Enhanced interfacial compatibility of FeS@N,S-C anode with ester-based electrolyte enables stable sodium-ion full cells

The development of sodium-ion full cells is seriously suppressed by the incompatibility between electrodes and electrolytes. Most representatively, high-voltage ester-based electrolytes required by the cathodes present poor interfacial compatibility with the anodes due to unstable solid electrode interphase(SEI). Herein, Fe S@N,S-C(spindle-like Fe S nanoparticles individually encapsulated in N,S-doped carbon) with excellent structural stability is synthesized as a potential sodium anode material. It exhibits exceptional interfacial stability in ester-based electrolyte(1 M NaClO_(4) in ethylene carbonate/propylene carbonate with 5% fluoroethylene carbonate) with long-cycling lifespan(294 days) in Na|Fe S@N,S-C coin cell and remarkable cyclability in pouch cell(capacity retention of 82.2% after 170 cycles at 0.2 A g^(-1)).DFT calculation reveals that N,S-doping on electrode surface could drive strong repulsion to solvated Na_(2) and preferential adsorption to ClO_(4)^(-) anion, guiding the anion-rich inner Helmholtz plane.Consequently, a robust SEI with rich inorganic species(NaCl and Na_(2)O) through the whole depth stabilizes the electrode–electrolyte interface and protects its integrity. This work brings new insight into the role of electrode’s surface properties in interfacial compatibility that can guide the design of more versatile electrodes for advanced rechargeable metal-ion batteries.

Thermally Conductive Polyimide/Boron Nitride Composite Films with Improved Interfacial Compatibility Based on Modified Fillers by Polyimide Brushes

Polyimide-based composite films with high thermal conductivity,good mechanical property and electrical insulating performance are urgently needed in the electronics and microelectronics fields.As one of the key technical challenges to be solved,interfacial compatibility between filler and matrix plays an important role for composite film.Herein,boron nitride was modified by grafting polyimide brushes via a twostep method,and a series of thermally conductive polyimide/boron nitride composite films were prepared.Both characterization and performance results proved that the interfacial interaction and compatibility was greatly enhanced,resulting in a significant reduction in defects and interfacial thermal resistance.The interphase width of transition zone between two phases was also efficiently enlarged due to polyimide brushes grafted on filler surface.As a result,composite films based on polyimide-grafted boron nitride exhibited significantly improved properties compared with those based on pristine filler.Tensile strength can reach up to 80 MPa even if the filler content is as high as 50 wt%.The out-of-plane and in-plane thermal conductivity of composite film increased to 0.841 and 0.850 W·m^(-1)·K^(-1),respectively.In addition,thermal and dielectric properties of composite films were also enhanced to some extent.The above results indicate that surface modification by chemically grafting polymer brushes is an effective method to improve two-phase interfacial compatibility so as to prepare composite film with enhanced properties.

Interfacial compatibility issues in rechargeable solid-state lithium metal batteries:a review

Solid-state lithium metal batteries(SSLBs)contain various kinds of interfaces,among which the solid electrode|solid electrolyte(ED|SE)interface plays a decisive role in the battery's power density and cycling stability.However,it is still lack of comprehensive knowledge and understanding about various interfacial physical/chemical processes so far.Although tremendous efforts have been dedicated to investigate the origin of large interfacial resistance and sluggish charge(electron/ion)transfer process,many scientific and technological challenges still remain to be clarified.In this review,we detach and discuss the critical individual challenge,including charge transfer process,chemical and electrochemical instability,space charge layers,physical contact and mechanical instability.The fundamental concepts,individual effects on the charge transfer and potential solutions are summarized based on material's thermodynamics,electrode kinetics and mechanical effects.It is anticipated that future research should focus on quantitative analysis,modeling analysis and in-situ microstructure characterizations in order to obtain an efficient manipulation about the complex interfacial behaviors in all solid-state Li batteries.

Improved dispersion performance and interfacial compatibility of covalent-grafted MOFs in mixed-matrix membranes for gas separation

Mixed-matrix membranes(MMMs)have received much attention due to their processable advantages of polymer and high permeability and/or selectivity of porous metal-organic frameworks(MOFs)fillers.However,the interfacial defects caused by poor interaction between MOFs with polymers and the agglomeration phenomenon caused by uneven dispersion of MOFs are common problems in mixed-matrix membranes.Currently,the priming protocol is one of solutions to the above problems,but it cannot precisely regulate the dispersion of particles and the interfacial compatibility between two phases.Herein,covalent grafting of polyimide 6FDA-Durene onto the surface of UiO-66-NH2 can mitigate the aggregation of fillers inside the polymeric matrices and improve the interfacial interaction between two phases,thus significantly improving the CO_(2)/CH_(4)separation performance on the as-synthesized MMMs.The explored gas transport mechanism indicated that the improved separation was due to the raise of solubility selectivity.Furthermore,the stronger covalent bond between fillers and polyimide than physical interaction of priming protocol also endows the improved anti-plasticization phenomenon for CO_(2)/CH_(4)separation.

Rational Design of High-Performance PEO/Ceramic Composite Solid Electrolytes for Lithium Metal Batteries

Composite solid electrolytes(CSEs)with poly(ethylene oxide)(PEO)have become fairly prevalent for fabricating high-performance solid-state lithium metal batteries due to their high Li~+solvating capability,flexible processability and low cost.However,unsatisfactory room-temperature ionic conductivity,weak interfacial compatibility and uncontrollable Li dendrite growth seriously hinder their progress.Enormous efforts have been devoted to combining PEO with ceramics either as fillers or major matrix with the rational design of two-phase architecture,spatial distribution and content,which is anticipated to hold the key to increasing ionic conductivity and resolving interfacial compatibility within CSEs and between CSEs/electrodes.Unfortunately,a comprehensive review exclusively discussing the design,preparation and application of PEO/ceramic-based CSEs is largely lacking,in spite of tremendous reviews dealing with a broad spectrum of polymers and ceramics.Consequently,this review targets recent advances in PEO/ceramicbased CSEs,starting with a brief introduction,followed by their ionic conduction mechanism,preparation methods,and then an emphasis on resolving ionic conductivity and interfacial compatibility.Afterward,their applications in solid-state lithium metal batteries with transition metal oxides and sulfur cathodes are summarized.Finally,a summary and outlook on existing challenges and future research directions are proposed.

用于气体分离的含多孔材料的混合基质膜--从金属有机框架到离散分子笼

混合基质膜(MMMs)将多孔材料与聚合物基质相结合,因其互补特性和协同激活已经在气体分离领域引起了相当大的研究兴趣。多孔材料的可塑性和多样性赋予MMMs可延伸的功能和出色的分离性能。为了发挥MMMs的全部潜力,研究人员关注多孔填料与聚合物基质的合理匹配,以实现这些材料之间界面的增强相容性。在本文中,我们重点介绍采用不同策略将金属-有机框架(MOFs)和金属-有机笼(MOCs)与聚合物基质相结合制备MMMs的最新进展。文中进一步讨论未来MMMs发展所面临的机遇和挑战,并旨在通过合理的材料设计和选择推动MMMs的制备。

A leap by the rise of solid-state electrolytes for Li-air batteries

Li-air batteries have attracted extensive attention because of their ultrahigh theoretical energy density. However, the potential safety hazard of flammable organic liquid electrolytes hinders their practical applications. Replacing liquid electrolytes with solidstate electrolytes(SSEs) is expected to fundamentally overcome the safety issues. In this work, we focus on the development and challenge of solid-state Li-air batteries(SSLABs). The rise of different types of SSEs, interfacial compatibility and verifiability in SSLABs are presented. The corresponding strategies and prospects of SSLABs are also proposed. In particular, combining machine learning method with experiment and in situ(or operando)techniques is imperative to accelerate the development of SSLABs.

Practical development and challenges of garnet-structured Li_(7)La_(3)Zr_(2)O_(12) electrolytes for all-solid-state lithium-ion batteries:A review

All-solid-state Li-ion batteries(ASSLIBs)have been widely studied to achieve Li-ion batteries(LIBs)with high safety and energy density.Recent reviews and experimental papers have focused on methods that improve the ionic conductivity,stabilize the electrochemical performance,and enhance the electrolyte/electrode interfacial compatibility of several solid-state electrolytes(SSEs),including oxides,sulfides,composite and gel electrolytes,and so on.Garnet-structured Li_(7)La_(3)Zr_(2)O_(12)(LLZO)is highly regarded an SSE with excellent application potential.However,this type of electrolyte also possesses a number of disadvantages,such as low ionic conductivity,unstable cubic phase,and poor interfacial compatibility with anodes/cathodes.The benefits of LLZO have urged many researchers to explore effective solutions to overcome its inherent limitations.Herein,we review recent developments on garnet-structured LLZO and provide comprehensive insights to guide the development of garnet-structured LLZO-type electrolytes.We not only systematically and comprehensively discuss the preparation,element doping,structure,stability,and interfacial improvement of LLZOs but also provide future perspectives for these materials.This review expands the current understanding on advanced solid garnet electrolytes and provides meaningful guidance for the commercialization of ASSLIBs.

Challenges and prospects for room temperature solid-state sodiumsulfur batteries

Room temperature sodium-sulfur(Na-S)batteries,known for their high energy density and low cost,are one of the most promising next-generation energy storage systems.However,the polysulfide shuttling and uncontrollable Na dendrite growth as well as safety issues caused by the use of organic liquid electrolytes in Na-S cells,have severely hindered their commercialization.Solid-state electrolytes instead of liquid electrolytes are considered to be the most direct and effective solution to solve the above problems.However,its practical application is still greatly challenged due to the poor interfacial compatibility between the all-solid-state electrolytes and the anode/cathode,ionic conductivity,and the shuttle effect caused by the presence of liquid phase in the quasi-solid-state electrolytes.This paper presents a comprehensive review of solid-state Na-S batteries from the perspective of regulating interfacial compatibility and improving ionic conductivity as well as suppressing polysulfide shuttle.According to different components,solid-state electrolytes were divided into five categories:solid inorganic electrolytes,solid polymer electrolytes,polymer/inorganic solid hybrid electrolytes,gel polymer electrolytes,and liquid–solid inorganic hybrid electrolytes.Finally,the prospect of developing high performance solid-state electrolytes to improve the cycling stability of room temperature Na-S cells is envisaged.

An artificial interphase enables stable PVDF-based solid-state Li metal batteries

Composite polymer electrolytes(CPEs)have attracted much attention for high energy density solid-state lithium-metal batteries owing to their flexibility,low cost,and easy scale-up.However,the unstable Li/CPE interface is always challengeable for the practical utilization of CPEs.Herein,a polymer interlayer containing K+prepared by ultraviolet(UV)-curing precursor solution is coated on Li surface to stabilize the interface between poly(vinylidene difluoride)(PVDF)composite electrolytes and Li anode.Benefiting from the physical barrier of the interlayer,the continuous decomposition of PVDF is restrained and the intimate contact between electrode and electrolyte is also achieved to reduce the interface impedance.Moreover,the added K+is utilized to further regulate smooth Li deposition.As a consequence,the symmetric Li|Li cell with coated Li demonstrates steady cycling at 0.4 mAh·cm^(-2) and a high critical current density of 1 mA·cm^(-2).The assembled Li|LiFePO_(4) cell presents outstanding cycling stability(capacity retention of 90%after 400 cycles at 1 C)and good rate performance.The associated pouch cell performs impressive flexibility and safety.This work provides a convenient strategy to achieve stable Li/PVDF interface for high-performance PVDF-based solid state Li metal batteries.

ZIF-8-functionalized polymer electrolyte with enhanced performance for high-temperature solid-state lithium metal batteries

Solid polymer electrolytes(SPEs)with high ionic conductivity are desirable for solid-state lithium metal batteries(SSLMBs)to achieve enhanced safety and energy density.Incorporating nanofillers into a polymeric matrix to develop nanocomposite solid electrolytes(NCSEs)has become a promising method for improving the ionic conductivity of the SPEs.Here,a novel ZIF-8-functionalized NCSE was prepared for high-temperature S SLMB s using an in situ radical polymerization method.It is found that the ZIF-8 nanoparticles could reduce the crystallinity of polymer segments and offer a Lewis acid surface that promotes the dissociation of lithium bis(trifluoromethanesulfonyl)imide(LiTFSI)and stabilizes the TFSI^(-) anion movement.Thus,the as-prepared NCSE exhibits an outstanding ionic conductivity of 1.63×10^(-3)S·cm^(-1),an electrochem ical stability window of 5.0 V at 80℃,and excellent interface compatibility with lithium metal anode with a stable polarization over 2000 h.Furthermore,the assembled SSLMBs with LiFePO_(4)cathode show dendrite-free Li-metal surface,good rate capability,and stable cycling stability with a capacity retention of 70%over 1000 cycles at a high temperature of 80℃.This work provides valuable insights into promoting the ionic conductivity of SPEs.

Electrolyte design for rechargeable anion shuttle batteries

As an emerging new type of battery chemistry,the anion shuttle battery(ASB),based on the shuttling and storage of anions,is considered a sustainable alternative to gigawatt-scale energy storage due to the associated resource abundance,low cost,high safety,and high energy density.Although significant progress has been achieved,practical applications of ASBs are still hindered by tough challenges,such as short lifetime,limited reversible capacity,and low Coulombic efficiency.Therefore,it is very necessary to design and explore new electrolyte systems with high electrochemical/chemical stability,sufficient compatibility towards electrodes,and excellent kinetics/reversibility for anion electrochemical reactions.Here,we review the recent achievements and main challenges in developing electrolytes for ASBs,which include solid,non-aqueous,and aqueous electrolytes.We mainly focus on the unique properties and basic principles of designing these electrolytes,and their various performance parameters.Perspectives on design strategies for ASB electrolytes are also presented,which could facilitate the development of advanced ASBs for grid-scale energy storage.