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Lithium metal anode is regarded as the ultimate negative electrode material due to its high theoretical capacity and low electrochemical potential. However, the significantly high reactivity of Li metal limits the practical application of Li metal batteries. To improve the stability of the interface between Li metal and an electrolyte, a facile and scalable blade coating method was used to cover the commercial polyethylene membrane separator with an inorganic/organic composite solid electrolyte layer containing lithium-ion-conducting ceramic fillers. The coated separator suppressed the interfacial resistance between the Li metal and the electrolyte and consequently prolonged the cycling stability of deposition/dissolution processes in Li/Li symmetric cells. Furthermore, the effect of the coating layer on the discharge/charge cycling performance of lithium-oxygen batteries was investigated.

Research devoted to room temperature lithium–sulfur (Li/S 8 ) and lithium–oxygen (Li/O 2 ) batteries has significantly increased over the past ten years. The race to develop such cell systems is mainly motivated by the very high theoretical energy density and the abundance of sulfur and oxygen. The cell chemistry, however, is complex, and progress toward practical device development remains hampered by some fundamental key issues, which are currently being tackled by numerous approaches. Quite surprisingly, not much is known about the analogous sodium-based battery systems, although the already commercialized, high-temperature Na/S 8 and Na/NiCl 2 batteries suggest that a rechargeable battery based on sodium is feasible on a large scale. Moreover, the natural abundance of sodium is an attractive benefit for the development of batteries based on low cost components. This review provides a summary of the state-of-the-art knowledge on lithium–sulfur and lithium–oxygen batteries and a direct comparison with the analogous sodium systems. The general properties, major benefits and challenges, recent strategies for performance improvements and general guidelines for further development are summarized and critically discussed. In general, the substitution of lithium for sodium has a strong impact on the overall properties of the cell reaction and differences in ion transport, phase stability, electrode potential, energy density, etc. can be thus expected. Whether these differences will benefit a more reversible cell chemistry is still an open question, but some of the first reports on room temperature Na/S 8 and Na/O 2 cells already show some exciting differences as compared to the established Li/S 8 and Li/O 2 systems.

Aprotic lithium‐oxygen (Li‐O2) batteries represent a promising next‐generation energy storage system due to their extremely high theoretical specific capacity compared with all known batteries. Their practical realization is impeded, however, by the sluggish kinetics for the most part, resulting in high overpotential and poor cycling performance. Due to the high catalytic activity and favorable stability of Co‐based transition metal oxides, they are regarded as the most likely candidate catalysts, facilitating researchers to solve the sluggish kinetics issue. Herein, this review first presents recent advanced design strategies for Co‐based transition metal oxides in Li‐O2 batteries. Then, the fundamental insights related to the catalytic processes of Co‐based transition metal oxides in traditional and novel Li‐O2 electrochemistry systems are summarized. Finally, we conclude with the current limitations and future development directions of Co‐based transition metal oxides, which will contribute to the rational design of catalysts and the practical applications of Li‐O2 batteries. Advanced design strategies, fundamental insights, and challenges for CoxOy‐catalyzed lithium‐oxygen batteries are critically analyzed, with possible development directions emphasized.

The rational design of a stable and catalytic carbon cathode is crucial for the development of rechargeable lithium‐oxygen (LiO2) batteries. An edge‐site‐free and topological‐defect‐rich graphene‐based material is proposed as a pure carbon cathode that drastically improves LiO2 battery performance, even in the absence of extra catalysts and mediators. The proposed graphene‐based material is synthesized using the advanced template technique coupled with high‐temperature annealing at 1800 °C. The material possesses an edge‐site‐free framework and mesoporosity, which is crucial to achieve excellent electrochemical stability and an ultra‐large capacity (>6700 mAh g−1). Moreover, both experimental and theoretical structural characterization demonstrates the presence of a significant number of topological defects, which are non‐hexagonal carbon rings in the graphene framework. In situ isotopic electrochemical mass spectrometry and theoretical calculations reveal the unique catalysis of topological defects in the formation of amorphous Li2O2, which may be decomposed at low potential (∼ 3.6 V versus Li/Li+) and leads to improved cycle performance. Furthermore, a flexible electrode sheet that excludes organic binders exhibits an extremely long lifetime of up to 307 cycles (>1535 h), in the absence of solid or soluble catalysts. These findings may be used to design robust carbon cathodes for LiO2 batteries. An edge‐site‐free and topological‐defect‐rich graphene mesosponge (GMS) is proposed as a carbon cathode for lithium‐oxygenbatteries. The GMS is highly stable, with high discharge capacity, low charge plateau and enhanced electrochemical stability compared to other commercial carbon materials. The table of contents image shows the formation of easily‐decomposable Li2O2 at the topological defects on GMS.

ABSTRACT Bacterial cellulose (BC) as a natural polymer possessing ultrafine nanofibrous network and high crystallinity, leading to its remarkable tensile strength, moisture retention and natural degradability. In this study, we revealed that this BC membrane has excellent affinity to organic electrolyte, high ionic conductivity and inherent ion selectivity as well. Due to its ability of migrating lithium ions and suppressing the shuttling of anions across the membranes, it is deemed as available model for iodide‐assisted lithium‐oxygen batteries (LOBs). The cycle life of the LOBs significantly extends from 74 rounds to 341 rounds at 1.0 A g−1 with a fixed capacity of 1000 mAh g−1, when replacing glass fiber (GF) by BC membrane. More importantly, the rate performance improves significantly from 42 to 36 cycles to 215 and 116 cycles after equipping with the BC membrane at 3.0 and 5.0 A g−1. Surprisingly, the full discharge capacity dramatically enhanced by ca. eight times from 4,163 mAh g−1 (GF) to 32,310 mAh g−1 (BC). Benefited from the convenient biosynthesis, cost‐effectiveness and high chemical‐thermal stability, these qualities of the BC membrane accelerate the development and make it more viable for application in advancing next‐generation environmentally friendly LOBs technology with high energy density. Bacterial cellulose (BC) is a natural polymer with ultrafine nanofibrous network. BC membrane has excellent affinity to organic electrolyte, high ionic conductivity and inherent ion selectivity, which can transfer lithium ions and suppress the shuttling of anions across the membrane, available for iodide‐assisted lithium‐oxygen batteries (LOBs). Summary Bacterial cellulous (BC) membranes could be utilized as separator after purification. BC membranes exhibited high Li+ conductivity and minimum permeation of I− and I3−. BC separators significantly enhanced the LiI‐mediated lithium‐oxygen batteries. BC separators are cost‐effective with high thermal and chemical stability.

In recent years, the demand for high-performance rechargeable lithium batteries has increased significantly, and many efforts have been made to boost the use of advanced electrode materials. Since graphene was first isolated by Novoselov et al., graphene/graphene-based materials have become an active area of research and are considered to be promising high-performance electrode materials. Graphene is a two-dimensional single-atom carbon-packed material that possesses fascinating properties, including a large surface area, remarkable electrical conductivity, extraordinary intrinsic electron mobility, high Young's modulus, superior mechanical strength, optical transmittance, catalytic performance, and stability. Therefore, graphene is considered an attractive material for rechargeable lithium-ion batteries (LIBs), lithium-sulfur batteries (LSBs), and lithium-oxygen batteries (LOBs). In this comprehensive review, we emphasise the recent progress in the controllable synthesis, functionalisation, and role of graphene in rechargeable lithium batteries. Finally, in this review, we aim to address the most promising results, benefits, challenges, critical issues, research directions, and perspectives to explain the developmental directions of graphene for batteries.

Sluggish kinetic characteristics of the electrode reactions and low electrode space utilization for solid Li2O2 deposition are limiting factors for Li–O2 batteries. In this work, iron‐/cobalt‐doped micron‐sized honeycomb‐like carbon (Fe‐MHC, Co‐MHC) with a hierarchical pore structure is prepared by using nano‐CaCO3 as a template. The effect of the transition‐metal nanoparticles as a second template on further pore construction and optimization is presented. As graphitization catalysts, the added transition metals also affect the formation of the graphene‐rich structure in the carbon framework. As a result, the obtained hierarchical carbon materials doped with trace metals exhibit higher electrochemical catalytic activity and stability than non‐doped samples. In particular, an enhanced discharge capacity as high as 9260 mAh g−1 is achieved for the Fe‐MHC cathode, which is attributed to its enlarged pore volume and high utilization of the electrode space. Improving cathodes: Added transition‐metal components, as assisting templates and graphitization catalysts, have a great effect on the pore optimization and graphene‐rich structure formation in carbon frameworks (see figure). The obtained hierarchical carbon materials doped with trace metals exhibit enhanced discharge capacities, electrocatalytic activities, and stabilities for use in Li–O2 batteries.

The energy-power trade-off in lithium-oxygen batteries (LOBs) arises from sluggish oxygen (O ) transport in the porous positive electrode and pore clogging by lithium peroxide (Li O ). While increasing porosity enhances electrolyte accessibility and Li O storage, it also increases electrolyte demand, compromising the overall energy density of the cell and necessitating alternative strategies to boost power capabilities without sacrificing energy density. In this study, theoretical simulations of O transport reveal that reducing tortuosity by improving pore interconnectivity has a more significant impact on O transport than porosity itself. Based on this insight, a freestanding graphene-based electrode with a highly interconnected macroporous network is fabricated via a non-solvent-induced phase separation approach using polyacrylonitrile (PAN) as a carbon scaffold and polyethylene oxide (PEO) as a sacrificial porogen. The selective decomposition of PEO creates spatially interconnected macropores, effectively reducing tortuosity. The resulting electrode enables LOB cells to achieve >2500 mAh g at 1.0 mA cm under lean-electrolyte conditions. Stable cycling at 4 mAh cm is maintained with only 3.25 g Ah electrolyte, and high-rate performance persists over 90 cycles at 1.5 mA cm . This work demonstrates a robust strategy to simultaneously improve energy and power performance in practical LOBs through rational electrode architecture.

Metallic lithium is deemed as the “Holy Grail” anode in high-energy-density secondary batteries. Uncontrollable lithium dendrite growth and related issues originated from uneven concentration distribution of Li + in the vicinity of the anode, however, induce severe safety concerns and poor cycling efficiency, dragging lithium metal anode out of practical application. Herein we address these issues by using cross-linked lithiophilic amino phosphonic acid resin as the effective host with the ion-transport-enhancement feature. Based on theoretical calculations and multiphysics simulation, it is found that this ion-transport-enhancement feature is capable of facilitating the self-concentration kinetics of Li + and accelerating Li + transfer at the electrolyte/electrode interface, leading to uniform bulk lithium deposition. Experimental results show that the proposed lithium-hosting resin decreases the irreversible lithium capacity and improves lithium utilization (with the Coulombic efficiency (CE) of 98.8% over 130 cycles). Our work demonstrates that inducing the self-concentrating distribution of Li + at the interface can be an effective strategy for improving the interfacial ion concentration gradient and optimizing lithium deposition, which opens a new avenue for the practical development of next-generation lithium metal batteries.

Sustainable energy is the key issue for the environment protection, human activity and economic development. Ionic liquids (ILs) and deep eutectic solvents (DESs) are dogmatically regarded as green and sustainable electrolytes in lithium-ion, lithium-metal (e.g., lithium-sulphur, lithium-oxygen) and post-lithium-ion (e.g., sodium-ion, magnesium-ion, and aluminum-ion) batteries. High electrochemical stability of ILs/DESs is one of the prerequisites for green, sustainable and safe energy; while easy electrochemical decomposition of ILs/DESs would be contradictory to the concept of green chemistry by adding the cost, releasing volatile/hazardous by-products and hindering the recyclability. However, (1) are ILs/DESs-based electrolytes really electrochemically stable when they are not used in batteries? (2) are ILs/DESs-based electrolytes really electrochemically stable in real batteries? (3) how to design ILs/DESs-based electrolytes with high electrochemical stability for batteries to achieve sustainability and green development? Up to now, there is no summary on this topic, to the best of our knowledge. Here, we review the effect of chemical structure and non-structural factors on the electrochemical stability of ILs/DESs in simulated conditions. More importantly, electrochemical stability of ILs/DESs in real lithium-ion, lithium-metal and post-lithium-ion batteries is concluded and compared. Finally, the strategies to improve the electrochemical stability of ILs/DESs in lithium-ion, lithium-metal and post-lithium-ion batteries are proposed. This review would provide a guide to design ILs/DESs with high electrochemical stability for lithium-ion, lithium-metal and post-lithium-ion batteries to achieve sustainable and green energy. Electrochemical stability of ionic liquids-/deep eutectic solvents-based electrolytes in lithium-ion, lithium-metal and post-lithium-ion batteries is reviewed. [Display omitted] •ILs and DESs are widely used as electrolytes in lithium-ion, lithium-metal and post-lithium-ion batteries.•This review for the first time summarizes the electrochemical stability of ILs-/DESs-based electrolytes in real batteries.•This review would favor the design of ILs/DESs with high electrochemically stable batteries.