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1.
    
Lithium metal (LM) is a promising anode material for next generation lithium ion based electrochemical energy storage devices. Critical issues of unstable solid electrolyte interphases (SEIs) and dendrite growth however still impede its practical applications. Herein, a composite gel polymer electrolyte (GPE), formed through in situ polymerization of pentaerythritol tetraacrylate with fumed silica fillers, is developed to achieve high performance lithium metal batteries (LMBs). As evidenced theoretically and experimentally, the presence of SiO2 not only accelerates Li+ transport but also regulates Li+ solvation sheath structures, thus facilitating fast kinetics and formation of stable LiF-rich interphase and achieving uniform Li depositions to suppress Li dendrite growth. The composite GPE-based Li||Cu half-cells and Li||Li symmetrical cells display high Coulombic efficiency (CE) of 90.3% after 450 cycles and maintain stability over 960 h at 3 mA cm−2 and 3 mAh cm−2, respectively. In addition, Li||LiFePO4 full-cells with a LM anode of limited Li supply of 4 mAh cm−2 achieve capacity retention of 68.5% after 700 cycles at 0.5 C (1 C = 170 mA g−1). Especially, when further applied in anode-free LMBs, the carbon cloth||LiFePO4 full-cell exhibits excellent cycling stability with an average CE of 99.94% and capacity retention of 90.3% at the 160th cycle at 0.5 C.  相似文献   

2.
    
Lithium phosphorous oxynitride (LiPON) as one of the most successful solid-state electrolytes (SSEs), has attracted great interest both in academia and technology due to its exceptional interfacial compatibility, broad electrochemical stability window, and excellent thermal stability, which enables the realization of extremely stable electrolyte/electrode interphase toward high-energy density solid-state lithium-metal batteries (SSLMBs). However, insufficiency in ionic diffusion, mechanical robustness, and interfacial stability hinder its commercialization process. Herein, the characteristics of amorphous structure LiPON, fundamental understanding on the bulk ionic diffusion and electrode/electrolyte interface are systematically discussed, and the improvement strategies to boost the electrochemical performance are highlighted. Then, innovative characterization and computational methods help to unravel the design principle of LiPON are summarized. Furthermore, the approaches to realize high-efficient preparation of LiPON are analyzed, followed by the investigation of present application of LiPON in current batteries. Finally, remaining challenges associated with the fundamental understanding and rational prediction of structure and interface design, high efficient preparation, and potential opportunities for future application of LiPON are properly prospected.  相似文献   

3.
    
Composite polymer electrolytes demonstrate the predictable potential for achieving high-performance all-solid-state sodium metal batteries (ASSMBs). However, the insufficient ionic conductivity resulting from the sluggish Na+ transport kinetics and the inferior interfacial stability caused by simultaneous Na+ and anion transport have hindered practical applications. Herein, a rational structural design strategy is proposed to construct an anion-trapping boron-contained covalent organic framework (B-COF) network in the polymer matrix to facilitate selective Na+ migration and interfacial compatibility for ASSMBs. The abundant Lewis-acid sites on the B-COF network can promote the dissociation of sodium salt and simultaneously constrain the migration of TFSI− anions through the strong anion-capturing effect. Moreover, the well-defined ion-conducting channel formed by the in situ generation of intimately packed B-COF combined with the above synergistic effects can afford continuous and accessible pathways for selectively rapid Na+ transport, which significantly elevates the ionic conductivity and Na+ transference number, respectively. Surprisingly, the Na plating/stripping with small polarization is retained under 0.1 mA cm−2 for more than 365 d (>8800 h), representing a record-high cycling stability for ASSMBs. As proof of applied studies, the ASSMBs exhibit a high capacity retention (≈81.2%) after 1200 cycles at 1 C, signifying promising application in all-solid-state electrochemical energy storage systems.  相似文献   

4.
    
Sodium metal batteries are promising for cost-effective energy storage, however, the sluggish ion transport in electrolytes and detrimental sodium-dendrite growth stall their practical applications. Herein, a cross-linking quasi-solid electrolyte with a high ionic conductivity of 1.4 mS cm−1 at 25 °C is developed by in-situ polymerizing poly (ethylene glycol) diacrylate-based monomer. Benefiting from the refined solvation structure of Na+ with a much lower desolvation barrier, random Na+ diffusion on the Na surface is restrained, so that the Na dendrite formation is suppressed. Consequently, symmetrical Na||Na cells employing the electrolyte can be cycled >2000 h at 0.1 mA cm−2. Na3V2(PO4)3||Na batteries reveal a high discharge specific capacity of 66.1 mAh g−1 at 15 C and demonstrate stable cycling over 1000 cycles with a capacity retention of 83% at a fast rate of 5 C.  相似文献   

5.
    
The key hurdle to the practical application of polymeric electrolytes in high-energy-density solid lithium-metal batteries is the sluggish Li+ mobility and inferior electrode/electrolyte interfacial stability. Herein, a dynamic supramolecular polymer electrolyte (SH-SPE) with loosely coordinating structure is synthesized based on poly(hexafluoroisopropyl methacrylate-co-N-methylmethacrylamide) (PHFNMA) and single-ion lithiated polyvinyl formal. The weak anti-cooperative H-bonds between the two polymers endow SH-SPE with a self-healing ability and improved toughness. Meanwhile, the good flexibility and widened energy gap of PHFNMA enable SH-SPE with efficient ion transport and superior interfacial stability in high-voltage battery systems. As a result, the as-prepared SH-SPE exhibits an ionic conductivity of 2.30 × 10−4 S cm−1, lithium-ion transference number of 0.74, electrochemical stability window beyond 4.8 V, and tensile strength up to 11.9 MPa as well as excellent adaptability with volume change of the electrodes. In addition, no major electrolyte decomposition inside batteries made from SH-SPE and LiNi0.8Mn0.1Co0.1O2 cathode can be observed in the in situ differential electrochemical mass spectrometry test. This study provides a new methodology for the macromolecular design of polymer electrolytes to address the interfacial issues in high-voltage solid batteries.  相似文献   

6.
    
In this work, a structurable gel‐polymer electrolyte (SGPE) with a controllable pore structure that is not destroyed after immersion in an electrolyte is produced via a simple nonsolvent induced phase separation (NIPS) method. This study investigates how the regulation of the nonsolvent content affects the evolving nanomorphology of the composite separators and overcomes the drawbacks of conventional separators, such as glass fiber (GF), which has been widely used in sodium ion batteries (SIBs), through the regulation of pore size and gel‐polymer position. The interfacial resistance is reduced through selective positioning of a poly(vinylidene fluoride‐co‐hexa fluoropropylene) (PVdF‐HFP) gel‐polymer with the aid of NIPS, which in turn enhances the compatibility between the electrolyte and electrode. In addition, the highly porous morphology of the GF/SGPE obtained via NIPS allows for the absorption of more liquid electrolyte. Thus, a greatly improved cell performance of the SIBs is observed when a tailored SGPE is incorporated into the GF separator through charge/discharge testing compared with the performance observed with pristine GF and conventional GF coated with PVdF‐HFP gel‐polymer.  相似文献   

7.
    
All-solid-state lithium batteries (ASSBs) have the potential to trigger a battery revolution for electric vehicles due to their advantages in safety and energy density. Screening of various possible solid electrolytes for ASSBs has revealed that garnet electrolytes are promising due to their high ionic conductivity and superior (electro)chemical stabilities. However, a major challenge of garnet electrolytes is poor contact with Li-metal anodes, resulting in an extremely large interfacial impedance and severe Li dendrite propagation. Herein, an innovative surface tension modification method is proposed to create an intimate Li | garnet interface by tuning molten Li with a trace amount of Si3N4 (1 wt%). The resultant Li-Si-N melt can not only convert the Li | garnet interface from point-to-point contact to consecutive face-to-face contact but also homogenize the electric-field distribution during the Li stripping/depositing process, thereby significantly decreasing its interfacial impedance (1 Ω cm2 at 25 °C) and improving its cycle stability (1000 h at 0.4 mA cm−2) and critical current density (1.8 mA cm−2). Specifically, the all-solid-state full cell paired with a LiFePO4 cathode delivered a high capacity of 145 mAh g−1 at 2 C and maintained 97% of the initial capacity after 100 cycles at 1 C.  相似文献   

8.
    
Promoting the interfacial Li+ transport and suppressing detrimental lithium dendrites are the main challenges for developing practical solid-state lithium metal batteries. In this respect, interface rationalizing to synergize the enhancement of ion transport and suppression of lithium dendrites is of paramount significance. Herein, a novel strategy is demonstrated to address those issues by a designed multifunctional composite interlayer. The photocrosslinkable polymer is introduced in a scalable elastic skeleton, which promotes the migration and diffusion of Li+. Moreover, adding perfluoropolyether in the interlayer benefits to regulating the formation of LiF-rich interface, sufficiently suppress the growth of lithium dendrites. Benefitting from the elasticity, high Li+ conductivity and the lithium dendrites suppression capability, the interlayer can significantly improve the interfacial performance of the solid electrolyte/lithium interface, thus leading to the greatly enhanced electrochemical performance of solid-state lithium metal batteries. A high critical current density of 3.6 mA cm−2 and a long cycling life at 1.0 mA cm−2 for >400 h are achieved for the symmetric cells. Besides, when used in a pouch-type full cell coupled with LiNi0.6Co0.2Mn0.2O2 cathode, a high charged capacity of 3.25 mAh cm−2 can be maintained through 20 cycles, demonstrating its great potentials for practical application.  相似文献   

9.
由于干态聚合物电解质目前还不能满足聚合物锂离子电池的应用要求,人们致力于开发含液体增塑剂的聚合物电解质,包括凝胶型和微孔型两类体系。本文综述了含液聚合物电解质的最新进展,重点论述了各种新体系和新方法。  相似文献   

10.
    
Sodium metal batteries (SMBs) are promising for large scale energy storage due to the remarkable capacity of sodium metal anode (SMA) and the natural abundance of Na-containing resources. However, multiple challenges exist with regards to the usage of SMBs, including dendritic Na growth, poor cyclability of SMA, and severe safety hazards stemming from the employment of the highly flammable liquid electrolytes. Herein, by introducing two functional fluorinated solvents, 1,1,2,2-tetra-fluoroethyl 2,2,3,3-tetrafluoropropyl ether (HFE) and fluoroethylene carbonate (FEC) into trimethyl phosphate (TMP)-based electrolyte, a SMA-compatible flame-retardant electrolyte is enabled, in which Na/Na symmetrical cells can cycle for 800 h at 1.0 mA cm−2 or 3.0 mAh cm−2. Specifically, the non-solvating HFE plays a critical role in increasing the local electrolyte concentration and reducing the unfavorable decomposition of TMP molecules. By introducing FEC as the co-solvent simultaneously, its preferential defluorination induces a fluoride-rich solid-electrolyte interphase that prevents Na metal surface against the continuous parasitic reactions. More importantly, the designed electrolyte is endowed with an intrinsic non-flammability, which manifests a prerequisite for the real-life application of SMBs.  相似文献   

11.
    
Rechargeable Li-metal batteries (RLBs) can boost energy yet possess poor cycle stability and safety concerns when utilizing carbonate electrolytes. Countless effort has been invested in researching and developing electrolytes for RLBs to obtain stable and safe batteries. However, only few existing electrolytes meet the requirements for practical RLBs. In this perspective, the challenges of organic liquid electrolytes in the application in RLBs are summarized, and requirements for electrolytes for practical RLBs are proposed. This perspective briefly reviews the recent achievements of electrolytes (liquid- and solid-state) for RLBs and analyzes the corresponding drawbacks of each electrolyte. Further, possible solutions to the existing shortcomings of various electrolytes are proposed. In particular, this perspective outlines the development strategy of in situ gelation electrolytes, accompanied by a call for people using pouch cells to evaluate performance and paying more attention to battery safety research. This perspective aims to expound on the challenges and the possible research directions of RLBs electrolytes to promote practical RLBs better.  相似文献   

12.
    
Aqueous Zn-ion batteries are promising and safe energy storage technologies. However, current aqueous electrolyte Zn-ion battery technology is hindered by undesirable reactions between the electrolyte and electrodes, which can lead to Zn dendrite growth, gas evolution, and cathode degradation. In this study, a hydrated gel electrolyte (HGE) that combines adiponitrile (ADN) and Zn(ClO4)2·6H2O in a polymeric framework is created. ADN is found to stabilize the interface between the electrolyte and anode/cathode, enabling smooth Zn stripping/plating and reducing parasitic reactions. The HGE is simple to fabricate, inexpensive, safe, and flexible. Zn/HGE/Zn symmetrical cells can cycle more than 1000 h at 0.5 mA cm−2 and 2000 h at 0.2 mA cm−2 without short-circuiting, indicating effective suppression of Zn dendrites. Moreover, with a NASICON-type Sr-doped Na3V2(PO4)3 (SNVP) cathode, a Zn/HGE/SNVP full cell can be cycled over 8000 times at 10 C while retaining a high capacity of 90 mAh g−1.  相似文献   

13.
    
Scientific and technological interest in solid‐state Li metal batteries (SSLMBs) arises from their excellent safety and promising high energy density. However, the practical application of SSLMBs is hindered by poor contact between the Li metal anode (LMA) and solid‐state electrolytes (SSEs). To circumvent this limitation, a pattern‐guided approach that shapes the LMA/SSE contact is disclosed to offer fast Li ion conduction in the interface. A thermally‐treated copper foam is used as the lithophilic pattern to confine and guide Li for forming a tight contact with garnet‐type SSE. The contact can be easily manipulated according to the shape of lithiophilic pattern, facilitating cell assembly. The resulting Li|patterned garnet|Li symmetric cell exhibits an interfacial resistance of 9.8 Ω cm2, which is dramatically lower than that of 998 Ω cm2 for Li|pristine garnet|Li symmetric cell. Being used in Li–sulfur batteries, the patterned garnet effectively eliminates the polysulfide shuttle and enables stable cycling performance, showing a low capacity decay of 0.035% per cycle over 1000 cycles. The fundamental contact process of metallic anodes/SSEs is carefully investigated. This contact strategy provides a new design concept to improve the interface wettability via a lithiophilic pattern for a variety of SSEs that cannot wet with metallic anodes.  相似文献   

14.
    
Lithium batteries (LBs) are developed tremendously owing to their excellent energy density as well as cyclic persistence, exhibiting promising applications from portable devices to e-transportation and grid fields. However, with the ever-increasing demand for intelligent wearable electronics, more requests are focused on high safety, good durability, and satisfied reliability of LBs. The self-healing route, which can simulate the ability of organic organisms to repair damage and recover initial function through its intrinsic vitality, is believed to be an efficient strategy to alleviate the unavoidable physical or chemical fatigue and damage issues of LBs, beneficial for the realization of the above mentioned high requests. In this review, the applicability and development of self-healing materials are summarized in electrodes, electrolytes, and interfacial layers in recent years, focusing on exploring the feasibility of different self-healing strategies in LBs, discussing the advantages and disadvantages of existing strategies in different parts of batteries, and indicating the possible research directions for beginners who are interested in this field. Finally, the critical challenges and the future research directions as well as opportunities are prospected.  相似文献   

15.
    
Li metal batteries (LMBs) are considered as promising candidates for future rechargeable batteries with high energy density. However, Li metal anode (LMA) is extensively sensitive to general liquid electrolytes, leading to unstable interphase and dendrites growth. Herein, a novel gel polymer electrolyte consisting of a micro-nanostructured poly(vinylidene fluoride-co-hexafluoropropylene) matrix and inorganic fillers of Zeolite Socony Mobil-5 (ZSM-5) and SiO2 nanoparticles, is fabricated to expedite Li+ ions transport and suppress Li dendrite growth. Due to the Lewis acid interaction, SiO2 can absorb amounts of PF6− and promote the dissociation of LiPF6. The specific sub-nanometer pore structure of ZSM-5 greatly enhances the Li+ ion transference number. These structures can restrain the decomposition of electrolytes and build stable interphase on LMA. Therefore, the Li||Ni0.8Co0.1Mn0.1O2 full cell maintains 92% capacity retention after 300 cycles at 1 C (1 C ≈190 mAh g−1) in carbonate electrolyte. This multiscale design provides an effective strategy for electrolyte exploration in high-performance LMBs.  相似文献   

16.
    
The practical implementation of garnet-type solid electrolytes, such as Li6.4La3Zr1.4Ta0.6O12 (LLZTO), faces the significant challenge of Li dendrites. Though artificial interfacial strategies are effective in dendrite suppression, further investigation is needed to understand the mechanism of homogeneous Li deposition and its practicability under real-world conditions. Herein, a bilayer interface is constructed to address these issues. Such a bilayer interface consists of one conformal Li2O-rich layer, generated by rubbing LLZTO pellets inside molten Li with low-dose In2O3, and another Li2O layer deposited through atomic layer deposition (ALD). The regulatory effect of the initial Li2O-rich layer on achieving uniform Li deposition is explored, and the critical current density is enhanced to 2.4 mA cm−2. However, simple interfacial strategy is insufficient to prevent anodic degradation for cycling at room temperature without stack pressure, leading to increased current leakage and directly reducing Li+ within the electrolyte. After insulating it with a second ALD-Li2O layer that minimally hampers ionic conduction, the Li/Li symmetric cells achieve long cycling life exceeding 1000 h at 0.5 mA cm−2 and maintain stable operation even at 2 mA cm−2. This work provides valuable insights for interfacial strategies towards practical solid-state batteries.  相似文献   

17.
    
Polymer gel electrolytes are usually utilized in various energy storage devices due to their advantages of excellent ionic conductivity and outstanding mechanical properties. However, they are often not biodegradable and lose their flexibility and electrochemical performance during the dehydration/hydration process. Herein, sustainable dough-based gel electrolytes with high biosafety and environmental friendliness are developed. In the dough electrolytes, gluten molecules connect with each other through disulfide bonds to construct gluten network and water that contains abundant ions adheres on it to achieve a continuous ion transport pathway. Therefore, the dough electrolytes possess outstanding mechanical properties and excellent ionic conductivities. More impressively, they also exhibit the ability to recover their electrochemical and mechanical performance after dehydration/hydration cycles as well as the self-adhering, degradable, and edible behaviors. As a proof of concept, the dough electrolytes are used in supercapacitors and zinc-ion batteries. The resultant devices display comparable electrochemical performance in comparison with the counterparts with polymer gel electrolytes. Furthermore, the multiple functions of dough electrolytes are also integrated into the supercapacitors and zinc-ion batteries devices. This work provides a promising route to design highly sustainable gel electrolytes for different aqueous energy storage devices.  相似文献   

18.
    
Although batteries fitted with sodium metal anodes and sulfur cathodes are attractive for their higher energy density and lower cost, the threat of polysulfide migration in organic liquid electrolytes, uncontrollable dendrites, and corresponding safety issues has locked the deployment of the battery system. Introduction of solid-state electrolytes to replace conventional liquid-based electrolytes has been considered an effective approach to address these issues and further render solid-state sodium-sulfur battery (SSSSB) systems with higher safety and improved energy density. Nevertheless, the practical applications of SSSSB are still hampered by grand challenges, such as poor interfacial contact, sluggish redox kinetics of sulfur conversion, and Na dendrites. Currently, various strategies have been proposed and utilized to negate the problems within the solid-state battery. Herein, a timely and comprehensive review of emerging strategies to promote the development of SSSSB is presented. The critical challenges that prevent the real application of the SSSSB technique are analyzed initially. Subsequently, various strategies for boosting the development of SSSSB are comprehensively summarized, containing the developing of the advanced cathode and cathode/electrolyte interface, tailoring the solid electrolyte, and designing the stable anode and anode/electrolyte interface. Finally, further perspectives on stimulating the practical application of SSSSB technology are provided.  相似文献   

19.
    
All‐solid‐state lithium metal batteries (ASSLMBs) have attracted significant attention due to their superior safety and high energy density. However, little success has been made in adopting Li metal anodes in sulfide electrolyte (SE)‐based ASSLMBs. The main challenges are the remarkable interfacial reactions and Li dendrite formation between Li metal and SEs. In this work, a solid‐state plastic crystal electrolyte (PCE) is engineered as an interlayer in SE‐based ASSLMBs. It is demonstrated that the PCE interlayer can prevent the interfacial reactions and lithium dendrite formation between SEs and Li metal. As a result, ASSLMBs with LiFePO4 exhibit a high initial capacity of 148 mAh g?1 at 0.1 C and 131 mAh g?1 at 0.5 C (1 C = 170 mA g?1), which remains at 122 mAh g?1 after 120 cycles at 0.5 C. All‐solid‐state Li‐S batteries based on the polyacrylonitrile‐sulfur composite are also demonstrated, showing an initial capacity of 1682 mAh g?1. The second discharge capacity of 890 mAh g?1 keeps at 775 mAh g?1 after 100 cycles. This work provides a new avenue to address the interfacial challenges between Li metal and SEs, enabling the successful adoption of Li metal in SE‐based ASSLMBs with high energy density.  相似文献   

20.
    
Sodium-ion batteries (SIBs) suffer from severe capacity decay as the harmful substances caused by the violent decomposition of electrolyte under high voltages continue to erode the cathodes. Therefore, the design of high-voltage electrolyte and construction of robust cathode–electrolyte interface (CEI) are critical for long-life SIBs. Herein, an electrically coupled composite electrolyte that takes the merits of cross-linked gel polymers and s well-tuned antioxidant additive (4-trifluoromethylphenylboronic acid, TFPBA) is proposed. Through an electrical coupling effect, TFPBA can be anchored by the cross-linked polymer framework to immobilize the PF6− anion and adsorb onto cathode surface spontaneously, both of which promote the formation of a robust CEI layer to facilitate Na+ transportation and suppress subsequent side reactions and corrosive cracking. As a result, the cells integrating high-voltage P2/O3 cathode and well-tailored gel polymer electrolyte achieve stable cycling over 550 cycles within 1.8–4.2 V with a capacity retention of 71.0% and a high-rate discharge capacity of 77.4 mAh g−1 at 5 C. The work paves the way for the development of functionalized quasi-solid electrolyte for practical next generation high-voltage SIBs.  相似文献   

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