Better living through water-splitting Chemists have known how to use electricity to split water into hydrogen and oxygen for more than 200 years. Nonetheless, because the electrochemical route is inefficient, most of the hydrogen made nowadays comes from natural gas. Seh et al. review recent progress in electrocatalyst development to accelerate water-splitting, the reverse reactions that underlie fuel cells, and related oxygen, nitrogen, and carbon dioxide reductions. A unified theoretical framework highlights the need for catalyst design strategies that selectively stabilize distinct reaction intermediates relative to each other. Science , this issue p. 10.1126/science.aad4998
Due to their high energy density and low material cost, lithium-sulfur batteries represent a promising energy storage system for a multitude of emerging applications, ranging from stationary grid storage to mobile electric vehicles. This review aims to summarize major developments in the field of lithium-sulfur batteries, starting from an overview of their electrochemistry, technical challenges and potential solutions, along with some theoretical calculation results to advance our understanding of the material interactions involved. Next, we examine the most extensively-used design strategy: encapsulation of sulfur cathodes in carbon host materials. Other emerging host materials, such as polymeric and inorganic materials, are discussed as well. This is followed by a survey of novel battery configurations, including the use of lithium sulfide cathodes and lithium polysulfide catholytes, as well as recent burgeoning efforts in the modification of separators and protection of lithium metal anodes. Finally, we conclude with an outlook section to offer some insight on the future directions and prospects of lithium-sulfur batteries.
Polysulfide binding and trapping to prevent dissolution into the electrolyte by a variety of materials has been well studied in Li−S batteries. Here we discover that some of those materials can play an important role as an activation catalyst to facilitate oxidation of the discharge product, Li 2 S, back to the charge product, sulfur. Combining theoretical calculations and experimental design, we select a series of metal sulfides as a model system to identify the key parameters in determining the energy barrier for Li 2 S oxidation and polysulfide adsorption. We demonstrate that the Li 2 S decomposition energy barrier is associated with the binding between isolated Li ions and the sulfur in sulfides; this is the main reason that sulfide materials can induce lower overpotential compared with commonly used carbon materials. Fundamental understanding of this reaction process is a crucial step toward rational design and screening of materials to achieve high reversible capacity and long cycle life in Li−S batteries. T he ever-increasing demand for energy storage devices with high energy density, low material cost, and long cycle life has driven the development of new battery systems beyond the currently dominant lithium ion batteries (LIBs) (1). Among alternative battery chemistries, lithium−sulfur (Li−S) batteries have attracted remarkable attention due to their high theoretical energy density of 2,600 watt hours per kilogram, 5 times higher than those of state-of-the-art LIBs (2-4). In addition, sulfur, as a byproduct of the petroleum refining process, is naturally abundant, inexpensive, and environmentally friendly (5). However, the practical application of Li−S batteries is still plagued with numerous challenges. For example, the insulating nature of sulfur and discharge products Li 2 S/Li 2 S 2 leads to low active material utilization. In addition, the easy dissolution of lithium polysulfides (LiPSs) into the electrolyte causes LiPSs shuttling between cathode and anode and uncontrollable deposition of sulfide species on the lithium metal anode, inducing fast capacity fading and low coulombic efficiency (2, 6).Tremendous efforts have been taken to circumvent these concerns, with the nanostructuring of electrodes as one of the most effective approaches to overcoming the issues facing highcapacity electrode materials (2, 7). For example, the integration of nanostructured carbon materials with sulfur is one of the primary strategies for improving the electrical conductivity of the composites and suppression of polysulfide shuttling through physical confinement (8-14). However, it was first recognized by Zheng et al. (11) that the weak interaction between nonpolar carbon-based materials and polar LiPSs/Li 2 S species leads to weak confinement and easy detachment of LiPSs from the carbon surface, with further diffusion into the electrolyte causing capacity decay and poor rate performance. Therefore, the introduction of heteroatoms into carbonaceous materials (such as nitrogen, oxygen, boron, phosphorous, sulfur, or ...
Owing to its low cost and high natural abundance, sodium metal is among the most promising anode materials for energy storage technologies beyond lithium ion batteries. However, room-temperature sodium metal anodes suffer from poor reversibility during long-term plating and stripping, mainly due to formation of nonuniform solid electrolyte interphase as well as dendritic growth of sodium metal. Herein we report for the first time that a simple liquid electrolyte, sodium hexafluorophosphate in glymes (mono-, di-, and tetraglyme), can enable highly reversible and nondendritic plating–stripping of sodium metal anodes at room temperature. High average Coulombic efficiencies of 99.9% were achieved over 300 plating–stripping cycles at 0.5 mA cm–2. The long-term reversibility was found to arise from the formation of a uniform, inorganic solid electrolyte interphase made of sodium oxide and sodium fluoride, which is highly impermeable to electrolyte solvent and conducive to nondendritic growth. As a proof of concept, we also demonstrate a room-temperature sodium–sulfur battery using this class of electrolytes, paving the way for the development of next-generation, sodium-based energy storage technologies.
The hydrogen evolution reaction (HER) is an important energy conversion process that underpins many clean energy technologies including water splitting. Herein, we report for the first time the application of two-dimensional (2D) layered transition metal carbides, MXenes, as electrocatalysts for the HER. Our computational screening study of 2D layered M 2 XT x (M = metal; X = (C, N); and T x = surface functional groups) predicts Mo 2 CT x to be an active catalyst candidate for the HER. We synthesized both Mo 2 CT x and Ti 2 CT x MXenes, and in agreement with our theoretical predictions, Mo 2 CT x was found to exhibit far higher HER activity than Ti 2 CT x . Theory suggests that the basal planes of Mo 2 CT x are catalytically active toward the HER, unlike in the case of widely studied MoS 2 , in which only the edge sites of the 2H phase are active. This work paves the way for the development of novel 2D layered materials that can be applied in a multitude of other clean energy reactions for a sustainable energy future.
Lithium–sulfur batteries have attracted attention due to their six-fold specific energy compared with conventional lithium-ion batteries. Dissolution of lithium polysulfides, volume expansion of sulfur and uncontrollable deposition of lithium sulfide are three of the main challenges for this technology. State-of-the-art sulfur cathodes based on metal-oxide nanostructures can suppress the shuttle-effect and enable controlled lithium sulfide deposition. However, a clear mechanistic understanding and corresponding selection criteria for the oxides are still lacking. Herein, various nonconductive metal-oxide nanoparticle-decorated carbon flakes are synthesized via a facile biotemplating method. The cathodes based on magnesium oxide, cerium oxide and lanthanum oxide show enhanced cycling performance. Adsorption experiments and theoretical calculations reveal that polysulfide capture by the oxides is via monolayered chemisorption. Moreover, we show that better surface diffusion leads to higher deposition efficiency of sulfide species on electrodes. Hence, oxide selection is proposed to balance optimization between sulfide-adsorption and diffusion on the oxides.
Although the rechargeable lithium-sulfur battery system has attracted significant attention due to its high theoretical specific energy, its implementation has been impeded by multiple challenges, especially the dissolution of intermediate lithium polysulfide (Li2Sn) species into the electrolyte. Introducing anchoring materials, which can induce strong binding interaction with Li2Sn species, has been demonstrated as an effective way to overcome this problem and achieve long-term cycling stability and high-rate performance. The interaction between Li2Sn species and anchoring materials should be studied at the atomic level in order to understand the mechanism behind the anchoring effect and to identify ideal anchoring materials to further improve the performance of Li-S batteries. Using first-principles approach with van der Waals interaction included, we systematically investigate the adsorption of Li2Sn species on various two-dimensional layered materials (oxides, sulfides, and chlorides) and study the detailed interaction and electronic structure, including binding strength, configuration distortion, and charge transfer. We gain insight into how van der Waals interaction and chemical binding contribute to the adsorption of Li2Sn species for anchoring materials with strong, medium, and weak interactions. We understand why the anchoring materials can avoid the detachment of Li2S as in carbon substrate, and we discover that too strong binding strength can cause decomposition of Li2Sn species.
The first use of non-centrosymmetric Janus Au-TiO(2) photocatalysts in efficient, plasmon-enhanced visible-light hydrogen generation is demonstrated. The intense localization of plasmonic near-fields close to the Au-TiO(2) interface, coupled with optical transitions involving localized electronic states in amorphous TiO(2) brings about enhanced optical absorption and the generation of electron-hole pairs for photocatalysis.
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