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![A schematic showing different models for the growth of lithium dendrite through the solid electrolyte. a Model 1: Continuous root growth mechanism. b Model 2: Sporadic bulk growth mechanism. c Total density of states for the stoichiometric slab of cubic Li7La3Zr2O12, non-stoichiometric slab of cubic Li7La3Zr2O12, non-stoichiometric slab of tetragonal Li7La3Zr2O12, and of LiPON. d Partial density of states from different elements of the stoichiometric surface of cubic Li7La3Zr2O12. Reproduced with permission from [99]](publication/353679536/figure/fig10/AS:1052949908320259@1628054229982/A-schematic-showing-different-models-for-the-growth-of-lithium-dendrite-through-the-solid.png)
A schematic showing different models for the growth of lithium dendrite through the solid electrolyte. a Model 1: Continuous root growth mechanism. b Model 2: Sporadic bulk growth mechanism. c Total density of states for the stoichiometric slab of cubic Li7La3Zr2O12, non-stoichiometric slab of cubic Li7La3Zr2O12, non-stoichiometric slab of tetragonal Li7La3Zr2O12, and of LiPON. d Partial density of states from different elements of the stoichiometric surface of cubic Li7La3Zr2O12. Reproduced with permission from [99]
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All-solid-state battery is considered as the next generation of the energy storage system because of its improved safety and high-energy density compared to the conventional lithium-ion battery. Among different solid-state battery systems that have been studied, the garnet structured solid electrolyte based solid-state battery has attained tremendo...
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Citations
... Polyethylene oxide (PEO) with Li 7 La 3 Zr 2 O 12 (LLZO), as a representative composite polymer electrolyte (CPE) system, has been extensively researched [21][22][23]. In the "ceramic in polymer" type electrolytes, the morphology of the LLZO fillers significantly influences the electrolyte's properties [24,25]. According to the dimension of the LLZO fillers, it can be categorized into 0, 1, 2, and 3 dimensions (0, 1, 2, 3D) [26]. ...
All-solid-state lithium batteries (ASSLBs) are regarded as the most promising alternative to traditional liquid lithium-ion batteries due to their high-energy density and excellent safety. As an important part of ASSLBs, composite polymer electrolytes (CPEs) with excellent comprehensive performance have attracted wide attention from researchers. Herein, a series of CPEs were prepared by employing Li6.4Ga0.2La3Zr2O12 (LGLZO) submicron particles with cubic phase as fillers in polyethylene oxide (PEO) matrix. The tape-casting method was employed to prepare PEO-LiTFSI-x% LGLZO (CPE-x, where x = 0–80). In these CPE-x, the CPE-40 exhibits elevated ionic conductivity (6.20 × 10⁻⁵ S cm⁻¹ at 20 °C and 1.88 × 10⁻⁴ S cm⁻¹ at 60 °C), attractive Li⁺ transference number (0.31 at 60 °C), low activation energy barrier of lithium-ion migration, wide electrochemical window, and high critical current density of 1.3 mA cm⁻². Furthermore, the LiFePO4 | CPE-40 | Li batteries deliver outstanding cycle performance (capacity retention of 85.43% after 225 cycles at 0.2C and 60 °C) and rate performance. These results show that the PEO-base solid-state electrolytes filled with submicron LGLZO particles possess a broad application prospect.
... Solid-state lithium metal batteries (SSLMBs) based on solid-state electrolytes are strong candidates for next-generation technologies due to their potential high safety and high energy density [1][2][3] . SSLMBs transcend the capacity limitations of conventional liquid lithium-ion batteries and answer the transportation industry's requirement for increased power and energy density [4,5] . Therefore, the solid-state electrolyte has received extensive research [6,7] ; highly ionic conductive solid electrolytes (SEs), including sulfide electrolytes and oxide electrolytes, have been developed by numerous researchers [8][9][10][11][12] . ...
Solid-state batteries have garnered attention due to their potentiality for increasing energy density and enhanced safety. One of the most promising solid electrolytes is garnet-type Li7La3Zr2O12 (LLZO) ceramic electrolyte because of its high conductivity and ease of manufacture in ambient air. The complex gas-liquid-solid sintering mechanism makes it difficult to prepare LLZO with excellent performance and high consistency. In this study, an in-situ Li2O-atmosphere assisted solvent-free route is developed for producing the LLZO ceramics. First, the lithium-rich additive Li6Zr2O7 (LiZO) is applied to in-situ supply Li2O atmosphere at grain boundaries, where its decomposition products (Li2ZrO3) build the bridge between the grain boundaries. Second, comparisons were studied between the effects of dry and wet routes on the crystallinity, surface contamination, and particle size of calcined powders and sintered ceramics. Third, by analyzing the grain boundary composition and the evolution of ceramic microstructure, the impacts of dry and wet routes and lithium-rich additive LiZO on the ceramic sintering process were studied in detail to elucidate the sintering behavior and mechanism. Lastly, exemplary Nb-doped LLZO pellets with 2 wt% LiZO additives sintered at 1,300 °C × 1 min deliver Li⁺ conductivities of 8.39 × 10⁻⁴ S cm⁻¹ at 25 °C, relative densities of 96.8%, and ultra-high consistency. It is believed that our route sheds light on preparing high-performance LLZO ceramics for solid-state batteries.
... Several studies have focused on elucidating the lithiophobic nature of LLZ SEs and relevant strategies for doing so [11][12][13][14][15] . Initial efforts have included polishing the LLZ surface to improve Li wetting. ...
The development of solid-state Li-metal batteries has been limited by the Li-metal plating and stripping rates and the tendency for dendrite shorts to form at commercially relevant current densities. To address this, we developed a single-phase mixed ion- and electron-conducting (MIEC) garnet with comparable Li-ion and electronic conductivities. We demonstrate that in a trilayer architecture with a porous MIEC framework supporting a thin, dense, garnet electrolyte, the critical current density can be increased to a previously unheard of 100 mA cm⁻², with no dendrite-shorting. Additionally, we demonstrate that symmetric Li cells can be continuously cycled at a current density of 60 mA cm⁻² with a maximum per-cycle Li plating and stripping capacity of 30 mAh cm⁻², which is 6× the capacity of state-of-the-art cathodes. Moreover, a cumulative Li plating capacity of 18.5 Ah cm⁻² was achieved with the MIEC/electrolyte/MIEC architecture, which if paired with a state-of-the-art cathode areal capacity of 5 mAh cm⁻² would yield a projected 3,700 cycles, significantly surpassing requirements for commercial electric vehicle battery lifetimes.
... Aluminum is one of them (Li 6.28 Al 0.24 La 3 Zr 2 O 12 ), which gives structural stability to the cubic phase at room temperatures with good ionic conductivity [14,16]. However, the practical challenge of creating a perfect contact between a solid electrolyte and the electrode remained unresolved for garnet as well [17][18][19]. In addition, garnet structured solid electrolyte has a lithiophobic nature which intrinsically repels metallic lithium when it comes to contact. ...
... Due to the behavior, the electrode-electrolyte interphase suffers from voids, and the electric field localization eventually leads to dendrite growth through grain boundaries. Thus, achieving a good critical current density needs suitable interphase modifications [17]. Introducing suitable interlayers, alloying lithium, or incorporating appropriate addictive materials were found to be enhancing the contact. ...
... Since lithium has a low melting point, it is easy to create alloys with it or add suitable addictive so that garnet's lithiophobic nature could turn into lithiophilic. Many interlayers, like Au, C, LiNbO 3 , Al, etc., were introduced to the garnet-lithium interphase [17,[20][21][22][23]. However, despite the introduction of a stable interlayer between lithium and the garnet solid electrolyte may have a positive benefit in the beginning to enhance the contact, it has fatal flaws in the long run. ...
Abstract
Garnet-structured solid-state electrolytes are getting considerable attention due to their high figure of merit over other inorganic solid-state electrolytes. The high lithium-ion conductivity and exceptional stability with metallic lithium over a wide voltage window open the door for the practical realization of an all-solid-state battery. However, the lithiophobic nature of garnet solid electrolytes creates huge interface resistance, which restricts achieving high critical current density. Herein a multifunctional composite anode containing lithium metal and lithium titanate (Li4Ti5O12) is introduced to tackle the interface challenges with the garnet solid electrolyte. The partial reduction of titanium in the composite enhances the electronic conductivity of the anode, and the intrinsic structural advantages of lithium titanate are expected to accommodate volume change as well. The prepared symmetric cell with the composite anode is found to have a minimal areal-specific resistance of 27 Ω cm2, while that of the pristine lithium anode is 249 Ω cm2. The cell has also run with a better critical current density (0.35 mA cm−2) than the pristine lithium (0.15 mA cm−2). A full cell study with a lithium iron phosphate cathode offers a capacity of 145 mAh g−1 at 0.2 C and runs for 100 cycles at 1 C with minimum capacity loss.
... In this regard, the lithium-ion battery (LiB) is considered as a preferred power source due to its high energy density and long lifespan [1]. The LiB has been widely used in electric vehicles, portable electronics, and aviation [2,3]. The growing market for electric vehicles has boosted the demand for LiBs, which further exacerbates the information management dilemmas in the LiB supply chain [4]. ...
... Therefore, it is possible to determine whether there is a cross-site scripting attack by monitoring the variation of values. (2) Hackers have little information about the client logic of the Cloud ERP system, so they often use one-by-one tests to find fields that can induce suspicious system operating requests. So the timestamp becomes dense and is chosen as another representative field. ...
... one comparison to determine where the unsafe behavior occurs. Its computational complexity is ( 2) O N ∧ . Assuming that the time complexity of manual screening is N, even if the basic K-means classification algorithm is used, the time complexity of the recursive unsupervised binary classification algorithm is ( ( )) ( ( ( ))) O NLog N O K means N * − , which is far more complicated than in the UBMA model. ...
Cloud enterprise resource planning (Cloud ERP) provides an efficient big data management solution for lithium-ion battery (LiB) enterprises. However, in the open ecological environment, Cloud ERP makes the LiB supply chain face multi-user and multi-subject interactions, which can generate sensitive data and privacy data security issues (such as user override access behavior). In this study, we take the value and information interaction into account to examine the user behaviors of the diverse stakeholders in the LiB supply chain. Therefore, a user behavior monitoring algorithm (UBMA), different from the mainstream supervised algorithms and unsupervised learning algorithms, is proposed to monitor the unsafe behaviors that may threaten data privacy in Cloud ERP. The results show that the UBMA can accurately search out the user behavior sequence where the unsafe behavior is located from a large amount of user behavior information, which reduces the complexity of directly identifying the unsafe behavior. In addition, compared with the recursive unsupervised binary classification method, the UBMA model has a lower resource consumption and higher efficiency. In addition, the UBMA has great flexibility. The UBMA can be further updated and extended by re-establishing the statistical characteristics of the standard user behavior fields to quickly adapt to user changes and function upgrades in the LiB supply chain.
... Lithium-ion batteries (LIBs) have been widely applied due to their long cycle life, high energy density, high working voltage, and environment friendly [1,2]. However, the current commercial LIBs based on liquid electrolyte meet disadvantage such as inflammability and explosion, etc. [3]. Solid-state LIBs (SS-LIBs) assembled with solid-state electrolytes (SSEs) are regarded as the promising candidates of new generation of LIBs [4,5]. ...
... Oxynitride electrolytes always have low conductivity (e.g., LiPON has conductivity in order of 10 -6 S cm -1 ) and that limits them for LIB application for high energy density. While, oxide-based electrolytes containing good conductivity and high electrochemical window are the very promising electrolytes [3,7]. Common oxide-based electrolytes include LISICON (lithium superionic conductor), NASICON (sodium superionic conductor), perovskite-type (Li,La)TiO 3 (LLTO), and garnet-type [e.g., Li 7 La 2 Zr 3 O 12 (LLZO)]. ...
... This leads to the shrinkage of LiO 6 octahedra centered on Li (2), so that the possibility of lithium ions passing through the oxygen octahedron decreases. The same is true for the oxygen octahedron centered on Li (3). Based on preceding studies on the migration path of lithium ions in LZNO, the lithium-ion migration path of LZNO is in the O-T-O direction inside the oxygen polyhedron [14]. ...
Lithium-ion batteries (LIBs) based on solid-state electrolytes have attracted much attention for their high safety and energy density. Li29Zr9Nb3O40 (LZNO), as a new kind of Li-ion conductor, has great potential in applications of solid-state LIBs. In this work, various contents of LiF are selected to modify LZNO Li-ion conductor, and the optimal content of LiF is 5 wt% (weight%). The phase component, crystal structure, ionic conductivity, and electrochemical performance are investigated. The refinement of crystallographic information based on the bond valence site energy theory is induced to reveal the possible lithium-ion migration channel. The results show that modification with LiF enhanced the 3D migration pathways and conductivity of LZNO-based electrolytes. The 5 wt% LiF modified LZNO presents total conductivity of 0.943 × 10⁻⁴ S cm⁻¹ at ambient temperature and has low activation energy of conduction (0.16 eV). The cycle performance of the lithium symmetric cell characterizes the cycle of 140 h.
... Among the various candidates, Li-stuffed garnet-type oxide with the composition of Li 7 La 3 Zr 2 O 12 (LLZO) has been extensively investigated for application to solid-state batteries [4][5][6][7][8][9][10] because of the high ionic conductivity of 10 −4 -10 −3 S cm −1 at room temperature, good thermal stability, and moderate chemical stability in air. Although the dopant elements used to stabilize highly conductive cubic phase and improve ionic conducting properties may affect the electrochemical stability of LLZO against Li metal [11][12][13], LLZO generally exhibits good chemical and electrochemical stability against Li metal compared to other solid electrolyte materials. ...
... The current density at which Li dendrite growth and propagation into a solid electrolyte occurred is commonly called the critical current density (CCD). CCD may be affected by the testing method because the interface condition between Li metal and a solid electrolyte is generally changed by the area-specific capacity and cycling numbers of Li plating/stripping [7,[19][20][21]. In order to directly compare the CCD values reported by other groups, the test conditions must be considered as well. ...
Garnet-type Ta-doped Li7La3Zr2O12 (LLZO) ceramic solid electrolytes with Ga2O3 additive were synthesized using a conventional solid-state reaction process. When the amounts of Ga2O3 additive were below 2 mol %, the sintered sample has a dense structure composed of grains with an average size of 5 to 10 μm, whereas 3 mol % or more Ga2O3 addition causes a significant increase in grain size above several 10 to 100 μm, due to high-temperature sintering with a large amount of liquid Li-Ga-O phase. At room temperature, the highest total (bulk + grain-boundary) ionic conductivity of 1.1 mS cm−1 was obtained in the sample with 5 mol % Ga2O3 addition. However, this sample was shorted by Li dendrite growth into solid electrolyte at a current density below 0.2 mA cm−2 in galvanostatic testing of the symmetric cell with Li metal electrodes. The tolerance for Li dendrite growth is maximized in the sample sintered with 2 mol % Ga2O3 addition, which was shorted at 0.8 mA cm−2 in the symmetric cell. Since the interfacial resistance between Li metal and solid electrolyte was nearly identical among all samples, the difference in tolerance for Li dendrite growth is primarily attributed to the difference in microstructure of sintered samples depending on the amounts of Ga2O3.
... Among them, oxide-type Li 7 La 3 Zr 2 O 12 (LLZO) has relatively high ionic conductivity, wide electrochemical window, and good chemical stability to lithium metal [10,11]. The electrochemical performance of LLZO can be further improved by controlling the crystal structure and lithium content by doping, controlling the microstructure and size in material processing and thin film fabrication, and tuning the LLZO-electrode interface [12,13]. Therefore, LLZO is regarded as a promising candidate material for solid electrolytes [14,15]. ...
Garnet-type Li7La3Zr2O12 (LLZO) is considered as a promising solid electrolyte. However, the synthesis of LLZO often requires a high temperature, which may lead to the evaporation of the lithium and result in a decrease in ionic conductivity. Therefore, it is an important issue how to reduce the synthesis temperature of LLZO and simultaneously increase its ionic conductivity. Herein, we synthesized garnet-type solid electrolytes of Li6.1Ga0.3La3Zr2O12 (LLZO-Ga) with x wt% CuO (x = 0, 0.2, 0.5, 1, 2) by the traditional solid-state reaction method, in which CuO was introduced as a sintering aid to reduce the sintering temperature of LLZO-Ga and increase its Li-ion conductivity. It is found that adding a small amount of CuO as an additive can reduce the sintering temperature from 1100 ℃ to about 1000 ℃. As a result, when the amount of CuO is 0.5 wt%, LLZO-Ga shows the highest room-temperature ionic conductivity and the lowest activation energy, which are 1.111 mS/cm and 0.27 eV, respectively.
... Current research on the next-generation batteries can be divided into LIB-related research, which corresponds to the mature stage, and future battery-related fields, corresponding to the introduction/growth stage, in consideration of the technological cycle. Lithium-sulfur battery (LSB), [17][18][19][20][21][22][23][24][25] lithium-metal battery (LMB), [26][27][28][29][30][31][32][33][34][35] and lithium-air battery (LAB) [36][37][38][39][40][41][42][43][44][45][46][47][48] have been studied to overcome the limitations of LIB energy density, and all-solidstate batteries have been developed to overcome safety issues of battery. In addition, other next-generation battery technologies are emerging such as flexible batteries [49][50][51][52][53][54][55][56][57][58][59][60][61][62] that can bend, and sodium-ion [63][64][65][66][67][68][69][70][71][72][73][74] and zinc-air batteries 41,[75][76][77][78][79][80][81][82][83][84][85][86] for price and supply stability. ...
Batteries are a promising technology in the field of electrical energy storage and have made tremendous strides in recent few decades. In particular, lithium‐ion batteries are leading the smart device era as an essential component of portable electronic devices. From the materials aspect, new and creative solutions are required to resolve the current technical issues on advanced lithium (Li) batteries and improve their safety. Metal‐organic frameworks (MOFs) are considered as tempting candidates to satisfy the requirements of advanced energy storage technologies. In this review, we discuss the characteristics of MOFs for application in different types of Li batteries. A review of these emerging studies in which MOFs have been applied in lithium storage devices can provide an informative blueprint for future MOF research on next‐generation advanced energy storage devices. In this review, we discuss the characteristics of metal‐organic frameworks (MOFs) applied to lithium storage devices containing Li‐ion, Li‐sulfur, Li‐metal, and Li‐O2. We summarize the origin, nomenclature, and synthesis method of MOFs, and report on recent studies in which MOFs and MOF‐derived materials are applied to lithium rechargeable batteries. This provides an informative roadmap for next‐generation advanced energy storage devices.
... All-solid-state batteries are attracting significant scientific attention because such power sources have a number of advantages over commercially available lithium-ion batteries [1][2][3][4][5][6][7]. In particular, they offer improved safety over a wider operating temperature range and increased stability to aggressive atmospheres and high pressures. ...
Cathode modification by Li2O–B2O3–SiO2 glass addition can be considered one of the ways to solve the problem of the increased interfacial resistance between solid electrolyte and solid cathode. The chemical and thermal stability of composite solid electrolyte based on Li7La3Zr2O12 in contact with LiCoO2 and glass additive was studied using XRD and DSC analysis. It was established that the interaction in the mixture studied begins at 670 °C. Therefore, 650 °C at 1 h was chosen as heat treatment conditions for (100-x)LiCoO2 + x 65Li2O·27B2O3·8SiO2 | solid electrolyte half-cells (x = 0–20 wt%). It was established that 5 wt% of glass addition is optimal to reduce the interfacial resistance. It can be concluded that Li2O–B2O3–SiO2 glass addition in LiCoO2 leads to the tight contact with composite electrolyte based on Li7La3Zr2O12 and the decrease in the interface resistance between the two solids.
