Functionalized Boron Nitride Nanosheets/Graphene Interlayer for Fast and Long‐Life Lithium–Sulfur Batteries
TL;DR: In this article, a thin and selective interlayer structure has been designed and produced to decrease the charge transfer resistance and mitigate the shuttling problem, simply by coating the surface of cathode with a thin film of functionalized boron nitride nanosheets/graphene.
Abstract: Lithium–sulfur (Li–S) batteries have a much higher energy density than Li ion batteries and thus are considered as next generation batteries for electric vehicle applications. However, the problem of rapid capacity fading due to the shuttling of soluble polysulfides between electrodes remains the main obstacle for practical applications. Here, a thin and selective interlayer structure has been designed and produced to decrease the charge transfer resistance and mitigate the shuttling problem, simply by coating the surface of cathode with a thin film of functionalized boron nitride nanosheets/graphene. Due to this thin and ultralight interlayer, the specific capacity and cycling stability of the Li–S batteries with a cathode of sulfur-containing porous carbon nanotubes (≈60 wt% sulfur content) have been improved significantly with a life of over 1000 cycles, an initial specific capacity of 1100 mA h g−1 at 3 C, and a cycle decay as low as 0.0037% per cycle. This new interlayer provides a promising approach to significantly enhance the performance of Li–S batteries.
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TL;DR: In this paper, an in situ constructed VO2-VN binary host was proposed for Li-S batteries, which combines the merits of ultrafast anchoring (VO2) with electronic conducting (VN) to accomplish smooth immobilization-diffusion-conversion of LiPSs.
Abstract: Lithium–sulfur (Li–S) batteries are deemed as one of the most promising next-generation energy storage systems. However, their practical application is hindered by existing drawbacks such as poor cycling life and low Coulombic efficiency due to the shuttle effect of lithium polysulfides (LiPSs). We herein present an in situ constructed VO2–VN binary host which combines the merits of ultrafast anchoring (VO2) with electronic conducting (VN) to accomplish smooth immobilization–diffusion–conversion of LiPSs. Such synchronous advantages have effectively alleviated the polysulfide shuttling, promoted the redox kinetics, and hence improved the electrochemical performance of Li–S batteries. As a result, the sulfur cathode based on the VO2–VN/graphene host exhibited an impressive rate capability with ∼1105 and 935 mA h g−1 at 1C and 2C, respectively, and maintained long-term cyclability with a low capacity decay of 0.06% per cycle within 800 cycles at 2C. More remarkably, favorable cyclic stability can be attained with a high sulfur loading (13.2 mg cm−2). Even at an elevated temperature (50 °C), the cathodes still delivered superior rate capacity. Our work emphasizes the importance of immobilization–diffusion–conversion of LiPSs toward the rational design of high-load and long-life Li–S batteries.
421 citations
TL;DR: In this article, a review of the advanced interlayer systems is presented, and the operating mechanisms and widespread availability of interlayers in lithium-sulfur batteries are concluded.
340 citations
TL;DR: Li et al. as mentioned in this paper used zinc sulfide (ZnS) as an activation catalyst in Li-S battery to suppress the soluble polysulfide shuttle effect by powering kinetics redox reactions.
328 citations
TL;DR: The proposed strategy of constructing an all-MXene-based cathode can be readily extended to assemble a large number of MXene-derived materials, from a group of 60+ MAX phases, for applications such as various batteries and supercapacitors.
Abstract: High-energy-density lithium–sulfur (Li–S) batteries hold promise for next-generation portable electronic devices, but are facing great challenges in rational construction of high-performance flexible electrodes and innovative cell configurations for actual applications Here we demonstrated an all-MXene-based flexible and integrated sulfur cathode, enabled by three-dimensional alkalized Ti3C2 MXene nanoribbon (a-Ti3C2 MNR) frameworks as a S/polysulfides host (a-Ti3C2–S) and two-dimensional delaminated Ti3C2 MXene (d-Ti3C2) nanosheets as interlayer on a polypropylene (PP) separator, for high-energy and long-cycle Li–S batteries Notably, an a-Ti3C2 MNR framework with open interconnected macropores and an exposed surface area guarantees high S loading and fast ionic diffusion for prompt lithiation/delithiation kinetics, and the 2D d-Ti3C2 MXene interlayer remarkably prevents the shuttle effect of lithium polysulfides via both chemical absorption and physical blocking As a result, the integrated a-Ti3C2–S/d
309 citations
TL;DR: In this paper, the challenges and prospects for designing highly efficient catalysts for Li-S batteries are discussed, and various catalysts with high activity for stabilizing the lithium-polysulfide shuttle process and thus improving the electrochemical performance of Li S batteries are reviewed.
307 citations
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TL;DR: The energy that can be stored in Li-air and Li-S cells is compared with Li-ion; the operation of the cells is discussed, as are the significant hurdles that will have to be overcome if such batteries are to succeed.
Abstract: Li-ion batteries have transformed portable electronics and will play a key role in the electrification of transport. However, the highest energy storage possible for Li-ion batteries is insufficient for the long-term needs of society, for example, extended-range electric vehicles. To go beyond the horizon of Li-ion batteries is a formidable challenge; there are few options. Here we consider two: Li-air (O(2)) and Li-S. The energy that can be stored in Li-air (based on aqueous or non-aqueous electrolytes) and Li-S cells is compared with Li-ion; the operation of the cells is discussed, as are the significant hurdles that will have to be overcome if such batteries are to succeed. Fundamental scientific advances in understanding the reactions occurring in the cells as well as new materials are key to overcoming these obstacles. The potential benefits of Li-air and Li-S justify the continued research effort that will be needed.
7,895 citations
TL;DR: The development of novel composite cathode materials including sulfur-carbon and sulfur-polymer composites are described, describing the design principles, structure and properties, and electrochemical performances of these new materials.
Abstract: Electrical energy storage is one of the most critical needs of 21st century society. Applications that depend on electrical energy storage include portable electronics, electric vehicles, and devices for renewable energy storage from solar and wind. Lithium-ion (Li-ion) batteries have the highest energy density among the rechargeable battery chemistries. As a result, Li-ion batteries have proven successful in the portable electronics market and will play a significant role in large-scale energy storage. Over the past two decades, Li-ion batteries based on insertion cathodes have reached a cathode capacity of ∼250 mA h g(-1) and an energy density of ∼800 W h kg(-1), which do not meet the requirement of ∼500 km between charges for all-electric vehicles. With a goal of increasing energy density, researchers are pursuing alternative cathode materials such as sulfur and O2 that can offer capacities that exceed those of conventional insertion cathodes, such as LiCoO2 and LiMn2O4, by an order of magnitude (>1500 mA h g(-1)). Sulfur, one of the most abundant elements on earth, is an electrochemically active material that can accept up to two electrons per atom at ∼2.1 V vs Li/Li(+). As a result, sulfur cathode materials have a high theoretical capacity of 1675 mA h g(-1), and lithium-sulfur (Li-S) batteries have a theoretical energy density of ∼2600 W h kg(-1). Unlike conventional insertion cathode materials, sulfur undergoes a series of compositional and structural changes during cycling, which involve soluble polysulfides and insoluble sulfides. As a result, researchers have struggled with the maintenance of a stable electrode structure, full utilization of the active material, and sufficient cycle life with good system efficiency. Although researchers have made significant progress on rechargeable Li-S batteries in the last decade, these cycle life and efficiency problems prevent their use in commercial cells. To overcome these persistent problems, researchers will need new sulfur composite cathodes with favorable properties and performance and new Li-S cell configurations. In this Account, we first focus on the development of novel composite cathode materials including sulfur-carbon and sulfur-polymer composites, describing the design principles, structure and properties, and electrochemical performances of these new materials. We then cover new cell configurations with carbon interlayers and Li/dissolved polysulfide cells, emphasizing the potential of these approaches to advance capacity retention and system efficiency. Finally, we provide a brief survey of efficient electrolytes. The Account summarizes improvements that could bring Li-S technology closer to mass commercialization.
1,888 citations
TL;DR: In this paper, the authors report a quantitative analysis of the shuttle phenomenon in Li/S rechargeable batteries and present experimental evidence that selfdischarge, charge-discharge efficiency, charge profile, and overcharge protection are all facets of the same phenomenon.
Abstract: This work reports a quantitative analysis of the shuttle phenomenon in Li/S rechargeable batteries. The work encompasses theoretical models of the charge process, charge and discharge capacity, overcharge protection, thermal effects, self-discharge, and a comparison of simulated and experimental data. The work focused on the features of polysulfide chemistry and polysulfide interaction with the Li anode, a quantitative description of these phenomena, and their application to the development of a high-energy rechargeable battery. The objective is to present experimental evidence that self-discharge, charge-discharge efficiency, charge profile, and overcharge protection are all facets of the same phenomenon.
1,793 citations
TL;DR: A simple adjustment to the traditional lithium-sulphur battery configuration is reported to achieve high capacity with a long cycle life and rapid charge rate and with a significant improvement not only in the active material utilization but also in capacity retention without involving complex synthesis or surface modification.
Abstract: The limitations in the cathode capacity compared with that of the anode have been an impediment to advance the lithium-ion battery technology. The lithium–sulphur system is appealing in this regard, as sulphur exhibits an order of magnitude higher capacity than the currently used cathodes. However, low active material utilization and poor cycle life hinder the practicality of lithium–sulphur batteries. Here we report a simple adjustment to the traditional lithium–sulphur battery configuration to achieve high capacity with a long cycle life and rapid charge rate. With a bifunctional microporous carbon paper between the cathode and separator, we observe a significant improvement not only in the active material utilization but also in capacity retention, without involving complex synthesis or surface modification. The insertion of a microporous carbon interlayer decreases the internal charge transfer resistance and localizes the soluble polysulphide species, facilitating a commercially feasible means of fabricating the lithium–sulphur batteries. The practical performance of lithium sulphide batteries is much less than their predicted performance because redox products dissolve over time. Su and Manthiram show that microporous carbon membranes inserted between cathode and separator localize soluble polysulphide species and improve battery cycling characteristics.
1,289 citations
TL;DR: In this paper, a metal-organic framework (MOF)-based separator was proposed to mitigate the shuttling problem in lithium-sulfur batteries, which selectively sieves Li+ ions while efficiently suppressing undesired polysulfides migrating to the anode side.
Abstract: Lithium–sulfur batteries are a promising energy-storage technology due to their relatively low cost and high theoretical energy density. However, one of their major technical problems is the shuttling of soluble polysulfides between electrodes, resulting in rapid capacity fading. Here, we present a metal–organic framework (MOF)-based battery separator to mitigate the shuttling problem. We show that the MOF-based separator acts as an ionic sieve in lithium–sulfur batteries, which selectively sieves Li+ ions while efficiently suppressing undesired polysulfides migrating to the anode side. When a sulfur-containing mesoporous carbon material (approximately 70 wt% sulfur content) is used as a cathode composite without elaborate synthesis or surface modification, a lithium–sulfur battery with a MOF-based separator exhibits a low capacity decay rate (0.019% per cycle over 1,500 cycles). Moreover, there is almost no capacity fading after the initial 100 cycles. Our approach demonstrates the potential for MOF-based materials as separators for energy-storage applications. One of the major problems in Li–S batteries is the undesired shuttling of lithium polysulfides between electrodes. Here the authors present a metal–organic framework-based separator to mitigate the shuttle effect, leading to stable long cycles.
971 citations