The electrolyte comprising more robust water and superhalides transforms Zn-metal anode reversibly and dendrite-free

A great challenge for all aqueous batteries,including Zn-metal batteries,is the parasitic hydrogen evolution reaction on the low-potential anode.Herein,we report the formula of a highly concentrated aqueous electrolyte that mitigates hydrogen evolution by transforming water molecules more inert.The electrolyte comprises primarily ZnCl_(2) and LiCl as an additive,both of which are inexpensive salts.The O-H covalent bonds in water get strengthened in a chemical environment that has fewer hydrogen bonding interactions and a greater number of Zn-Cl superhalides,as suggested by integrated characterization and simulation.As a result,the average Coulombic efficiency of zincmetal anode is raised to an unprecedented>99.7%at 1mA cm^(−2).In the new electrolyte,the plating/stripping processes leave the zinc-metal anode dendrite-free,and the zinc-metal anode delivers stable plating/stripping cycles for 4000 hours with an areal capacity of 4 mAh cm^(−2) at 2mA cm^(−2).Furthermore,the high Coulombic efficiency of zinc-metal anode in the ZnCl_(2)-LiCl mixture electrolyte is demonstrated in full cells with a limited anode.The V_(2)O_(5)·H_(2)O||Zn full cell with an N/P mass ratio of 1.2 delivers a stable life of more than 2500 cycles,and the LiMn_(2)O_(4)||Zn hybrid cell with an N/P mass ratio of 0.6 exhibits 1500 cycles in its stable life.

ZnS coating of cathode facilitates lean‐electrolyte Li‐S batteries

Tremendous effort has been devoted to lithium‐sulfur batteries,where flooded electrolytes have been employed ubiquitously.The use of lean electrolytes albeit indispensable for practical applications often causes low capacity and fast capacity fading of the sulfur cathode;thus,the electrolyte/sulfur active mass ratios below 5μL/mg have been rarely reported.Herein,we demonstrate that ZnS coating transforms sulfur cathode materials electrolyte‐philic,which tremendously promotes the performance in lean electrolytes.The ZnS‐coated Li2S@graphene cathode delivers an initial discharge capacity of 944mAh/g at an E/S ratio of 2μL/mg at the active mass loading of 5.0 mg Li2S/cm^2,corresponding to an impressive specific energy of 500Wh/kg based on the mass of cathode,electrolyte,and the assumed minimal mass of lithium metal anode.Density functional theory calculations reveal strong binding between ZnS crystals and electrolyte solvent molecules,explaining the better wetting properties.We also demonstrate the reversible cycling of a hybrid cathode of ZnS‐coated Li2S@graphene mixed with VS2 as an additive at an E/AM(active mass)ratio of 1.1μL/mg,equivalent to the specific energy of 432 Wh/kg on the basis of the mass of electrodes and electrolyte.

A review of halide charge carriers for rocking-chair and dual-ion batteries

This review discusses how halide ion species have been used as charge carriers in both anion rocking-chair and dual-ion battery(DIB)systems.The anion rocking-chair batteries based on fluoride and chloride have emerged over the past decade and are garnering increased research interest due to their large theoretical energy density values and the natural abundance of halide-containing materials.Moreover,DIBs that use halide species as their anionic charge carrier are seen as one of the promising next-generation battery technologies due to their low cost and high working potentials.Although numerous polyatomic anions have been studied as charge carriers,the use of single halide ions(i.e.,F−and Cl−)and metal-based superhalides(e.g.,[MgCl_(3)]−)as anionic charge carriers in DIBs has been considerably less explored.Herein,we provide an overview of some of the key advances and recent progress that has been made with regard to halide ion charge carriers in electrochemical energy storage.We offer our perspectives on the current state of the field and provide a roadmap in hopes that it helps researchers toward making new advances in these promising and emerging areas.

Counter-ion insertion of chloride in Mn3O4 as cathode for dual-ion batteries: A new mechanism of electrosynthesis for reversible anion storage

Irreversible reductive insertion of Zn2+transforms Mn3O4 such that the resulting Zn0.2Mn3O4 exhibits highly reversible storage properties of chloride ions,thus rendering Zn0.2Mn3O4 an excellent cathode of aqueous dual-ion batteries.With Zn2+trapped,Zn0.2Mn3O4 delivers the chloride-storage capacity over 200 mAh/g at an average potential of 1.6 V vs Zn2+/Zn by reversibly forming a new ionic compound equivalent to Zn0.2Mn3O4Cl1.7.Electrochemical quartz crystal microbalance results suggest chloride as the primary charge carrier in the reversible oxidative anion insertion.The Mn3O4 anion-hosting cathode couples with Zn metal anode in a full-cell dual-ion battery,demonstrating stable cycling in practical pouch cells with an energy density of 150 Wh/kg based on the mass of both electrodes.

Electrocatalytic and stoichiometric reactivity of 2D layered siloxene for high-energy-dense lithium-sulfur batteries

Lithium-sulfur batteries(LSBs)have emerged as promising power sources for high-performance devices such as electric vehicles.However,the poor energy density of LSBs owing to polysulfide shuttling and passivation has limited their further market penetration.To mitigate this challenge,two-dimensional(2D)siloxene(2DSi),a Si-based analog of graphene,is utilized as an additive for sulfur cathodes.The 2DSi is fabricated on a large scale by simple solvent extraction of calcium disilicide to form a thin-layered structure of Si planes functionalized with vertically aligned hydroxyl groups in the 2DSi.The stoichiometric reaction of 2DSi with polysulfides generates a thiosulfate redox mediator,secures the intercalation pathway,and reveals Lewis acidic sites within the siloxene galleries.The 2DSi utilizes the corresponding in-situ-formed electrocatalyst,the 2D confinement effect of the layered structure,and the surface affinity based on Lewis acid-base interaction to improve the energy density of 2DSi-based LSB cells.Combined with the commercial carbon-based current collector,2DSi-based LSB cells achieve a volumetric energy density of 612 Wh Lcell^(−1) at 1 mA cm^(−2) with minor degradation of 0.17%per cycle,which rivals those of state-of-the-art LSBs.This study presents a method for the industrial production of high-energy-dense LSBs.

Burning magnesium in carbon dioxide for highly effective phosphate removal

Magnesium oxide was found to have high-phosphate-affinity as an effective component to enhance the phosphate removal ability of common adsorbent materials.However,the currently prepared MgO-based hybrid adsorbents by conventional methods still suffer from the limited low loading of MgO and inferior removal performances,much far away from practical application.In this study,an ingenious carbon coated MgO nanocomposite is designed by directly burning magnesium in CO_(2),a well-known textbook reaction.X-ray diffraction analysis,scanning electron microscope and aberration-corrected high-resolution transmission electron microscope demonstrate the sample is well prepared.Consequently,the high content of nanosized MgO combined with defect-rich carbon layer brings unprecedented phosphate removal capacity of 1135.0 mg/g,removal rate of 99% and benign compatibility with coexisting anions and solution pH.Furthermore,the removal mechanism is also investigated in detail by characterizing the sample before and after adsorption.

Carbon energy: A multidisciplinary exploration of energy technologies and carbon materials science

Today’s world is stressed by the ever-increasing demand for energy and the disastrous climate changes.New technologies that generate,convert,and store energy in a greener and more efficient way become increasingly critical in building a sustainable society.On this front,batteries,capacitors,fuel cells,and solar cells play the indispensable roles as the powers for applications,for example,electric vehicles shall mitigate our reliance on the depleting fossil fuels.It is crucial to invent new materials or technologies to improve the electrochemical performance of energy storage/conversion devices with higher energy,better power,longer cycle life,and better safety.One of the most important areas pertains to carbon-based materials.Researchers from different fields design carbon-based materials for low-cost energy devices with great portability and functionality.

A perspective of ZnCl_(2)electrolytes:The physical and electrochemical properties

Molten ZnCl_(2)hydrates are ionic liquids at room temperature,which exhibit intriguing physical and electrochemical properties.Continuous efforts have been devoted over several decades to understanding the properties of the molten ZnCl_(2)hydrates that have been dubbed as water-in-salt electrolytes recently.The physical properties of molten ZnCl_(2)hydrates can be described from the perspectives of ions in their speciation and water molecules regarding their chemical environments.Recently,attention has been given to molten ZnCl_(2)hydrates as electrolytes for Zn metal batteries.It was revealed that the physical properties of such electrolytes have rich implications in their electrochemical properties.Therefore,it demands a holistic understanding of the physical and electrochemical properties of molten ZnCl_(2)hydrates to design functional electrolytes to serve high-performing Zn metal batteries.This perspective attempts to review the works that described the properties of concentrated ZnCl_(2)as an ionic liquid and as an emerging electrolyte.The author also provides a perspective to highlight the needs of future research to circumvent the limits of this electrolyte.

Prussian Blue Analogues as Electrodes for Aqueous Monovalent Ion Batteries

Aqueous batteries have engendered increasing attention as promising solutions for stationary energy storage due to their potentially low cost and innate safety.In various aqueous battery systems,Prussian blue analogues(PBAs)represent a class of promising electrode materials with fascinating electrochemical performance,owing to their large open frameworks,abundant ion insertion sites,and facile preparation.To date,PBAs have shown substantial progress towards storage of alkali metal ions(Li^(+),Na^(+),and K^(+)),H^(+),and NH4^(+) in aqueous electrolytes,which,however,has yet not been specifically summarized.This review selects some representative research to introduce the progress of PBAs in these battery systems and aims to discuss the crucial role of ionic charge carrier in affecting the overall electrode performance.Besides,some critical knowledge gaps and challenges of PBA materials have been pointed out for future development.

Improved flexible Li-ion hybrid capacitors： Techniques for superior stability

Flexible power devices play an increasingly crucial role in emerging flexible electronics. To improve the electrochemical performance of flexible power devices, novel electrode structures and new energy-storage systems should be designed. Herein, a novel flexible Li-ion hybrid capacitor （LIC） is designed based on an anode comprising Li4TisO12 nanoplate arrays coated on carbon textile （LTO/CT） and a cathode comprising a flexible N-doped graphene/carbon-nanotube composite （NGC） film. The LTO/CT anode is fabricated by directly growing Li4TisO12 nano- plates on CT with robust adhesion using a simple one-pot hydrothermal reaction. Considering the volume of a real-device flexible LIC, the NGC//LTO/CT con- figuration delivers high volumetric energy and power densities of 2 mWh·cm-3 and 185 mW·cm-3, respectively. Furthermore, the flexible LIC shows excellent flexibility and electrochemical stability, with extremely small capacity fluctuation under different bending states. This work demonstrates a scalable route to assemble flexible LICs as high-performance power devices.