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Lithium metal is the “holy grail” anode for next‐generation high‐energy rechargeable batteries due to its high capacity and lowest redox potential among all reported anodes. However, the practical application of lithium metal batteries (LMBs) is hindered by safety concerns arising from uncontrollable Li dendrite growth and infinite volume change du...
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Citations
... of Li metal batteries. [4][5][6] Various strategies have been employed to tackle this issue, such as developing electrolytes and additives, [7][8][9][10] introducing artificial solid electrolyte interphase (SEI) layers, modifying the surface of the Li host material [11][12][13][14] and modifying the design of the host material. [15] Among these, modifying the Li host has been identified as the most effective method for controlling Li deposition behavior, as it can be easily controlled by the electrode design and highly influences the surface atmosphere. ...
Uniform lithium deposition is essential to hinder dendritic growth. Achieving this demands even seed material distribution across the electrode, posing challenges in correlating the electrode's surface structure with the uniformity of seed material distribution. In this study, the effect of periodic surface and facet orientation on seed distribution is investigated using a model system consisting of a wrinkled copper (Cu)/graphene structure with a [100] facet orientation. A new methodology is developed for uniformly distributed silver (Ag) nanoparticles over a large area by controlling the surface features of Cu substrates. The regularly arranged Ag nanoparticles, with a diameter of 26.4 nm, are fabricated by controlling the Cu surface condition as [100]‐oriented wrinkled Cu. The wrinkled Cu guides a deposition site for spherical Ag nanoparticles, the [100] facet determines the Ag morphology, and the presence of graphene leads to spacings of Ag seeds. This patterned surface and high lithiophilicity, with homogeneously distributed Ag nanoparticles, lead to uniform Li⁺ flux and reduced nucleation energy barrier, resulting in excellent battery performance. The electrochemical measurements exhibit improved cyclic stability over 260 cycles at 0.5 mA cm⁻² and 100 cycles at 1.0 mA cm⁻² and enhanced kinetics even under a high current density of 5.0 mA cm⁻².
... A thick SEI layer can form on the lithium surface that consumes both the electrolyte and the lithium metal due to the instability of the lithium anodes with the electrolyte, which can also lead to irreversible reactions between the lithium metal and the electrolyte. The SEI layer, the deterioration of the active components and electrode, and even battery swelling can all result from the volume variations of the lithium anodes [4][5][6][7]. Computational modelling is used to simulate and examine the battery's behavior in order to overcome these issues. The formation and effects of lithium dendrites [8,9], as well as the intercalation, diffusion, migration, and reaction of lithium ions [10,11], can all be simulated using computational simulations, such as molecular dynamics (MD) simulations and first-principles calculations based on density function theory (DFT). ...
In the area of high energy density batteries, lithium metal has attracted a lot of interest as an electrode material. But since lithium is so reactive, lithium metal batteries frequently have safety problems like thermal runaway, particularly under conditions such as overcharging, over-discharging, high temperatures, and mechanical impact. These safety issues can lead to dangerous situations such as battery explosion and fire. Furthermore, lithium-metal batteries are prone to dendrite development during the cycling process, which can pierce the separator and result in internal short-circuits, shortening the battery's cycle life. Lithium-metal battery use is strongly constrained by these important problems. To overcome these challenges, researchers are exploring various strategies, such as developing new electrolytes and additives, designing new battery structures, and exploring new anode materials. Computational simulations have emerged as a powerful tool to aid in this research. This review summarizes the recent applications of computational simulations in lithium metal batteries. Specifically, molecular dynamics (MD) and first-principles calculations have been widely employed to study key issues such as interface reactions, ion transport, and dendrite formation in lithium batteries. Additionally, this review discusses recent research directions in new types of ion electrolytes that can effectively address the safety concerns of lithium batteries and increase energy density, while still facing challenges in interface resistance and conductivity. The discussion of potential avenues for future research that will be pursued finishes this paper. These possibilities include multiscale simulations, the creation and manufacturing of new electrolyte materials, and the functional modification of lithium-metal anode surfaces.
... Figure 3A-E illustrates the detailed formation mechanism of dead lithium and the consequent failure process of lithium batteries. Notably, dendrite necks with larger curvature tend to accumulate at a higher electron density and exhibit faster rates of lithium dissolution [17] . This often results in dendrite fractures at these sites. ...
The energy density of conventional graphite anode batteries is insufficient to meet the requirement for portable devices, electric cars, and smart grids. As a result, researchers have diverted to lithium metal anode batteries. Lithium metal has a theoretical specific capacity (3,860 mAh·g-1) significantly higher than that of graphite. Additionally, it has a lower redox potential of -3.04 V compared to standard hydrogen electrodes. These properties make high-energy lithium metal batteries a promising candidate for next-generation energy storage devices, which have garnered significant interest for several years. However, the high activity of lithium metal anodes poses safety risks (e.g., short circuits and thermal runaway) that hinder their commercial growth. Currently, modification of reversible lithium anodes is the primary focus of lithium metal batteries. This article presents conceptual models and numerical simulations that address failure processes and offer specific techniques to mitigate the challenges of lithium metal anodes, including electrolyte design, interface engineering, and electrode modification. It is expected that lithium metal batteries will recover and become a feasible energy storage solution.
... Such degradations become more serious with increased Ni content, especially for NMC811 of commercial interest [17]. There are some strategies to overcome these challenges, for example, an artificial interlayer between electrode and electrolyte [18], solid-state electrolyte [19], porous current collector [20], and liquid electrolyte engineering [21]. Among these strategies, liquid electrolyte engineering is very efficient and fits best with the existing industry. ...
The combination of Li-metal anode and high-voltage cathode is regarded as a solution for the next-generation high-energy-density secondary batteries. However, a traditional electrolyte is either incompatible with the Li-metal anode or vulnerable to high voltage. This work reports a 1 M dual-salts Localized-High-Concentration-Electrolyte with Fluoroethylene carbonate (FEC) additive. It enables stable cycling of Li||LiNi0.8Co0.1Mn0.1O2 (NMC811) battery, which shows 81.5% capacity retention after 300 cycles with a charge/discharge current density of 1 C and a voltage range of 2.7–4.4 V. Scanning electron microscopy (SEM) images show that this electrolyte not only largely reduced Li dendrites and ‘dead’ Li on anode surface but also well protected the microstructure of NMC811 cathode. Possible components of both solid-electrolyte interlayer (SEI) and cathode-electrolyte interlayer (CEI) were characterized by energy-dispersive X-ray spectroscopy (EDX). The result illustrates that FEC protected Li salts from decomposition on the anode side and suppressed the decomposition of solvents on the cathode side.
... Lithium-ion battery technologies[23][24][25]. ...
With the increasing adoption of electric vehicles (EVs), optimizing lithium-ion battery capacity is critical for overall powertrain performance. Recent studies have optimized battery capacity in isolation without considering interactions with other powertrain components. Furthermore, even when the battery is considered within the full powertrain, most works have only modeled the electrical behavior without examining thermal or ageing dynamics. However, this fails to capture systemic impacts on overall performance. This study takes a holistic approach to investigate the effects of battery capacity optimization on convergence of the full EV powertrain. A battery multiphysics model was developed in MATLAB/Simulink, incorporating experimental data on electrical, thermal, and ageing dynamics and interactions with other components. The model was evaluated using real-world WLTP and Artemis driving cycles to simulate realistic conditions lacking in prior works. The findings reveal significant impacts of battery optimization on total powertrain performance unaccounted for in previous isolated studies. By adopting a system-level perspective and realistic driving cycles, this work provides enhanced understanding of interdependent trade-offs to inform integrated EV design.
... 25 Finally, Li anodes may experience an uneven mass transfer, further leading to unlimited volume changes during the stripping/depositing process, giving rise to anode pulverization and poor electrochemical performance. Considerable efforts have been made to suppress the formation of undesired Li dendrite, including modification of the liquid electrolyte, [26][27][28] construction of the artificial electrolyte/anode interface, 29,30 use of solid electrolyte, [31][32][33] polymer electrolytes, 34,35 and designing of dendrite-free current collectors. 36,37 Given the lightweight, natural abundance, and structural designability, carbon materials and their composites have attracted extensive attention as favorable interfacial layers/hosts for Li anodes. ...
Metallic lithium (Li) is considered the “Holy Grail” anode material for the next‐generation of Li batteries with high energy density owing to the extraordinary theoretical specific capacity and the lowest negative electrochemical potential. However, owing to inhomogeneous Li‐ion flux, Li anodes undergo uncontrollable Li deposition, leading to limited power output and practical applications. Carbon materials and their composites with controllable structures and properties have received extensive attention to guide the homogeneous growth of Li to achieve high‐performance Li anodes. In this review, the correlation between the behavior of Li anode and the properties of carbon materials is proposed. Subsequently, we review emerging strategies for rationally designing high‐performance Li anodes with carbon materials, including interface engineering (stabilizing solid electrolyte interphase layer and other functionalized interfacial layer) and architecture design of host carbon (constructing three‐dimension structure, preparing hollow structure, introducing lithiophilic sites, optimizing geometric effects, and compositing with Li). Based on the insights, some prospects on critical challenges and possible future research directions in this field are concluded. It is anticipated that further innovative works on the fundamental chemistry and theoretical research of Li anodes are needed.
... The interfacial stability is determined by poor electrolyte-electrode contact, lithium dendrite growth and high-pressure decomposition [27]. To solve these problems, CPEs with the advantages of two components (organic and inorganic) become popular in recent years [158,159]. ...
With excellent energy densities and highly safe performance, solid-state lithium batteries (SSLBs) have been hailed as promising energy storage devices. Solid-state electrolyte is the core component of SSLBs and plays an essential role in the safety and electrochemical performance of the cells. Composite polymer electrolytes (CPEs) are considered as one of the most promising candidates among all solid-state electrolytes due to their excellent comprehensive performance. In this review, we briefly introduce the components of CPEs, such as the polymer matrix and the species of fillers, as well as the integration of fillers in the polymers. In particular, we focus on the two major obstacles that affect the development of CPEs: the low ionic conductivity of the electrolyte and high interfacial impedance. We provide insight into the factors influencing ionic conductivity, in terms of macroscopic and microscopic aspects, including the aggregated structure of the polymer, ion migration rate and carrier concentration. In addition, we also discuss the electrode-electrolyte interface and summarize methods for improving this interface. It is expected that this review will provide feasible solutions for modifying CPEs through further understanding of the ion conduction mechanism in CPEs and for improving the compatibility of the electrode-electrolyte interface.
... [7,8] The uneven Li deposition and huge volume change cause dendritic Li growth and solid electrolyte interphase (SEI) fracture, leading to the side reactions between Li anode and electrolyte and consuming active materials. [9][10][11][12] Besides, the extreme growth of Li dendrites would result in an internal short circuit. And the Li dendrites are easily detached from the anode, causing loss of metallic Li ("dead Li"). ...
Constructing a 3D composite Li metal anode (LMA) along with the engineering of artificial solid electrolyte interphase (SEI) is a promising strategy for achieving dendrite‐free Li deposition and high cycling stability. The nanostructure of artificial SEI is closely related to the performance of the LMA. Herein, the self‐grown process and morphology of in situ formed Li2S during lithiation of CuxS is studied systematically, and a large‐sized sheet‐like Li2S layer as an artificial SEI is in situ generated on the inner surface of a 3D continuous porous Cu skeleton (3DCu@Li2S‐S). The sheet‐like Li2S layer with few interfacial pitfalls (Cu/Li2S heterogeneous interface) possesses enhanced diffusion of Li ions. And the continuous porous structure provides transport channels for lithium‐ion transport. As a result, the 3DCu@Li2S‐S presents a high Coulombic efficiency (99.3%), long cycle life (500 cycles), and high‐rate performance (10 mA cm⁻²). Furthermore, Li/3DCu@Li2S anode fabricated by thermal infusion method inherits the synergistic advantages of sheet‐like Li2S and continuous porous structure. The Li/3DCu@Li2S anode shows significantly enhanced cycling life in both liquid and solid electrolytes. This work provides a new concept to design artificial SEI for LMA with high safe and high performance.
... The unstable SEI layer causes continuous exhaustion of the electrolyte, and lithium is discharged from lithium dendrites exhibiting a lower impedance during discharging, with some lithium being trapped in the SEI layer ("dead Li"), which becomes electrically inactive [75]. In this repeated process, the lithium anode endures significant volumetric expansion, threatening battery stability [76]. Therefore, forming a stable SEI layer during the commencement 12 International Journal of Energy Research of the battery reaction can be an effective method to prevent lithium dendrite formation and electrolyte depletion. ...
Although Li–S batteries (LSB) are one of the most promising electrochemical energy storage technologies, their practical applications are limited by their rapid capacity decay and uncontrolled lithium dendrite formation. In addition to the well-known role of a separator in lithium-ion batteries, LSB separators must perform additional functions. Using a facile electrospinning method, we developed an eco-friendly separator prepared from natural cellulose with an interconnected fibrous and porous structure rich in polar oxygen-containing functional groups. These polar functional groups enhance electrolyte wettability, polysulfide adsorption, and lithiophilicity, thus boosting LSB performance. A cellulose separator with a thickness (22 μm) comparable to that of a commercial polypropylene (Celgard) separator delivers an initial discharge capacity of 1458 mAh·g−1 at 0.1C with a high sulfur utilization of 87%, including a high reversible discharge capacity of 1091 mAh·g−1 for 100 cycles, exhibiting a 1.8-times greater capacity retention than those of Celgard-containing LSBs. In addition, an excellent rate capability of 908 mAh·g−1 can be achieved at a high rate of 1C. These intriguing characteristics indicate that these separators could replace conventional synthetic polymer-based separators for commercial LSBs.
... [44][45][46][47] In light of the significant achievements, several review articles have been published. [48][49][50][51][52][53][54][55] But there are rarely focused on liquid electrolytes toward fast-charging LMBs. This review first introduces how the electrolytes affect the fast-charging properties of LMBs and then summarizes the modifications of liquid electrolytes on LMBs in detail, including the Li salts, electrolyte additives, and novel solvents ( Figure 1). ...
Lithium (Li) metal batteries (LMBs) with fast‐charging capabilities could ease mileage anxiety, which is essential for the popularization of electric vehicles (EVs). However, the uncontrollable growth of Li dendrites and the repeated formation of electrode electrolyte interfaces will lead to safety risks and low coulombic efficiency, which hinder the practical application of LMBs. Liquid electrolytes play an extremely important role in solving these problems. This review focuses on the recent achievements of liquid electrolytes for fast‐charging LMBs. The main factors limiting the fast transportation of Li ions are first introduced. The recent progress in electrolyte regulation for fast‐charging LMBs, including Li salts, electrolyte additives, and novel organic solvents are summarized. Finally, a general conclusion and perspectives are proposed. This article is protected by copyright. All rights reserved.
