Sulfiphilic surfaces: The design of novel host materials for sulfur cathodes in lithium–sulfur batteries has been achieved through modification of the surface chemistry, by employing sulfiphilic ...surfaces with high electrical conductivity to develop stable, high‐energy batteries. Compared to the physical‐confinement technique (see picture), systems prepared by this method exhibited remarkable enhancements of both capacity and cycling stability.
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Owing to high specific energy, low cost, and environmental friendliness, lithium–sulfur (Li–S) batteries hold great promise to meet the increasing demand for advanced energy storage beyond portable ...electronics, and to mitigate environmental problems. However, the application of Li–S batteries is challenged by several obstacles, including their short life and low sulfur utilization, which become more serious when sulfur loading is increased to the practically accepted level above 3–5 mg cm−2. More and more efforts have been made recently to overcome the barriers toward commercially viable Li–S batteries with a high sulfur loading. This review highlights the recent progress in high‐sulfur‐loading Li–S batteries enabled by hierarchical design principles at multiscale. Particularly, basic insights into the interfacial reactions, strategies for mesoscale assembly, unique architectures, and configurational innovation in the cathode, anode, and separator are under specific concerns. Hierarchy in the multiscale design is proposed to guide the future development of high‐sulfur‐loading Li–S batteries.
High‐sulfur‐loading lithium–sulfur (Li–S) batteries enabled by multiscale hierarchical design principles are reviewed. The basic insights into the interfacial reactions, strategies for mesoscale assembly, unique architectures, and configurational innovation in the cathode, anode, and separator are of specific concern. Hierarchy in the multiscale design is proposed to guide the future development of high‐sulfur‐loading Li–S batteries.
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Dilute alloying is an effective strategy to tune properties of solid catalysts but is rarely leveraged in complex reactions beyond small molecule conversion. In this work, dilute dopants are ...demonstrated to serve as activating centers to construct multiatom catalytic domains in metal nitride electrocatalysts for lithium–sulfur (Li–S) batteries, of which the sulfur cathode suffers from sluggish and complex conversion reactions. With titanium nitride (TiN) as a model system, the dilute cobalt alloying is shown to greatly improve the reaction kinetics while inducing negligible catalyst reconstruction. Compared to the pristine TiN, the dilute nitride alloy catalyst enables onefold increase in the high rate (2.0 C) capacities of Li–S batteries, as well as an impressively low cyclic decay rate of 0.17% at a sulfur loading of 4.0 mgS cm−2. This work opens up new opportunities toward the rational design of Li–S electrocatalysts by dilute alloying and also enlightens the understandings of complex domain‐catalyzed reactions in energy applications.
Dilute alloying implants “activating” centers in nitride alloy electrocatalysts to boost lithium–sulfur (Li–S) batteries. Dilute Co dopants activate the surrounding N and Ti atoms to construct multiatom active domains for efficient bidirectional catalysis of S redox reactions. The corresponding dilute nitride alloy improves the reaction kinetics and electrochemical performance of Li–S batteries.
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The discovery of non-magnetic extreme magnetoresistance (XMR) materials has induced great interest because the XMR phenomenon challenges our understanding of how a magnetic field can alter electron ...transport in semimetals. Among XMR materials, the LaSb shows XMR and field-induced exotic behaviors but it seems to lack the essentials for these properties. Here, we study the magnetotransport properties and electronic structure of LaBi, isostructural to LaSb. LaBi exhibits large MR as in LaSb, which can be ascribed to the nearly compensated electron and hole with rather high mobilities. More importantly, our analysis suggests that the XMR as well as field-induced resistivity upturn and plateau observed in LaSb and LaBi can be well explained by the two-band model with the compensation situation. We present the critical conditions leading to these field-induced properties. It will contribute to the understanding of the XMR phenomenon and explore novel XMR materials.
Lithium–sulfur (Li–S) batteries deliver a high theoretical energy density of 2600 Wh kg−1, and hold great promise to serve as a next‐generation high‐energy‐density battery system. Great progress has ...been achieved in cathode design to deal with the intrinsic problems of sulfur cathodes, including low conductivity, the dissolution of polysulfide intermediate, and volume fluctuation. However, aiming at the practical applications of Li–S batteries, the weight percentage of sulfur in cathode materials and the overall areal sulfur loading need to be significantly increased, which inevitably complicate the process and cause heavy shuttle effect, slow redox kinetics, and more undesirable reaction pathways. Recently, rationally designing efficient mediators, as well as incorporating them into a working battery, emerges to be a promising method to construct high‐energy‐density Li–S batteries. The influence of mediators on Li–S batteries appears to be the enhancement in redox kinetics and the increase in reaction efficiency. In this feature article, the mechanistic understanding of redox kinetics in Li–S reactions is discussed, and then a comprehensive analysis of the recent advances in both heterogeneous and homogeneous mediator design is provided. A mediator perspective in building high‐energy‐density Li–S batteries is also included.
Mediators in lithium–sulfur batteries can enhance the redox kinetics and increase the reaction efficiency, which benefit the practical applications requiring a high sulfur content and a high areal loading amount. This feature article discusses the mechanism of redox kinetics, and reviews the recent advances in heterogeneous/homogeneous mediator design in lithium–sulfur batteries.
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Porous materials capable of selectively capturing CO2 from flue‐gases or natural gas are of interest in terms of rising atmospheric CO2 levels and methane purification. Size‐exclusive sieving of CO2 ...over CH4 and N2 has rarely been achieved. Herein we show that a crystal engineering approach to tuning of pore‐size in a coordination network, Cu(quinoline‐5‐carboxyate)2n (Qc‐5‐Cu) ena+bles ultra‐high selectivity for CO2 over N2 (SCN≈40 000) and CH4 (SCM≈3300). Qc‐5‐Cu‐sql‐β, a narrow pore polymorph of the square lattice (sql) coordination network Qc‐5‐Cu‐sql‐α, adsorbs CO2 while excluding both CH4 and N2. Experimental measurements and molecular modeling validate and explain the performance. Qc‐5‐Cu‐sql‐β is stable to moisture and its separation performance is unaffected by humidity.
Sieves you right: Crystal engineering of supramolecular isomers of Cu(quinoline‐5‐carboxyate)2n metal–organic materials enables the right pore‐chemistry for ultra‐high CO2/N2 and CO2/CH4 selectivity even in the presence of water vapor.
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Flexible energy storage systems are imperative for emerging flexible devices that are revolutionizing our life. Lithium-ion batteries, the current main power sources, are gradually approaching their ...theoretical limitation in terms of energy density. Therefore, alternative battery chemistries are urgently required for next-generation flexible power sources with high energy densities, low cost, and inherent safety. Flexible lithium-sulfur (Li-S) batteries and analogous flexible alkali metal-chalcogen batteries are of paramount interest owing to their high energy densities endowed by multielectron chemistry. In this review, we summarized the recent progress of flexible Li-S and analogous batteries. A brief introduction to flexible energy storage systems and general Li-S batteries has been provided first. Progress in flexible materials for flexible Li-S batteries are reviewed subsequently, with a detailed classification of flexible sulfur cathodes as those based on carbonaceous (
e.g.
, carbon nanotubes, graphene, and carbonized polymers) and composite (polymers and inorganics) materials and an overview of flexible lithium anodes and flexible solid-state electrolytes. Advancements in other flexible alkali metal-chalcogen batteries are then introduced. In the next part, we emphasize the importance of cell packaging and flexibility evaluation, and two special flexible battery prototypes of foldable and cable-type Li-S batteries are highlighted. In the end, existing challenges and future development of flexible Li-S and analogous alkali metal-chalcogen batteries are summarized and prospected.
This review summarizes recent progress in flexible Li-S and analogous alkali metal-chalcogen batteries, including flexible chalcogen cathodes, flexible alkali metal anodes, flexible solid-state electrolytes, and flexible battery prototypes.
Lithium–sulfur (Li–S) batteries hold great promise to serve as next‐generation energy storage devices. However, the practical performances of Li–S batteries are severely limited by the sulfur cathode ...regarding its low conductivity, huge volume change, and the polysulfide shuttle effect. The first two issues have been well addressed by introducing mesoporous carbon hosts to the sulfur cathode. Unfortunately, the nonpolar nature of carbon materials renders poor affinity to polar polysulfides, leaving the shuttling issue unaddressed. In this contribution, atomic cobalt is implanted within the skeleton of mesoporous carbon via a supramolecular self‐templating strategy, which simultaneously improves the interaction with polysulfides and maintains the mesoporous structure. Moreover, the atomic cobalt dopants serve as active sites to improve the kinetics of the sulfur redox reactions. With the atomic‐cobalt‐decorated mesoporous carbon host, a high capacity of 1130 mAh gS−1 at 0.5 C and a high stability with a retention of 74.1% after 300 cycles are realized. Implanting atomic metal in mesoporous carbon demonstrates a feasible strategy to endow nanomaterials with targeted functions for Li–S batteries and broad applications.
Atomic cobalt implantation to mesoporous carbon enhances the sulfur kinetics in Li–S batteries. Atomic cobalt dopants with high polarity endow the mesoporous carbon (represented by the apes) with high affinity with polysulfides (represented by the bananas). Therefore, the shuttle effect is eliminated and the sulfur kinetics is improved, facilitating highly stable Li–S batteries.
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Rechargeable lithium–sulfur batteries have attracted tremendous scientific attention owing to their superior energy density. However, the sulfur electrochemistry involves multielectron redox ...reactions and complicated phase transformations, while the final morphology of solid‐phase Li2S precipitates largely dominate the battery's performance. Herein, a triple‐phase interface among electrolyte/CoSe2/G is proposed to afford strong chemisorption, high electrical conductivity, and superb electrocatalysis of polysulfide redox reactions in a working lithium–sulfur battery. The triple‐phase interface effectively enhances the kinetic behaviors of soluble lithium polysulfides and regulates the uniform nucleation and controllable growth of solid Li2S precipitates at large current density. Therefore, the cell with the CoSe2/G functional separator delivers an ultrahigh rate cycle at 6.0 C with an initial capacity of 916 mAh g−1 and a capacity retention of 459 mAh g−1 after 500 cycles, and a stable operation of high sulfur loading electrode (2.69–4.35 mg cm−2). This work opens up a new insight into the energy chemistry at interfaces to rationally regulate the electrochemical redox reactions, and also inspires the exploration of related energy storage and conversion systems based on multielectron redox reactions.
A unique triple‐phase interface with synergistic properties of strong chemisorption, large electrical conductivity, and highly active electrocatalysis sites is proposed, which can effectively regulate the electrochemical redox reaction of soluble lithium polysulfides and tune Li2S nucleation and growth, enabling controllable Li2S precipitates on reactive interfaces at high current rates in a working Li–S battery.
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