Systematic Evaluation of Carbon Hosts for High-Energy Rechargeable Lithium-Metal Batteries
TL;DR: In this article, Li-metal batteries have great potential for high energy and low cost, but poor Li anode stability remains a challenge, and a number of host structures have been widely studied.
Abstract: Rechargeable lithium (Li)-metal batteries have great potential for high energy and low cost, but poor Li anode stability remains a challenge. Carbon host structures have been widely studied; howeve...
Citations
More filters
TL;DR: In this article , a quasi-double-layer composite polymer electrolytes (QDL-CPEs) is proposed by using plasticizers with high oxidation stability (propylene carbonate) and high reduction stability (diethylene glycol dimethyl ether) in a poly(vinylidene fluoride) (PVDF)-based electrolyte composites.
Abstract: Increasing the energy density and long-term cycling stability of lithium-ion batteries necessitates the stability of electrolytes under high/low voltage application and stable electrode/electrolyte interfacial contact. However, neither a single polymer nor liquid electrolyte can realize this due to their limited internal energy gap, which cannot avoid lithium-metal deposition and electrolyte oxidation simultaneously. Herein, a novel type of quasi-double-layer composite polymer electrolytes (QDL-CPEs) is proposed by using plasticizers with high oxidation stability (propylene carbonate) and high reduction stability (diethylene glycol dimethyl ether) in a poly(vinylidene fluoride) (PVDF)-based electrolyte composites. In-situ-polymerized propylene carbonate can function as a cathode electrolyte interface (CEI) film, which can enhance the antioxidant ability. The nucleophilic substitution reaction between diethylene glycol dimethyl ether and PVDF increases the reduction stability of the electrolyte on the anodic side, without the formation of lithium dendrites. The QDL-CPEs has high ionic conductivity, an enhanced electrochemical reaction window, adjustable electrode/electrolyte interphases, and no additional electrolyte-electrolyte interfacial resistance. Thus, this ingenious design of the QDL-CPEs improves the cycling performance of a fabricated LiNi0.8 Co0.1 Mn0.1 O2 (NCM811)//QDL-CPEs//hard carbon full cell at room temperature, paving a new way for designing solid-state battery systems accessible for practical applications.
27 citations
TL;DR: In this paper, a 20% lithium oxalate and a LiNi0.3Co 0.3Mn 0.5O2 composite cathode were used to extend the lifetime of anode-free lithium metal batteries.
Abstract: Anode-free lithium metal batteries (AFLMBs) have been extensively studied due to their intrinsic high energy and safety without a metallic Li anode in cell design. Yet, the dendrite and dead-Li buildup continuously consumes the active Li upon cycling, leading to the poor lifespan of AFLMBs. Here, we introduce lithium oxalate into the cathode as an electrode additive providing a Li reservoir to extend the lifespan of AFLMBs. The AFLMB using 20% lithium oxalate and a LiNi0.3Co0.3Mn0.3O2 composite cathode exhibits >80 and 40% capacity retention after 50 and 100 cycles, respectively, outperforming the poor cycle life of fewer than 20 cycles obtained from the cell using a pure LiNi0.3Co0.3Mn0.3O2 cathode. Surprisingly, the average Coulombic efficiency of AFLMBs is found to improve as the amount of lithium oxalate increases in the composite cathode. This abnormal phenomenon could be attributed to the as-formed carbon dioxide after the first activation cycle forming a Li2CO3-rich solid-electrolyte interphase and improving the Li deposition and stripping efficiency. The findings in this work provide a new strategy to delay the capacity roll-over of AFLMBs from an electrode engineering perspective, which can be coupled with other approaches such as functional electrolytes synergistically to further improve the cycle life of AFLMBs for practical application.
13 citations
TL;DR: In this article , the conversion reaction of metal fluorides is exploited because metallic nanodomains formed during this reaction induce an alloying reaction with lithium ions for uniform and sustainable lithium de-plating.
Abstract: All‐solid‐state batteries (ASSBs) that employ anode‐less electrodes have drawn attention from across the battery community because they offer competitive energy densities and a markedly improved cycle life. Nevertheless, the composite matrices of anode‐less electrodes impose a substantial barrier for lithium‐ion diffusion and inhibit operation at room temperature. To overcome this drawback, here, the conversion reaction of metal fluorides is exploited because metallic nanodomains formed during this reaction induce an alloying reaction with lithium ions for uniform and sustainable lithium (de)plating. Lithium fluoride (LiF), another product of the conversion reaction, prevents the agglomeration of the metallic nanodomains and also protects the electrode from fatal lithium dendrite growth. A systematic analysis identifies silver (I) fluoride (AgF) as the most suitable metal fluoride because the silver nanodomains can accommodate the solid‐solution mechanism with a low nucleation overpotential. AgF‐based full cells attain reliable cycling at 25 °C even with an exceptionally high areal capacity of 9.7 mAh cm−2 (areal loading of LiNi0.8Co0.1Mn0.1O2 = 50 mg cm–2). These results offer useful insights into designing materials for anode‐less electrodes for sulfide‐based ASSBs.
11 citations
TL;DR: In this paper , a composite Mg metal anodes with high capacity utilization of 75% are achieved by coating magnesiophilic gold nanoparticles on copper foils for the first time.
Abstract: Metallic magnesium is a promising high-capacity anode material for energy storage technologies beyond lithium-ion batteries. However, most reported Mg metal anodes are only cyclable under shallow cycling (≤1 mAh cm-2) and thus poor Mg utilization (<3%) conditions, significantly compromising their energy-dense characteristic. Herein, composite Mg metal anodes with high capacity utilization of 75% are achieved by coating magnesiophilic gold nanoparticles on copper foils for the first time. Benefiting from homogeneous ionic flux and uniform deposition morphology, the Mg-plated Au-Cu electrode exhibits high average Coulombic efficiency of 99.16% over 170 h cycling at 75% Mg utilization. Moreover, the full cell based on Mg-plated Au-Cu anode and Mo6S8 cathode achieves superior capacity retention of 80% after 300 cycles at a low negative/positive ratio of 1.33. This work provides a simple yet effective general strategy to enhance Mg utilization and reversibility, which can be extended to other metal anodes as well.
10 citations
TL;DR: In this article , mechanically resilient graphene assembly microspheres with interlocked Ni/N-doped lithiophilic graphene nanostructures are developed as stable 3D graphene hosts for Li metal anodes.
Abstract: Li metal is considered the most attractive anode material for high‐energy Li batteries. However, the uncontrollable growth of Li dendrites and severe volume changes during Li plating and stripping inhibit the practical application of Li metal anodes. Herein, a synergistic strategy is developed not only to suppress Li dendrite growth but also to withstand repeated volume changes during long‐term cycling. Specifically, mechanically resilient graphene assembly microspheres with interlocked Ni/N‐doped lithiophilic graphene nanostructures grown in situ are developed as stable 3D graphene hosts for Li‐metal anodes. Importantly, the approach provides a novel strategy to control radial distribution of lithiophilic Ni nanocatalysts in the graphene assembly. These 3D graphene hosts can repeatedly guide the uniform deposition of Li owing to the high lithiophilicity of Ni nanocatalysts and the N‐doped graphene nanostructures. Furthermore, graphene nanoshell forms in situ between the graphene layers in the inner part of the graphene assembly, creating strong contacts between rGO layers and providing the 3D graphene host with high structural integrity. Notably, the approach emphasizes mechanical resilience of the 3D graphene host, which retains its initial morphology after repeated Li plating/stripping cycles. Consequently, the 3D graphene host maintains a highly stable coulombic efficiency of 99% over 500 cycles.
10 citations
References
More filters
TL;DR: This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium growth, summarizing the theoretical and experimental achievements and endeavors to realize the practical applications of lithium metal batteries.
Abstract: The lithium metal battery is strongly considered to be one of the most promising candidates for high-energy-density energy storage devices in our modern and technology-based society. However, uncontrollable lithium dendrite growth induces poor cycling efficiency and severe safety concerns, dragging lithium metal batteries out of practical applications. This review presents a comprehensive overview of the lithium metal anode and its dendritic lithium growth. First, the working principles and technical challenges of a lithium metal anode are underscored. Specific attention is paid to the mechanistic understandings and quantitative models for solid electrolyte interphase (SEI) formation, lithium dendrite nucleation, and growth. On the basis of previous theoretical understanding and analysis, recently proposed strategies to suppress dendrite growth of lithium metal anode and some other metal anodes are reviewed. A section dedicated to the potential of full-cell lithium metal batteries for practical applicatio...
3,812 citations
3,536 citations
TL;DR: In this article, various factors that affect the morphology and Coulombic efficiency of Li metal anodes have been analyzed, and the results obtained by modelling of Li dendrite growth have also been reviewed.
Abstract: Lithium (Li) metal is an ideal anode material for rechargeable batteries due to its extremely high theoretical specific capacity (3860 mA h g−1), low density (0.59 g cm−3) and the lowest negative electrochemical potential (−3.040 V vs. the standard hydrogen electrode). Unfortunately, uncontrollable dendritic Li growth and limited Coulombic efficiency during Li deposition/stripping inherent in these batteries have prevented their practical applications over the past 40 years. With the emergence of post-Li-ion batteries, safe and efficient operation of Li metal anodes has become an enabling technology which may determine the fate of several promising candidates for the next generation energy storage systems, including rechargeable Li–air batteries, Li–S batteries, and Li metal batteries which utilize intercalation compounds as cathodes. In this paper, various factors that affect the morphology and Coulombic efficiency of Li metal anodes have been analyzed. Technologies utilized to characterize the morphology of Li deposition and the results obtained by modelling of Li dendrite growth have also been reviewed. Finally, recent development and urgent need in this field are discussed.
3,394 citations
TL;DR: A review of post-lithium-ion batteries is presented in this paper with a focus on their operating principles, advantages and the challenges that they face, and the volumetric energy density of each battery is examined using a commercial pouch-cell configuration.
Abstract: Energy density is the main property of rechargeable batteries that has driven the entire technology forward in past decades. Lithium-ion batteries (LIBs) now surpass other, previously competitive battery types (for example, lead–acid and nickel metal hydride) but still require extensive further improvement to, in particular, extend the operation hours of mobile IT devices and the driving mileages of all-electric vehicles. In this Review, we present a critical overview of a wide range of post-LIB materials and systems that could have a pivotal role in meeting such demands. We divide battery systems into two categories: near-term and long-term technologies. To provide a realistic and balanced perspective, we describe the operating principles and remaining issues of each post-LIB technology, and also evaluate these materials under commercial cell configurations. Post-lithium-ion batteries are reviewed with a focus on their operating principles, advantages and the challenges that they face. The volumetric energy density of each battery is examined using a commercial pouch-cell configuration to evaluate its practical significance and identify appropriate research directions.
3,314 citations
TL;DR: Liu et al. as mentioned in this paper discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg−1, up to 500 Wh kg −1, for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials.
Abstract: State-of-the-art lithium (Li)-ion batteries are approaching their specific energy limits yet are challenged by the ever-increasing demand of today’s energy storage and power applications, especially for electric vehicles. Li metal is considered an ultimate anode material for future high-energy rechargeable batteries when combined with existing or emerging high-capacity cathode materials. However, much current research focuses on the battery materials level, and there have been very few accounts of cell design principles. Here we discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg−1, up to 500 Wh kg−1, for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials. We also provide an analysis of key factors such as cathode loading, electrolyte amount and Li foil thickness that impact the cell-level cycle life. Furthermore, we identify several important strategies to reduce electrolyte-Li reaction, protect Li surfaces and stabilize anode architectures for long-cycling high-specific-energy cells. Jun Liu and Battery500 Consortium colleagues contemplate the way forward towards high-energy and long-cycling practical batteries.
1,747 citations