Interfacial fusion-enhanced 11 μm-thick gel polymer electrolyte for high-performance lithium metal batteries

In the pursuit of ultrathin polymer electrolyte(<20 μm) for lithium metal batteries, achieving a balance between mechanical strength and interfacial stability is crucial for the longevity of the electrolytes.Herein, 11 μm-thick gel polymer electrolyte is designed via an integrated electrode/electrolyte structure supported by lithium metal anode. Benefiting from an exemplary superiority of excellent mechanical property, high ionic conductivity, and robust interfacial adhesion, the in-situ formed polymer electrolyte reinforced by titanosiloxane networks(ISPTS) embodies multifunctional roles of physical barrier, ionic carrier, and artificial protective layer at the interface. The potent interfacial interactions foster a seamless fusion of the electrode/electrolyte interfaces and enable continuous ion transport. Moreover, the built-in ISPTS electrolyte participates in the formation of gradient solid-electrolyte interphase(SEI) layer, which enhances the SEI's structural integrity against the strain induced by volume fluctuations of lithium anode.Consequently, the resultant 11 μm-thick ISPTS electrolyte enables lithium symmetric cells with cycling stability over 600 h and LiFePO_(4) cells with remarkable capacity retention of 96.6% after 800 cycles.This study provides a new avenue for designing ultrathin polymer electrolytes towards stable, safe,and high-energy–density lithium metal batteries.

Revealing the effect of electrolyte coordination structures on the intercalation chemistry of batteries

In-depth understanding of the electrolyte-dependent intercalation chemistry in batteries through direct operando/in situ characterizations is crucial for the development of the high-performance batteries.Herein,taking the Al/graphite battery as a model system,the effect of electrolyte coordination structure on the intercalation processes has been investigated over the batteries with either 1-hexyl-3-methylimidazolium chloride(HMICl)-AlCl_(3) or 1-ethyl-3-methylimidazolium chloride(EMICl)-AlCl_(3) ionic liquid electrolyte using operando X-ray photoelectron spectroscopy(XPS)and X-ray diffraction.With a weaker anion-cation interaction in HMI-based electrolyte,the XPS-derived atomic ratio between cointercalated N and intercalated Al is 0.9,which is lower than 1.6 for EMI-based electrolyte.Attributed to the additional de-solvation process,the batteries with the HMI-based electrolyte show a lower ionic diffusion rate,capacity,and cycling performance,which agree with the operando characterization results.Our findings highlight the critical role of the electrolyte coordination structure on the(co-)intercalation chemistry.

Electrolyte Solvation Structure Design for High Voltage Zinc-Based Hybrid Batteries

Zinc(Zn)metal anodes have enticed substantial curiosity for large-scale energy storage owing to inherent safety,high specific and volumetric energy capacities of Zn metal anodes.However,the aqueous electrolyte traditionally employed in Zn batteries suffers severe decomposition due to the narrow voltage stability window.Herein,we introduce N-methylformamide(NMF)as an organic solvent and modulate the solvation structure to obtain a stable organic/aqueous hybrid electrolyte for high-voltage Zn batteries.NMF is not only extremely stable against Zn metal anodes but also reduces the free water molecule availability by creating numerous hydrogen bonds,thereby accommodating high-voltage Zn‖LiMn_(2)O_(4)batteries.The introduction of NMF prevented hydrogen evolution reaction and promoted the creation of an Frich solid electrolyte interphase,which in turn hampered dendrite growth on Zn anodes.The Zn‖LiMn_(2)O_(4)full cells delivered a high average Coulombic efficiency of 99.7%over 400 cycles.

Reshaping Electrolyte Solvation Structure for High-Energy Aqueous Batteries

A highlight on reshaping aqueous electrolyte solvation structure for highenergy batteries is provided.Firstly,the recent key design routes for regulating solvation structure to widen electrochemical stability window(ESW)of aqueous electrolyte are briefly summarized.Then,the groundbreaking work of Wang et al.on reshaping electrolyte structure using urea as the diluent is elaborated.Finally,the significance of Wang's work is highlighted.

Study of GaAs/GaAlAs Multilayer Structural Materials by Electrolyte Electroreflectance

Electrolyte electroreflectance (EER) has been widely employed to investigate the electronic energy band structure and related physical properties of semiconductors. The electrolyte electroreflectance (EER) method combined with electrochemical anodic dissolution was used to study GaAs/GaAlAs multilayer structural materials. According to variation of the EER spectra during anodic dissolution the characteristics of GaAs/GaAlAs multilayer structural materials such as properties of the interface, p-n junction positions and Al content profiles were obtained.

Design of solid-state sodium-ion batteries with high mass-loading cathode by porous-dense bilayer electrolyte

Solid-state sodium-ion batteries with sodium metal anodes possess high safety and reliability,which are considered as a promising candidate for the next generation of energy storage technology.However,poor electronic and ionic conductivities at the interface between electrodes and solid-state electrolytes restrict its practical application.Herein,we demonstrate a β″-Al_(2)O_(3) electrolyte with a vertically porousdense bilayer structure to solve this problem.The carbon-coated vertically porous layer serves as a high mass-loading host for Na_(3)V_(2)(PO_(4))_(3) cathode and provides fast electronically and ionically conductive pathways.In addition,the dense layer is produced to prevent sodium dendrite growth and improve mechanical strength of β″-Al_(2)O_(3) electrolyte.Experimental results show that the cathode loading in vertically porous layer can reach to 8 mg cm^(-2),and the porous-dense bilayer β″-Al_(2)O_(3) electrolyte-based battery exhibits a reversible specific capacity of 87 mAh g^(-1) and a capacity retention of 95.5%over 100 cycles at a current density of 0.1 C,which is superior to that of the traditional dense β″-Al_(2)O_(3) electrolytebased battery.This work based on electrolyte structure design represents an efficient strategy for the development of solid-state sodium-ion batteries with high mass-loading cathode.

Structural energy storage composites based on modified carbon fiber electrode with metal-organic frame enhancing layered double hydroxide

Structural energy storage composites present advantages in simultaneously achieving structural strength and electrochemical properties.Adoption of carbon fiber electrodes and resin structural electrolytes in energy storage composite poses challenges in maintaining good mechanical and electrochemical properties at reasonable cost and effort.Here,we report a simple method to fabricate structural supercapacitor using carbon fiber electrodes(modified by Ni-layered double hydroxide(Ni-LDH)and in-situ growth of Co-metal-organic framework(Co-MOF)in a two-step process denoted as Co-MOF/Ni-LDH@CF)and bicontinuous-phase epoxy resin-based structural electrolyte.Co-MOF/Ni-LDH@CF as electrode material exhibits improved specific capacity(42.45 F·g^(-1))and cycle performance(93.3%capacity retention after 1000 cycles)in a three-electrode system.The bicontinuous-phase epoxy resin-based structural electrolyte exhibits an ionic conductivity of 3.27×10^(-4) S·cm^(-1).The fabricated Co-MOF/Ni-LDH@CF/SPE-50 structural supercapacitor has an energy density of 3.21 Wh·kg^(-1) at a power density of 42.25 W·kg^(-1),whilst maintaining tensile strength and modulus of 334.6 MPa and 25.2 GPa.These results show practical potential of employing modified commercial carbon fiber electrodes and epoxy resin-based structural electrolytes in structural energy storage applications.