in the all-solid-state lithium-sulfur battery is unstable, and the stability of the three-phase interface is poor. In order to solve the technical problems of slow sulfur conversion kinetics, blocked charge transfer and mechanical failure caused by low sulfur conversion rate, low sulfur conversion kinetics, blocked charge transfer and mechanical failure in the prior art, astaxanthin serving as an additive with the proportion of 0.5-10wt% is doped into a battery cathode composite material, and the multi-dimensional coordinated regulation and control of a three-phase interface are realized by utilizing the electronic switch effect of the astaxanthin; the generation of a Li2S active material instead of an inert by-product is promoted; a low-potential channel is constructed by hydroxyl and carbonyl functional groups so as to promote Li < + > transmission and catalyze a sulfur redox reaction; by using a chain structure as a flexible molecular scaffold, the volume expansion of the sulfur cathode is relieved, and the interface contact stability is maintained.
Need to check novelty before this filing date? Find Prior Art

Description

Technical Field

[0001] This invention relates to the field of battery materials technology, and in particular to the application of astaxanthin as an electronic switch in the three-phase interface regulation of all-solid-state lithium-sulfur batteries. Background Technology

[0002] Amidst the current wave of technological upgrades and iterations in new energy storage, high-energy-density and high-safety rechargeable batteries have become a core research and development direction in the energy storage field. Lithium-sulfur (Li-S) batteries, due to the high energy density of elemental sulfur (up to 2600Wh / kg), are particularly promising. -1 With its high theoretical energy density and abundant, low-cost raw materials, Li-S batteries are considered one of the most promising next-generation energy storage technologies. However, traditional liquid electrolyte Li-S batteries suffer from severe shuttle effects, which not only cause irreversible capacity decay and shorten cycle life, but also pose significant safety hazards due to the flammability of liquid electrolytes, making them unsuitable for practical applications. Against this backdrop, all-solid-state lithium-sulfur batteries (ASSLSBs), which use non-flammable solid electrolytes (SEs) to replace liquid electrolytes, have become a key technological path to eliminate shuttle effects and improve battery energy density and safety. Among them, sulfide solid electrolytes (SSEs) have a theoretical energy density >10 -3 S cm -1 Its superior ionic conductivity, good mechanical deformability, and excellent compatibility with sulfur cathodes make it stand out among various solid electrolytes, making ASSLSBs a research hotspot in the field of energy storage.

[0003] To overcome the technical bottleneck of instability at the three-phase interface formed by sulfur-containing active materials, conductive agents, and sulfur oxides (SSEs) in ASSLSBs, researchers have conducted extensive targeted studies. The most representative approach involves optimizing the electrode structure by introducing various conductive carbon materials, such as carbon doping modification, constructing carbon nanocages, and building three-dimensional carbon frameworks. These methods aim to enhance the electron conductivity of the electrode and improve the ion and electron transport efficiency within the cathode, attempting to establish a stable three-phase interface. Simultaneously, some studies have also explored ways to improve interfacial compatibility from the perspectives of electrolyte modification and electrode interface modification. Experimental data show that these approaches can indeed improve the cycle stability of batteries to some extent under low sulfur loading conditions and increase the kinetic rate of the sulfur redox reaction (SRR), providing preliminary technical support for the performance optimization of ASSLSBs.

[0004] Despite the progress made in current research, the application of ASSLSBs remains limited by a series of core problems caused by the three-phase interface, and the drawbacks of traditional conductive carbon modification schemes are particularly prominent in high-sulfur loading scenarios. Firstly, as the sulfur loading increases, the cathode thickness inevitably increases, and the long-range conductive path deteriorates rapidly, leading to Li… +Firstly, the electron conduction efficiency decreases significantly. Secondly, the insulation properties of sulfur require that the composite cathode under high sulfur load contains a large amount of conductive carbon, the presence of which will cause a significant increase in local specific surface area, thereby triggering violent electrolyte decomposition. The strong transfer of electrons from the PS bond to the Li-Cl bond will generate inert lithium chloride and accumulate at the interface, hindering interfacial mass transfer and inhibiting surface reaction kinetics. Thirdly, elemental sulfur will generate about 80% volume expansion during charging and discharging, causing severe mechanical stress and strain, resulting in the separation of the interface between active sulfur and SSEs and conductive carbon, damaging the solid-solid conductive contact.

[0005] Furthermore, existing technologies have not reported on the controllable adjustment of electrolyte decomposition pathways. In summary, the various problems in ASSLSBs ultimately lead to multiple challenges, including slow solid-solid SRR kinetics, hindered charge transport, and electrochemical-mechanical failure, making it difficult to meet the practical application requirements of high loads and long cycles. Summary of the Invention

[0006] To overcome the shortcomings of existing technologies, the purpose of this invention is to provide an application of astaxanthin as an electronic switch in the three-phase interface regulation of all-solid-state lithium-sulfur batteries. This invention incorporates astaxanthin as an additive in the battery cathode composite material at a ratio of 0.5~10 wt%, utilizing its electronic switching effect to achieve multi-dimensional synergistic regulation of the three-phase interface: it regulates the decomposition pathway of sulfide solid electrolytes through the electron pocket effect, promoting the formation of Li2S active materials rather than inert byproducts; and it constructs low-potential channels based on hydroxyl and carbonyl functional groups to promote Li... + It transports and catalyzes sulfur oxidation-reduction reactions; its chain-like structure acts as a flexible molecular scaffold, mitigating sulfur cathode volume expansion and maintaining interfacial contact stability.

[0007] To achieve the above objectives, the present invention provides the following solution: An application of astaxanthin as an electronic switch in the three-phase interface regulation of an all-solid-state lithium-sulfur battery is disclosed. The astaxanthin, acting as an electronic switch, dynamically regulates the three-phase interface of the all-solid-state lithium-sulfur battery through the electronic pocket effect. The three-phase interface is the interface between sulfur-active materials, conductive carbon materials, and a sulfide solid electrolyte. The regulation of the three-phase interface includes one or more of the following: regulating the decomposition pathway of the sulfide solid electrolyte to promote the formation of Li₂S active materials; constructing low-potential channels to promote Li₂S… + It transports and catalyzes sulfur oxidation-reduction reactions; it also acts as a flexible molecular scaffold to alleviate the volume expansion of the sulfur cathode and maintain interfacial contact stability.

[0008] According to specific embodiments provided by the present invention, the present invention discloses the following technical effects: (1) This invention achieves dynamic and controllable adjustment of the decomposition path of the sulfide solid electrolyte in all-solid-state lithium-sulfur batteries, effectively suppressing the generation of inert lithium chloride passivation reaction interface during electrolyte decomposition, while generating more active materials to provide capacity. This invention uses astaxanthin as an electronic switch, restricting electron migration through the electron pocket effect, allowing it to preferentially interact with its own oxygen sites, polarizing and weakening the PS bond in the sulfide solid electrolyte, inhibiting the formation of Li-Cl bonds, and promoting the directional decomposition of the electrolyte to generate Li2S active material; at the same time, by controlling the doping ratio of astaxanthin in the cathode composite material from 0.5 to 10 wt%, the generation ratio of active material and by-products can be balanced. Compared with batteries without astaxanthin modification, it can significantly improve the initial capacity of the battery, achieving an initial discharge specific capacity of not less than 1685.5 mAh·g at 0.1C rate. -1 Furthermore, the sulfur utilization rate is greater than 100%, laying a material foundation for the high-capacity output of the battery.

[0009] (2) This invention constructs a highly efficient lithium-ion transport and sulfur redox catalytic system, solving the technical problems of slow kinetics and hindered charge transport in the solid-solid sulfur redox reaction (SRR) of all-solid-state lithium-sulfur batteries. This invention relies on the hydroxyl and carbonyl functional groups of the astaxanthin molecule to form a low-potential region, providing a suitable catalytic environment for Li-ion transport and sulfur redox reactions. + Migration and setup of a dedicated channel to transfer Li + The migration barrier is reduced to 0.17 eV, significantly improving ion transport efficiency; simultaneously, astaxanthin catalyzes sulfur oxidation-reduction reactions, reducing electrochemical polarization, enabling the battery to maintain a capacity of no less than 839.4 mAh·g at a high rate of 1C. -1 The battery exhibits excellent rate performance and electrochemical reversibility, and retains 96.7% of its capacity when the discharge rate is restored to 0.1C, effectively improving the defect of rapid capacity drop at high rates in traditional batteries.

[0010] (3) This invention improves the mechanical stability and wide temperature range adaptability of all-solid-state lithium-sulfur batteries, and solves the electrochemical-mechanical failure problem caused by volume expansion under high sulfur load. In this invention, the chain structure of astaxanthin can serve as a flexible molecular scaffold to alleviate the volume expansion of the sulfur cathode during charging and discharging, and maintain the tight interfacial contact between the electrode and the electrolyte; based on this, the battery exhibits excellent cycle stability under different sulfur load scenarios, with a cycle stability of 1.46 mg·cm⁻¹. -2 After 300 cycles at sulfur loading and 0.2C rate, the coulombic efficiency is not less than 99.95% and the cycle decay rate is not greater than 0.082%, at 6.45 mg·cm⁻¹. -2 With 8.63 mg·cm -2 Under high sulfur load, the capacity retention rates after 100 cycles reached 84.9% and 78.8%, respectively; meanwhile, the battery can operate stably in a wide temperature range of -10℃ to 60℃, and still maintains 1191.31 mAh·g at a low temperature of -10℃.-1 The discharge capacity provides reliable support for the industrial application of high-load, wide-temperature-range all-solid-state lithium-sulfur batteries. Attached Figure Description

[0011] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the embodiments 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.

[0012] Figure 1 A schematic diagram illustrating the triple mechanism of astaxanthin as a multifunctional additive in all-solid-state lithium-sulfur batteries, as provided in an embodiment of the present invention. Figure 2 This is a comprehensive characterization and theoretical calculation diagram of the AXT-regulated ASSLSB interface decomposition and potential mechanism provided in an embodiment of the present invention; wherein, Figure 2 In the figure, 'a' represents the constant current charge-discharge curve of the symmetrical battery during the first four cycles. Figure 2 In this context, b represents the KB / S cathode under different AXT doping ratios. 31 p NMR spectrum, Figure 2 In the figure, c represents the Li 1s XPS spectra of the KB / S cathode with different AXT doping ratios after the first discharge. Figure 2 In the diagram, d represents the differential charge density map of AXT / LPSC under different AXT coverage rates. Figure 2 In the diagram, 'e' represents the bond order changes in the decomposition reaction of the electrolyte under different AXT coverage levels. Figure 2 f in the figure represents the energy barrier diagram of the decomposition reaction of the electrolyte under different AXT coverage. Figure 3 This is a comprehensive test and theoretical calculation diagram of the catalytic ability of AXT for sulfur redox reactions provided in an embodiment of the present invention; wherein, Figure 3 In the figure, 'a' represents the contour plot of the cyclic voltammograms of the cell with an AXT-modified cathode at different scan rates. Figure 3 In the diagram, b represents the two-dimensional intensity mapping of the DRT calculated from the in-situ EIS results. Figure 3 In the figure, c represents the Gibbs free energy diagram of sulfur species adsorbed at the Gh and Gh-AXT interfaces. Figure 3 d in Li + Migration energy barrier diagram at the Gh and Gh-AXT interfaces Figure 3 In the figure, e represents the electrostatic potential mapping of Gh and Gh-AXT; Figure 4 This is an in-situ detection and simulation analysis diagram of the mechanical behavior of AXT-optimized ASSLSBs provided in an embodiment of the present invention; wherein, Figure 4In the diagram, 'a' represents a schematic diagram of pressure monitoring in an all-solid-state Li-S battery. Figure 4 b in the figure is 0.3 mA·cm -2 Time-dependent changes in the electrochemical-stress curves of the KB / S-0.5% AXT battery under current during the first 5 cycles. Figure 4 c is 0.3 mA·cm -2 Time-dependent changes in the electrochemical-pressure curves of the KB / S battery under different currents during the first 5 cycles. Figure 4 d is 0.3 mA·cm -2 Time-dependent changes in the electrochemical-pressure curves of an LTO-Li metal battery under different currents during the first five cycles. Figure 4 In the figure, 'e' represents the decoupled pressure variation curves for KB / S - 0.5% AXT and KB / S. Figure 4 In the figure, f is a Forcite molecular dynamics simulation diagram of the interlayer of two different materials after embedding 40 Li ions. Figure 4 In the diagram, g represents the volume expansion ratio of the Gh and Gh-AXT systems; Figure 5 This is a comprehensive evaluation and comparison chart of the electrochemical performance of AXT-modified ASSLSBs provided in the embodiments of the present invention; wherein, Figure 5 In the figure, 'a' represents the rate performance of ASSLSBs with different AXT doping ratios. Figure 5 In the figure, b represents the charge-discharge curves of ASSLSBs with different AXT doping ratios at 0.5C. Figure 5 In the figure, c represents the long-cycle test graph of ASSLSBs with different AXT doping ratios at 0.5C for 300 cycles. Figure 5 In the figure, d represents the ASSLSB cycle stability plot of 0.5% AXT at 0.2C. Figure 5 In this context, 'e' represents the 6.45 mg·cm³ of high-sulfur-loaded ASSLSBs at 30°C. -2 Cyclic performance diagram under sulfur loading Figure 5 f in the figure represents 9.49 mg·cm³ of high-sulfur-loaded ASSLSBs at 60 °C. -2 Cyclic performance diagram under sulfur loading Figure 5 In the figure, g represents a comparison of the electrochemical performance of AXT-modified ASSLSBs with that of previous studies. Detailed Implementation

[0013] To make the above-mentioned objects, features and advantages of the present invention more apparent and understandable, the present invention will be further described in detail below with reference to the accompanying drawings and specific embodiments.

[0014] Example 1 Astaxanthin (AXT), a natural carotenoid, is hailed as the king of antioxidants. Based on its excellent structure and properties, it has been widely used in aquaculture, nutritional supplements, and cosmetics: AXT contains unsaturated hydroxyl and ketone groups, which can attract unpaired electrons from external molecules or donate electrons to the outside. This unique structure endows it with significant antioxidant activity, accelerates SRR kinetics, and plays an important role in regulating electrolyte decomposition; the high sensitivity of AXT's conjugated double bond chain to excited states enables it to participate in electron / ion transfer and lower the energy barrier, demonstrating AXT's good interfacial stability; AXT's rigid chain structure can enhance the system's flexibility and interfacial adhesion, and is expected to buffer the volume changes of sulfur cathodes.

[0015] Based on the above, such as Figure 1 As shown, this embodiment introduces AXT into a carbon / sulfur (C / S) composite cathode material to construct a smooth sulfur conversion interface for high-sulfur-loaded and high-capacity ASSLSBs. Electrochemical studies, including in-situ electrochemical impedance spectroscopy (EIS), in-situ pressure testing, and theoretical simulations, reveal that an appropriate amount of AXT can accelerate electrolyte decomposition through a local electron pocket effect, generating more active materials rather than byproducts, thereby increasing battery capacity. Simultaneously, aided by the low-potential channels surrounding oxygen-containing functional groups, AXT can also establish an efficient electron and ion transport network at the cathode / electrolyte interface, activating the sulfur redox reaction. More importantly, thanks to its flexible confinement and support capabilities, AXT can effectively suppress cathode volume expansion, ensuring close contact between the cathode and the SSE. Ultimately, AXT-doped ASSLSBs exhibit a capacity of 1685.5 mAh·g at 0.1C. -1 It exhibits high initial capacity (corresponding to sulfur utilization >100%), significant rate performance at 1C, and maintains stable cycling performance even under low loading of highly active materials. At a sulfur loading of 1.46 mg / cm³... -2 At that time, AXT-modified ASSLSB exhibited a current density of 1629.1 mAh·g at 0.2C. -1 It exhibits high initial capacity, a low cycle decay rate of 0.082%, and maintains a coulombic efficiency of 99.95% after 300 cycles; even under high sulfur loading (initial areal capacities of 9.35 and 10.01 mAh·cm³, respectively). -2 The concentrations were 6.45 and 8.63 mg cm, respectively. -2 It maintains 84.9% and 78.8% of its capacity under sulfur loading for more than 100 cycles and still exhibits excellent electrochemical performance over a wide temperature range (-10 to 60 °C).

[0016] The following specific experiment will further illustrate the above content. This experiment requires the preparation of a basic sulfur-carbon composite material first, and then the preparation of a composite cathode with / without astaxanthin (AXT). The specific process is as follows: The melt diffusion method was used to select Ketjen black (KB, model ECP600JD) and high-purity elemental sulfur (S, purity 99.99%) as raw materials and mix them thoroughly at a mass ratio of 3:7. The mixture was heated to 155℃ and kept at a constant temperature for 12 hours to ensure that the elemental sulfur completely melted and impregnated into the carbon matrix, thus obtaining the KB / S sulfur-carbon composite material.

[0017] The composite cathode was prepared by high-energy ball milling. The above-mentioned KB / S sulfur-carbon composite material was mixed with sulfide solid electrolyte Li6PS5Cl (LPSC) at a weight ratio of 4:6 and loaded into a sealed zirconium dioxide ball mill jar. The ball mill speed was set to 500 rpm and the ball milling was continued for 6 hours to obtain the KB / S composite cathode material.

[0018] In the above-mentioned KB / S and LPSC mixed system, astaxanthin (AXT, purity 96%) was added in an additional 0.5~10wt% of the total mass of the cathode composite material, and then the same high-energy ball milling process (i.e. 500 rpm, 6 hours) was used to obtain KB / S-AXT composite cathode material.

[0019] All-solid-state lithium-sulfur batteries (ASSLSB) were assembled using the prepared KB / S composite cathode material and KB / S-AXT composite cathode material. The entire process was carried out in a glove box with a water oxygen content of <0.1ppm. The specific procedure was as follows: First, 100 mg of LPSC electrolyte powder was weighed and placed in a 10 mm diameter polyetheretherketone (PEEK) sleeve, and cold-pressed at 200 MPa to form a dense solid electrolyte layer. Then, the prepared KB / S or KB / S-AXT composite cathode powder was pressed at 1~1.5 mg·cm⁻¹. -2 A sulfur mass loading is applied to one side of the solid electrolyte layer under a pressure of 200 MPa, and the pressure is maintained for 3 minutes to ensure tight interfacial contact. Finally, the lithium metal or Li-In alloy anode is cut into 10 mm diameter disks and attached to the other side of the solid electrolyte layer under a pressure of 100 MPa, completing the overall electrode-electrolyte assembly. To maintain tight solid-solid interface contact during battery cycling, an additional 50 MPa pressure is provided to the assembled battery via a stainless steel frame. Furthermore, if a symmetrical battery is to be prepared for interfacial performance testing, both the positive and negative electrodes use 10 mg of KB / S or KB / S-AXT cathode composite material; the remaining assembly process is the same as described above.

[0020] After completing the fabrication of KB / S and KB / S-AXT composite cathodes and the assembly of ASSLSB batteries, in order to verify the regulatory effect of AXT on the three-phase interface of all-solid-state lithium-sulfur batteries and the related performance improvement effect, a series of electrochemical tests, spectroscopic characterization and theoretical simulation experiments were carried out in three major directions: interface decomposition path regulation, sulfur oxidation-reduction reaction catalysis and mechanical stability optimization.

[0021] Example 2 Given that the cathode in ASSLSBs is a mixture of sulfur-active materials, sulfur-based electrolytes (SSEs) such as Li6PS5Cl (LPSC) and conductive carbon additives such as Ketjen Black (KB) , the carbon material typically initiates severe degradation reactions of the SSEs at the electrolyte / cathode interface. To understand the specific impact of AXT on the interfacial state, AXT at different mass ratios was added to the cathode composite material using a high-energy ball milling method and thoroughly mixed for subsequent experiments.

[0022] This embodiment aims to conduct experiments to decompose the AXT-controlled ASSLSB interface and verify its potential mechanisms, specifically including: AXT at different mass ratios was added to the cathode composite material using a high-energy ball milling method and thoroughly mixed for symmetric cell testing. In the experiment, symmetric cells containing 10 mg of cathode composite powder (with or without AXT) were specifically assembled, namely KB / S|LPSC|KB / S and KB / Sx%AXT|LPSC|KB / Sx%AXT cells (x=0.5, 2.5, 5), and subjected to four charge-discharge cycles within a voltage range of -0.7V to 0.7V.

[0023] like Figure 2 As shown in a, the KB / S|LPSC|KB / S battery exhibited 66.04 mAh·g in the first cycle. -1 The discharge capacity and 129.16 mAh·g -1 The charging capacity is [not specified]. In comparison, the KB / S-0.5%AXT|LPSC|KB / S-0.5%AXT battery shows a higher initial charge / discharge capacity, with a discharge capacity of 75.48 mAh·g. -1 The charging capacity is 145.75mAh·g -1 Furthermore, its charge-discharge capacity remained stable in the subsequent three cycles. This capacity improvement after AXT doping is attributed to the enhanced decomposition reaction of SSEs, resulting in the generation of additional sulfur / Li₂S active material. Subsequently, the capacity of the symmetric cell gradually decreased with increasing AXT doping concentration. When the AXT additive reached 5%, the symmetric cell exhibited negligible charge-discharge capacity, with a discharge capacity of 7.08 mAh·g⁻¹. -1 The charging capacity is 12.23mAh·g -1This is because when there is too much AXT, it will inhibit electrolyte decomposition, reduce the amount of sulfur / Li2S active material produced, and generate more by-products. This proves that adding AXT appropriately to the cathode composite material helps to regulate the electrolyte decomposition pathway (i.e., balance the generation of active materials and by-products) and improve the battery capacity.

[0024] To further confirm the controllability of AXT in electrolyte decomposition, this embodiment tested the CV curves of the LPSC / KB-AXT cathode cell. Preliminary experiments showed that AXT had no redox peaks in the 1.5-3V operating voltage range, while LPSC electrolytes typically undergo reduction decomposition below 1.7V and oxidation decomposition above 2.5V. Therefore, the peak intensity in the first CV cycle directly reflects the degree of electrolyte decomposition. Test results showed that the 0.5% AXT modified battery exhibited significantly higher decomposition peak intensities at 1.5V and 3V than other groups, proving that electrolyte decomposition was most complete at this ratio. In subsequent cycles, the CV curve of this battery also showed a 2V reduction peak and a 2.6V oxidation peak, which are characteristic sulfur redox peaks, and their peak intensities were the highest among all groups. Since no sulfur was added to the cathode, this signal could only originate from the active sulfur produced by electrolyte decomposition, further confirming that 0.5% AXT can maximize the induction of electrolyte decomposition to generate active materials.

[0025] Furthermore, by calculating the ratio of the first-cycle charge capacity to the discharge capacity (ASSLSB exhibits a characteristic where the first-cycle charge capacity is greater than the discharge capacity due to electrolyte decomposition), it can be found that the capacity ratio of the 0.5% AXT battery is 1.14, which is higher than that of the undoped AXT (1.11), 2.5% AXT (1.09), and 5% AXT (1.04) batteries. This quantitatively verifies that 0.5% AXT can enhance electrolyte decomposition. Therefore, it can be concluded that by appropriately adding AXT, SSE decomposition can be regulated, thereby generating active materials to enhance capacity.

[0026] To explore its underlying mechanism, this embodiment also conducted solid-state nuclear magnetic resonance, X-ray photoelectron spectroscopy (XPS) studies, and density functional theory (DFT) calculations. The initial LPSC electrolyte was at the cathode... 31 The p-NMR spectrum can be decomposed into three distinct components: PSCl3, PS2Cl2, and PSCl3. - and PS3Cl 2- It is worth noting that after introducing 0.5% AXT into the cathode, 31 The characteristic PO bond at 77.1 ppm was almost undetectable in the PO NMR spectrum, referring to... Figure 2b. With increasing AXT content, the strength of the PO bond increases proportionally. The P 2p XPS spectrum of the AXT-doped cathode composite further confirms the formation of the PO bond, with significant POP peaks detected at 133.75 / 133.86 eV. Since all experiments were conducted in a glove box (O2 and water <0.01 ppm), the O element in the PO bond is considered to originate from AXT. That is, excess AXT induces the structural evolution of the original cathode composite by forming PO bonds, thereby inhibiting electrolyte decomposition. The altered cathode structure can also be verified by the XRD results of the AXT-modified cathode composite, where the diffraction peaks caused by LPSC on the AXT-modified sample shift to a lower angle, indicating that AXT leads to an increase in the lattice spacing of the LPSC electrolyte.

[0027] To further clarify the ratio of active materials to electrolyte decomposition byproducts, Li 1s XPS spectroscopy was used in the experiment to analyze the existing forms and chemical states of lithium chloride, since lithium chloride is a redox product of electrolyte decomposition. Figure 2 As shown in c, compared to the original cathode (55.39 eV), the Li 1s peak after the first discharge of the KB / S-0.5% AXT cathode shifted by 0.21 eV towards a lower binding energy, indicating that after doping with 0.5% AXT, the decomposition products tend to become the active material Li₂S. Meanwhile, the Li 1s peaks of the cathodes doped with 2.5% and 5% AXT shifted by 0.08 eV and 0.38 eV towards higher binding energies, respectively, due to the formation of more lithium chloride.

[0028] Theoretically, based on DFT calculations, as the AXT coverage increases, the adsorption energy between SSEs and AXT decreases from -2.97 eV to -6.25 eV. This demonstrates that the gain of each AXT molecule is sublinear, indicating the existence of π-π interactions between AXT molecules. Intermolecular π-π stacking compresses / densifies the Li-Cl shell to a narrower and more uniform range, spatially preventing S escape and pre-stabilizing the Li-Cl transition state electronically, thus favoring lithium chloride formation. The negative charge is mainly concentrated on Cl (-0.07 e), weakening S polarization and stabilizing the Li-Cl transition state. Under these conditions, the synergistic polarization between multiple carbonyl and hydroxyl groups generates a coverage-induced collective polarization, forming a continuous electron density channel along the Li-Cl axis and driving Li... + To Cl - move.

[0029] Under low-coverage AXT, the Li-Cl coordination shell of LPSC is loose and inhomogeneous. The formation of localized electron pockets hinders electron leakage and delays Li-Cl bond formation, as shown in the reference. Figure 2 d. Li+ Attracted to the O / S sites of AXT and deviating from the original Li-S coordination in LPSC, the PS bond becomes polarized and weakened, thus promoting the formation of Li₂S active materials. This weakening of the PS bond can also be observed through Bader charge trend data (where Li₂S is the primary component of the Li₂S active material). + This is confirmed by the correction (+0.21e~+0.27e), the deelectronization of P (-0.35e), and the fact that S in LPSC becomes more negative (-0.11e).

[0030] Reference Figure 2 e and Figure 2 The calculations of f, bond order, and energy barrier further confirm this difference in electrolyte decomposition products dependent on AXT coverage. At low AXT coverage, the PS bond in LPSC weakens sharply in the transition state and almost disappears in the final state, while the enhancement of Li-Cl in lithium chloride only occurs in the final state, consistent with the lower energy barrier during Li₂S formation. However, at high AXT coverage, the Li-Cl bond appears in the transition state and dominates in the final state, while the PS bond maintains a certain strength, leading to a significant reduction in the energy barrier during lithium chloride formation.

[0031] Based on the experiments described in this embodiment, it can be concluded that in AXT with low doping concentrations, PO bonds that inhibit the decomposition of the cathode electrolyte will not form. Instead, a small amount of highly reducing AXT accelerates electrolyte decomposition and alters the decomposition pathway through the electron pocket effect. Electrons are confined in pockets around the AXT and cannot transfer from the PS bond to the Li-Cl bond. Instead, they preferentially interact with O sites, thus polarizing and weakening the PS bond. This is beneficial for the formation of active materials (such as Li₂S) rather than byproducts (such as lithium chloride), thereby increasing battery capacity. When the doping level of insulating AXT reaches a certain level, a significant PO coordination network forms in the cathode, inhibiting the decomposition of the electrolyte into active materials, but generating more insulating lithium chloride byproducts. In this state, intermolecular π-π stacking effects and continuous electron density channels within the AXT appear, stabilizing the Li-Cl transition state from a geometric and electronic perspective, thereby reducing battery capacity.

[0032] Example 3 This embodiment aims to verify the catalytic ability of AXT to catalyze sulfur redox kinetics, specifically including cyclic voltammetry at different scan rates, in-situ and ex-situ electrochemical impedance spectroscopy (EIS), and Li... + Diffusion analysis and theoretical calculations were used to elucidate the catalytic mechanism of sulfur redox reaction (SRR) and to clarify the enhancing effect and underlying principle of AXT on the kinetics of sulfur redox reaction (SRR).

[0033] To evaluate the effect of AXT on the sulfur redox reaction at the cathode, cyclic voltammetry tests at different scan rates were first performed on uncycled cells. The results showed that all cells exhibited a significant reduction peak at approximately 1.35 V and an oxidation peak at approximately 1.75 V, indicating an effective solid-solid conversion reaction between S8 molecules and Li2S at the cathode. Notably, the 0.5% AXT-modified cathode showed a higher current and an earlier redox potential than the original cathode. Furthermore, the cyclic voltammetry results were plotted as contour plots on... Figure 3 The value of 'a' in the figure shows a significant redox overpotential. Among all cathodes, the KB / S-0.5%AXT cathode has the lowest overpotential of 784 mV, compared to 862 mV for the undoped AXT cathode and 821 mV for the 2.5%AXT cathode. Cyclic voltammetry and capacity / differential voltage (dQ / dV) curves both indicate that the addition of a small amount of AXT achieves reduced polarization, improved sulfur utilization, and accelerated sulfur redox reaction. The rapid reaction kinetics and reduced polarization of the 0.5%AXT-modified cathode were further validated by intermittent galvanostatic titration (GITT), where the open-circuit voltage (OCV) at the end of discharge of the KB / S-0.5%AXT cathode was observed to be 1.78 V, lower than that of the KB / S cathode (1.89 V).

[0034] Given that AXT is an inert material with poor electrical and ionic conductivity, this embodiment conducts systematic in-situ and ex-situ EIS and Li... + Diffusion analysis. The Nyquist plots of ASSLSBs exhibit specific electrochemical process limitations; their semi-circular regions sometimes couple, making them difficult to fit with equivalent circuits. Therefore, the relaxation time (DRT) distribution method was used to analyze the EIS results. The analysis results show that the peaks at 0.1–1 seconds and 1–10 seconds correspond to the transport impedance (R0) at the cathode / electrolyte interface, respectively. ct The KB / S-2.5%AXT and KB / S-5%AXT cathodes showed that the large amount of inert material significantly increased the cathode ion diffusion resistance and the interfacial resistance between the cathode and the electrolyte, hindering electron and ion transport and affecting SRR kinetics. Conversely, for ASSLSB modified with 0.5%AXT, the addition of trace amounts of inert additives caused only a small increase in interfacial resistance and cathode ion diffusion resistance, indicating that 0.5%AXT had little effect on the electronic and ionic conductivity of the system.

[0035] Furthermore, this embodiment also performed in-situ EIS and related DRT analyses of ASSLSBs throughout the discharge process, and demonstrated that... Figure 3 b in the text. Throughout the discharge process, R... ctBoth Rct and W exhibit a gradual decay across all cells, followed by a slight increase, due to the conversion from S8 to Li2S2 and ultimately to Li2S (conductivity: S8 > Li2S > Li2S2). Careful analysis revealed that 0.5% AXT-modified ASSLSBs exhibited relatively smaller Rct and W compared to 2.5% and 0% AXT-based cells. This voltage-dependent resistive behavior suggests that introducing excessive AXT significantly increases the surface energy barrier of the cathode, thereby hindering SRR kinetics by suppressing charge / ion transfer; moderate amounts of AXT not only have a negligible effect on interfacial impedance but also promote ion transport in the electrolyte and catalyze the sulfur conversion reaction to accelerate the SRR reaction. This unaffected interfacial ionic conductivity of 0.5% AXT can also be observed through Li... + The diffusion coefficient was confirmed. Calculated using cyclic voltammetry, the Li in the composite cathode can be qualitatively evaluated by comparing the slope of the peak current with the square root of the scan rate. + Diffusion coefficient, KB / s-0.5% AXT cathode exhibits Li + The diffusion coefficient is slightly faster than that of the KB / S cathode and much greater than that of the KB / S-2.5%AXT cathode.

[0036] To further elucidate the SRR mechanism on the AXT catalyst, this embodiment employs theoretical calculations. From a thermodynamic perspective, calculations were performed... , and In pristine graphene (Gh) and Gh-AXT (“ " represents the adsorption energy (E) on the adsorbed state" ads ), and subsequently built → → The relative free energy curves of the pathways. The results show that the interaction between Gh-AXT and these three substances is significantly stronger ( , and E ads The values ​​were -0.63, -3.34, and -2.71 eV, respectively, while the interaction with Gh was weaker (E...). ads (respectively -0.25, -1.61, and -1.70 eV), especially in stable conditions. It performs exceptionally well in intermediates. Figure 3 The corresponding free energy diagram shown in c further indicates that, Converted to Gh-AXT The reaction exothermic energy is 0.76 eV more (1.62 eV for Gh-AXT and 0.86 eV for Gh), while Converted to Gh-AXT The reaction also produces a more favorable final state (-1.24 eV for Gh-AXT and -0.21 eV for Gh).

[0037] Meanwhile, the Li climbing image elastic band (CI-NEB) method under fixed lattice parameters was used to evaluate the Li + Migration energy barriers at the Gh and Gh-AXT interfaces. At the Gh interface, Li... + Migration occurs from a hexagonal vacancy to an adjacent vacancy via a bridging site; while in the Gh-AXT system, Li + Migration along the channel defined by the O site of AXT (from -OH to C=O). For example... Figure 3 As shown in d, Li + The minimum migration barrier on the Gh-AXT surface (0.17 eV) is 0.11 eV lower than that on the Gh surface (0.28 eV), which is equivalent to an increase of about 70 times in the theoretical migration rate at 300 K, indicating that Li + Migration is easier on the Gh-AXT surface.

[0038] Regarding electronic interactions, the partial density of states (PDOS) shows that, in the range of -4 eV to 0 eV, the O-2p states of AXT interact with anchored Li2S. x Enhanced orbital hybridization exists between the Li-2s / S-3p states (x=1, 2). This hybridization indicates electronic coupling between the AXT oxygen atom and the interfacial Li center, leading to charge delocalization from the Li-S bond to the Li-O bond. This charge redistribution weakens the Li-S covalent bond and promotes the subsequent transformation of Li₂S₂ to L₂S. Differential charge density plots further reveal the directional accumulation of Li-O charge and the Li₂S… x (x=1,2) Interfacial charge transfer between the carbonyl / hydroxyl O atoms of AXT at the Gh-AXT interface and the species, while the original Gh mainly exhibits charge polarization. Figure 3 The electrostatic potential (ESP) diagram shown in Figure e indicates that there are continuous negative electrostatic potential regions ("negative potential pockets") and low potential corridors around the C=O and –OH functional groups in the Gh-AXT system, which provide stronger adsorption for the Li2S2 intermediate and thus effectively accelerate the reaction process.

[0039] Based on the experiments described in this embodiment, it can be concluded that AXT can be achieved by constructing a low-energy interface reaction pathway and Li + Migration channels, and with the aid of polar Li-O coordination to stabilize the Li2S2 intermediate, achieve the SRR reaction and Li + A dual improvement in solid-solid interface transmission efficiency.

[0040] Example 4 This embodiment aims to conduct in-situ detection experiments on the mechanical behavior of AXT-optimized ASSLSBs, specifically including in-situ pressure monitoring, Li anode pressure contribution elimination, and molecular dynamics simulation, to verify the buffering effect of AXT on the volume expansion of sulfur cathodes and the effect of improving mechanical stability.

[0041] As is well known, the large volume expansion of the sulfur cathode is a major factor limiting the performance of Li-S batteries, especially in ASSLSBs. The repeated expansion and contraction of sulfur during (de)lithiation can easily lead to the disconnection of the electrode-SSE interface and the generation of voids and cracks. Under high sulfur loading, changes in stack pressure exacerbate interfacial contact failure. Therefore, this embodiment uses an in-situ electrochemical-pressure device to monitor the stack pressure evolution during the electrochemical process of ASSLSBs. A schematic diagram of the device is shown below. Figure 4 As shown in a, a force sensor with a signal conditioner is installed on the top of the stainless steel casing of the ASSLSB. During charging and discharging, the mechanical changes are converted into electrical signals, and the internal pressure changes are output as real-time feedback.

[0042] Figure 4 b and Figure 4 c in the figure shows the high sulfur loading of 3.6 mg·cm⁻¹. -2 The potential-pressure curves of KB / S-0.5%AXT|LPSC|Li and KB / S|LPSC|Li batteries under 0.05C constant current cycling are shown to change over time. The overall stack voltage decreases during discharge and increases during charging because the volume change caused by the (de)lithiation of the lithium anode is greater than the volume expansion / contraction of the sulfur cathode. Due to the higher sulfur conversion efficiency exhibited by the KB / S-0.5%AXT cathode, the stack voltage of the 0.5%AXT modified ASSLSB decreased by 0.739 MPa during the first discharge, followed by an increase of 0.749 MPa during charging, with a final overall pressure change of only 0.01 MPa. Conversely, the stack voltage of the KB / S|LPSC|Li battery decreased by 0.306 MPa during the first cycle, obtained by subtracting 0.268 MPa from 0.574 MPa. After 5 cycles, the pressure change of the KB / S|LPSC|Li battery was much greater than that of the KB / S-0.5%AXT|LPSC|Li battery. This non-negligible pressure change is not conducive to maintaining tight interfacial contact and increases the risk of electrochemical-mechanical failure.

[0043] To eliminate the contribution of the large volume change ratio of the Li anode to the overall pressure change of ASSLSBs and to more accurately define the mechanical behavior of the KB / S-0.5%AXT cathode, this embodiment uses Li4Ti5O 12 (LTO) is matched with Li metal and operates at 1.5-2.5V (relative to Li / Li). + Within a certain range, thanks to the zero-strain characteristics of LTO, the pressure change of the Li anode can be calibrated independently. Figure 4 The 'd' in the figure shows the potential-pressure change over time in the LTO|LPSC|Li battery, since the charge / discharge current density is constant at 0.3 mA·cm. -2 There is a linear relationship between the pressure and capacity of Li metal, and the pressure change rate of Li metal during lithiation / delithiation is fitted to be 0.262 kg·h. -1 By from Figure 4 Subtracting the contribution of the Li anode from the initial pressure curve shown in b, we obtain... Figure 4 The net pressure change of 'e' over time is shown in the figure. During discharge, the increase in stack pressure originates from the volume expansion of sulfur into Li₂S, while the decrease in stack pressure during charging represents the reversible transformation of Li₂S into sulfur and volume contraction. A comparison of stack pressure evolution among different batteries shows that the KB / S-0.5%AXT battery exhibits smaller pressure changes and a lower pressure drop rate than the KB / S battery, verifying the crucial role of AXT in mitigating volume changes and electrical contact failures caused by stress and strain during cycling.

[0044] To further elucidate the buffering mechanism of AXT on interlayer volume expansion, Forcite molecular dynamics simulations were performed in this embodiment. Different amounts of Li were gradually inserted between two Gh layers. + At the same time, the in-plane lattice constant is kept constant, referring to Figure 4 In the figure, f is taken as the baseline for relative expansion in the unlithiated state. Due to the intermolecular distance effect, Gh-AXT in the absence of Li + It exhibits a larger initial interlayer volume than Gh. However, with Li + With increasing content, the interlayer expansion process of Gh-AXT becomes slower, and its relative expansion rate remains lower than that of Gh. Figure 4 g in the text.

[0045] Based on the experiments described in this embodiment, it can be concluded that AXT can interact with Li through oxygen-containing functional groups (-OH and C=O). + The coordination effect, combined with the flexible molecular scaffold effect, redistributes out-of-plane strain, alleviates local stress concentration, effectively suppresses interlayer breathing, reduces the pressure fluctuation caused by the volume expansion of the sulfur cathode, maintains close interfacial contact between the electrode and the electrolyte, and improves the mechanical stability of ASSLSBs.

[0046] Example 5 This embodiment aims to conduct a comprehensive evaluation test of the electrochemical performance of AXT-modified ASSLSBs, specifically including rate performance testing, long-cycle performance testing, high sulfur loading and wide temperature range performance testing, so as to fully verify the effect of AXT modification on improving the electrochemical performance of ASSLSBs.

[0047] In this embodiment, KB / Sx%AXT (x=0, 0.5, 2.5, 5) is selected as the positive electrode, Li metal as the negative electrode, and LPSC as the electrolyte. The experiment was conducted at room temperature (30°C) and 1.5~3V (relative to Li / Li). + Electrochemical performance evaluation was conducted within the voltage range.

[0048] Figure 5 Figure 'a' shows the rate performance of four cathodes across current densities ranging from 0.1C to 1C. The cathode based on 0.5% AXT exhibits the best discharge specific capacity as the current density increases from 0.1C to 0.75C, with average values ​​of 1685.5, 1622.1, 1525.5, 1370.3, and 1114.9 mAh·g⁻¹, respectively. -1 Even with the current density increased to 1C, the KB / S-0.5% AXT cathode still maintains 839.4 mAh·g. -1 The high capacity of the positive electrode is compared to that of the other positive electrodes, which have significantly lower capacities (<352.2 mAh·g). -1 This indicates that the 0.5% AXT-modified cathode exhibits high rate performance due to the increased active material generated from SSE decomposition and the strong SRR catalytic performance of AXT. Notably, the charge / discharge rate was suddenly restored to 0.1C at the 31st cycle, and the discharge capacity recovered to 1605.1 mAh·g. -1 This represents 96.7% of the initial capacity during the first cycle, demonstrating that the battery with the KB / S-0.5% AXT cathode exhibits excellent electrochemical reversibility and sustained interfacial dynamic stability. Figure 5 The constant current charge-discharge curve shown in b further validates the maximum capacity of the KB / S-0.5%AXT cathode, and this cathode has less electrochemical polarization at 0.5C, which is attributed to the acceleration of the sulfur redox reaction and the close contact of the cathode / electrolyte interface. In contrast, the higher polarization of other AXT cathode ratios hinders charge and ion transport, leading to rapid capacity decline and electrochemical-mechanical failure.

[0049] Long-cycle performance tests were conducted on four types of cathodes at 30℃ and a charge / discharge rate of 0.5C. The results are as follows: Figure 5 As shown in c, the cathode containing 0.5% AXT exhibited an extremely high reversible capacity of 1431.7 mAh·g during the first discharge. -1 After 300 cycles, it decreased to 789.3 mAh·g. -1 (Equivalent to a decay rate of 0.15% per cycle). In contrast, the other three control samples exhibited lower capacities at the first cycle (KB / s, KB / s-2.5%AXT, and KB / s-5%AXT were 1403.2, 1220, and 974.4 mAh·g, respectively). -1And significant capacity decay occurred after 200 cycles (the capacities at KB / s, KB / s-2.5%AXT, and KB / s-5%AXT at 200 cycles were 547.6, 450.8, and 315.9 mAh·g, respectively). -1 This is because, in the absence of adequate AXT, electrolyte decomposition tends to generate inert LiCl, which passivates the three-phase interface and hinders charge transfer. Considering the side reaction effects of the Li anode and LPSC, a Li-In anode was used instead of Li metal for testing. Figure 5 The d-value shows that the assembled KB / S-0.5% AXT|LPSC|Li-In battery exhibits a capacity of 1625.1 mAh·g at 0.2C. -1 Its high initial capacity, decay rate of 0.082% per cycle, and coulombic efficiency of 99.95% after 300 cycles demonstrate its excellent cycling stability.

[0050] To verify practical feasibility, ASSLSBs with different anodes were constructed and tested over a wide temperature range with high sulfur content. For example... Figure 5 As shown in 'e', ​​the sulfur loading is 6.45 mg·cm³. -2 The 0.5% AXT modified battery has an initial capacity of 1468.3 mAh·g at 30℃ and 0.1C. -1 (Corresponding area capacity 9.35mAh·cm²) -2 After 100 cycles, the capacity retention rate was 84.9%; the sulfur loading increased to 8.63 mg·cm³. -2 After two activations at 0.05C, the initial capacity reached 1166.76 mAh·g. -1 After 100 cycles, the capacity is 920.42 mAh·g. -1 The attenuation rate was 0.22%. At 60℃ and a sulfur loading of 9.49 mg·cm⁻¹, the attenuation rate was... -2 Under certain conditions, such as Figure 5 As shown in f, the initial reversible capacity of the battery is 1300.95 mAh·g. -1 (Corresponding area capacity 16.56mAh·cm²) -2 It boasts a coulombic efficiency of 99.68% and its capacity increases progressively with cycling; even at a low temperature of -10℃, the battery still delivers 1191.31 mAh·g. -1 The discharge capacity remains stable for 50 cycles without any degradation.

[0051] Combination Figure 5The comparative analysis shown in g indicates that ASSLSBs doped with 0.5% AXT achieve record-breaking specific capacity and industry-competitive sulfur loading capacity through the triple effects of electrolyte decomposition regulation, SRR catalysis, and volume expansion suppression. Based on the experiments in this embodiment, it can be concluded that 0.5% AXT is the optimal doping ratio, enabling ASSLSBs to possess high rate performance, long cycle stability, high sulfur loading adaptability, and wide temperature tolerance, providing a reliable solution for the industrialization of high-energy-density ASSLSBs.

[0052] AXT-modified ASSLSBs exhibit excellent overall electrochemical performance: an initial discharge specific capacity of 1685.5 mAh·g at 0.1C rate. -1 Furthermore, the sulfur utilization rate exceeds 100%, and it still retains 839.4 mAh·g at a 1C rate. -1 Volume; 1.46 mg·cm³ -2 Under sulfur loading, after 300 cycles at 0.2C, the coulombic efficiency was 99.95% and the decay rate was only 0.082%; 6.45 mg·cm⁻¹ -2 Under high sulfur loading, the areal capacity after 100 cycles is 9.35 mAh·cm³. -2 It has a capacity retention rate of 84.9% and can operate stably in a wide temperature range of -10 to 60℃. At 60℃, the concentration is 9.49 mg / cm³. -2 The initial areal capacity under sulfur loading reaches 16.56 mAh·cm³. -2 .

[0053] In summary, an AXT / C / S cathode composite material was successfully synthesized via a simple high-energy ball milling method, achieving efficient control of the three-phase interface of an all-solid-state lithium-sulfur battery. AXT can directionally control the electrolyte decomposition pathway through the electron pocket effect, promoting the formation of Li₂S active material instead of inert LiCl byproducts; its oxygen-containing functional groups construct low-potential channels that can accelerate Li₂S decomposition. + It migrates and catalyzes sulfur oxidation-reduction reactions; at the same time, the flexible support effect of the chain structure can alleviate the volume expansion of the sulfur cathode and maintain the stability of the interface contact.

[0054] The various embodiments in this specification are described in a progressive manner, with each embodiment focusing on the differences from other embodiments. The same or similar parts between the various embodiments can be referred to each other.

[0055] This document uses specific examples to illustrate the principles and implementation methods of the present invention. The descriptions of the above embodiments are only for the purpose of helping to understand the method and core ideas of the present invention. Furthermore, those skilled in the art will recognize that, based on the ideas of the present invention, there will be changes in the specific implementation methods and application scope. Therefore, the content of this specification should not be construed as a limitation of the present invention.

Claims

1. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries, characterized in that, The astaxanthin dynamically regulates a three-phase interface of the all-solid-state lithium-sulfur battery through an electron pocket effect as an electronic switch, the three-phase interface being an interface between a sulfur active material, a conductive carbon material, and a sulfide solid-state electrolyte; and the regulation of the three-phase interface includes one or more of the following: regulating a decomposition path of the sulfide solid-state electrolyte to facilitate the generation of a Li2S active material; Constructing low-potential channels to facilitate Li + transport and catalyze sulfur redox reactions; The astaxanthin relieves the volume expansion of the sulfur cathode as a flexible molecular scaffold and maintains the stability of the interface contact.

2. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 1, characterized in that, The astaxanthin is added in the form of an additive to a cathode composite material of the all-solid-state lithium-sulfur battery, and the mass ratio of the astaxanthin in the cathode composite material is 0.5-10wt%.

3. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 2, characterized in that, The mass ratio of the astaxanthin in the cathode composite material is 0.5wt%.

4. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 1, characterized in that, The regulation of the decomposition path of the sulfide solid-state electrolyte is specifically as follows: the astaxanthin limits the migration of electrons through the electron pocket effect, causes the electrons to preferentially react with the oxygen sites of the astaxanthin, polarizes and weakens the P-S bond in the sulfide solid-state electrolyte, inhibits the formation of a Li-Cl bond, and further facilitates the decomposition of the sulfide solid-state electrolyte to generate a Li2S active material.

5. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 4, characterized in that, The full-solid-state lithium-sulfur battery regulated by astaxanthin at the three-phase interface has a sulfur loading of 1.46mg·cm -2 After 300 cycles at a 0.2C rate, the coulombic efficiency is not less than 99.95%, the cycle attenuation rate is not more than 0.082%, and the initial discharge specific capacity is not less than 1629.1mAh·g -1 .

6. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 4, characterized in that, The full-solid-state lithium-sulfur battery regulated by astaxanthin at the three-phase interface has an area capacity of 9.35 mAh·cm -2 -2 after 100 cycles when the sulfur loading is 6.45 mg·cm -2 , the capacity attenuation rate is 0.151%, and the capacity retention rate is 84.9%.

7. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 1, characterized in that, The construction of low potential channel is specifically: the hydroxyl and carbonyl functional groups of astaxanthin form a low potential region, which is Li + The migration provides a channel, and Li + The migration energy barrier is reduced to 0.17eV.

8. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 7, characterized in that, The all-solid-state lithium-sulfur battery regulated by astaxanthin at the three-phase interface has a sulfur loading of 8.63 mg·cm -2 When the capacity retention rate is 78.8% after 100 cycles, and the initial area capacity is 10.01 mAh·cm -2 .

9. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 1, characterized in that, The full-solid-state lithium-sulfur battery regulated by astaxanthin at the three-phase interface can stably operate in a wide temperature range of-10℃-60℃, and still maintains a discharge capacity of 1191.31mAh·g -1 at-10℃ low temperature environment.

10. Use of astaxanthin as an electronic switch in the regulation of the triple phase boundary in all-solid-state lithium-sulfur batteries according to claim 1, characterized in that, The full-solid-state lithium-sulfur battery regulated by astaxanthin at the three-phase interface has an initial discharge specific capacity of not less than 1685.5 mAh·g at 0.1C rate -1 , the sulfur utilization rate is greater than 100%, and the discharge capacity is not less than 839.4 mAh·g at 1C rate -1 , and the capacity recovery rate is 96.7% when restored to 0.1C rate.