High Reversible Pseudocapacity in Mesoporous Yolk–Shell Anatase TiO2/TiO2(B) Microspheres Used as Anodes for Li‐Ion Batteries

As an anode material for lithium‐ion batteries, titanium dioxide (TiO₂) shows good gravimetric performance (336 mAh g^?1 for LiTiO₂) and excellent cyclability. To address the poor rate behavior, slow lithium‐ion (Li⁺) diffusion, and high irreversible capacity decay, TiO₂ nanomaterials with tuned phase compositions and morphologies are being investigated. Here, a promising material is prepared that comprises a mesoporous “yolk–shell” spherical morphology in which the core is anatase TiO₂ and the shell is TiO₂(B). The preparation employs a NaCl‐assisted solvothermal process and the electrochemical results indicate that the mesoporous yolk–shell microspheres have high specific reversible capacity at moderate current (330.0 mAh g^?1 at C/5), excellent rate performance (181.8 mAh g^?1 at 40C), and impressive cyclability (98% capacity retention after 500 cycles). The superior properties are attributed to the TiO₂(B) nanosheet shell, which provides additional active area to stabilize the pseudocapacity. In addition, the open mesoporous morphology improves diffusion of electrolyte throughout the electrode, thereby contributing directly to greatly improved rate capacity.     

A High‐Energy Li‐Ion Battery Using a Silicon‐Based Anode and a Nano‐Structured Layered Composite Cathode

High capacity electrodes based on a Si composite anode and a layered composite oxide cathode, Ni‐rich Li[Ni_0.75Co_0.1Mn_0.15]O₂, are evaluated and combined to fabricate a high energy lithium ion battery. The Si composite anode, Si/C‐IWGS (internally wired with graphene sheets), is prepared by a scalable sol–gel process. The Si/C‐IWGS anode delivers a high capacity of >800 mAh g^?1 with an excellent cycling stability of up to 200 cycles, mainly due to the small amount of graphene (～6 wt%). The cathode (Li[Ni_0.75Co_0.1Mn_0.15]O₂) is structurally optimized (Ni‐rich core and a Ni‐depleted shell with a continuous concentration gradient between the core and shell, i.e., a full concentration gradient, FCG, cathode) so as to deliver a high capacity (>200 mAh g^?1) with excellent stability at high voltage (～4.3 V). A novel lithium ion battery system based on the Si/C‐IWGS anode and FCG cathode successfully demonstrates a high energy density (240 Wh kg^?1 at least) as well as an unprecedented excellent cycling stability of up to 750 cycles between 2.7 and 4.2 V at 1C. As a result, the novel battery system is an attractive candidate for energy storage applications demanding a high energy density and long cycle life.     

Walnut‐Like Multicore–Shell MnO Encapsulated Nitrogen‐Rich Carbon Nanocapsules as Anode Material for Long‐Cycling and Soft‐Packed Lithium‐Ion Batteries

Metal oxide‐based nanomaterials are widely studied because of their high‐energy densities as anode materials in lithium‐ion batteries. However, the fast capacity degradation resulting from the large volume expansion upon lithiation hinders their practical application. In this work, the preparation of walnut‐like multicore–shell MnO encapsulated nitrogen‐rich carbon nanocapsules (MnO@NC) is reported via a facile and eco‐friendly process for long‐cycling Li‐ion batteries. In this hybrid structure, MnO nanoparticles are uniformly dispersed inside carbon nanoshells, which can simultaneously act as a conductive framework and also a protective buffer layer to restrain the volume variation. The MnO@NC nanocapsules show remarkable electrochemical performances for lithium‐ion batteries, exhibiting high reversible capability (762 mAh g^?1 at 100 mA g^?1) and stable cycling life (624 mAh g^?1 after 1000 cycles at 1000 mA g^?1). In addition, the soft‐packed full batteries based on MnO@NC nanocapsules anodes and commercial LiFePO₄ cathodes present good flexibility and cycling stability.     

Self‐Standing Porous LiCoO2 Nanosheet Arrays as 3D Cathodes for Flexible Li‐Ion Batteries

Self‐standing electrodes are the key to realize flexible Li‐ion batteries. However, fabrication of self‐standing cathodes is still a major challenge. In this work, porous LiCoO₂ nanosheet arrays are grown on Au‐coated stainless steel (Au/SS) substrates via a facile “hydrothermal lithiation” method using Co₃O₄ nanosheet arrays as the template followed by quick annealing in air. The binder‐free and self‐standing LiCoO₂ nanosheet arrays represent the 3D cathode and exhibit superior rate capability and cycling stability. In specific, the LiCoO₂ nanosheet array electrode can deliver a high reversible capacity of 104.6 mA h g^?1 at 10 C rate and achieve a capacity retention of 81.8% at 0.1 C rate after 1000 cycles. By coupling with Li₄Ti₅O₁₂ nanosheet arrays as anode, an all‐nanosheet array based LiCoO₂//Li₄Ti₅O₁₂ flexible Li‐ion battery is constructed. Benefiting from the 3D nanoarchitectures for both cathode and anode, the flexible LiCoO₂//Li₄Ti₅O₁₂ battery can deliver large specific reversible capacities of 130.7 mA h g^?1 at 0.1 C rate and 85.3 mA h g^?1 at 10 C rate (based on the weight of cathode material). The full cell device also exhibits good cycling stability with 80.5% capacity retention after 1000 cycles at 0.1 C rate, making it promising for the application in flexible Li‐ion batteries.     

Few‐Layered SnS2 on Few‐Layered Reduced Graphene Oxide as Na‐Ion Battery Anode with Ultralong Cycle Life and Superior Rate Capability

Na‐ion Batteries have been considered as promising alternatives to Li‐ion batteries due to the natural abundance of sodium resources. Searching for high‐performance anode materials currently becomes a hot topic and also a great challenge for developing Na‐ion batteries. In this work, a novel hybrid anode is synthesized consisting of ultrafine, few‐layered SnS₂ anchored on few‐layered reduced graphene oxide (rGO) by a facile solvothermal route. The SnS₂/rGO hybrid exhibits a high capacity, ultralong cycle life, and superior rate capability. The hybrid can deliver a high charge capacity of 649 mAh g^?1 at 100 mA g^?1. At 800 mA g^?1 (1.8 C), it can yield an initial charge capacity of 469 mAh g^?1, which can be maintained at 89% and 61%, respectively, after 400 and 1000 cycles. The hybrid can also sustain a current density up to 12.8 A g^?1 (≈28 C) where the charge process can be completed in only 1.3 min while still delivering a charge capacity of 337 mAh g^?1. The fast and stable Na‐storage ability of SnS₂/rGO makes it a promising anode for Na‐ion batteries.     

Enhanced Ionic/Electronic Transport in Nano‐TiO2/Sheared CNT Composite Electrode for Na+ Insertion‐based Hybrid Ion‐Capacitors

Ion‐insertion capacitors show promise to bridge the gap between supercapacitors of high power densities and batteries of high energy densities. While research efforts have primarily focused on Li⁺‐based capacitors (LICs), Na⁺‐based capacitors (SICs) are theoretically cheaper and more sustainable. Owing to the larger size of Na⁺ compared to Li⁺, finding high‐rate anode materials for SICs has been challenging. Herein, an SIC anode architecture is reported consisting of TiO₂ nanoparticles anchored on a sheared‐carbon nanotubes backbone (TiO₂/SCNT). The SCNT architecture provides advantages over other carbon architectures commonly used, such as reduced graphene oxide and CNT. In a half‐cell, the TiO₂/SCNT electrode shows a capacity of 267 mAh g^?1 at a 1 C charge/discharge rate and a capacity of 136 mAh g^?1 at 10 C while maintaining 87% of initial capacity over 1000 cycles. When combined with activated carbon (AC) in a full cell, an energy density and power density of 54.9 Wh kg^?1 and 1410 W kg^?1, respectively, are achieved while retaining a 90% capacity retention over 5000 cycles. The favorable rate capability, energy and power density, and durability of the electrode is attributed to the enhanced electronic and Na⁺ conductivity of the TiO₂/SCNT architecture.     

Intercalated Electrolyte with High Transference Number for Dendrite‐Free Solid‐State Lithium Batteries

Solid‐state lithium (Li) batteries using solid electrolytes and Li anodes are highly desirable because of their high energy densities and intrinsic safety. However, low ambient‐temperature conductivity and poor interface compatibility of solid electrolytes as well as Li dendrite formation cause large polarization and poor cycling stability. Herein, a high transference number intercalated composite solid electrolyte (CSE) is prepared by the combination of a solution‐casting and hot‐pressing method using layered lithium montmorillonite, poly(ethylene carbonate), lithium bis(fluorosulfonyl)imide, high‐voltage fluoroethylene carbonate additive, and poly(tetrafluoroethylene) binder. The electrolyte presents high ionic conductivity (3.5 × 10^?4 S cm^?1), a wide electrochemical window (4.6 V vs Li⁺/Li), and high ionic transference number (0.83) at 25 °C. In addition, a 3D Li anode is also fabricated via a facile thermal infusion strategy. The synergistic effect of high transference number intercalated electrolyte and 3D Li anode is more favorable to suppress Li dendrites in a working battery. The solid‐state batteries based on LiFePO₄ (Al₂O₃ @ LiNi_0.5Co_0.2Mn_0.3O₂), CSE, and 3D Li deliver admirable cycling stability with discharge capacity 145.9 mAh g^?1 (150.7 mAh g^?1) and capacity retention 91.9% after 200 cycles at 0.5 C (92.0% after 100 cycles at 0.2 C) at 25 °C. This work affords a splendid strategy for high‐performance solid‐state battery.     

A Green and Facile Way to Prepare Granadilla‐Like Silicon‐Based Anode Materials for Li‐Ion Batteries

A yolk‐shell‐structured carbon@void@silicon (CVS) anode material in which a void space is created between the inside silicon nanoparticle and the outer carbon shell is considered as a promising candidate for Li‐ion cells. Untill now, all the previous yolk‐shell composites were fabricated through a templating method, wherein the SiO₂ layer acts as a sacrificial layer and creates a void by a selective etching method using toxic hydrofluoric acid. However, this method is complex and toxic. Here, a green and facile synthesis of granadilla‐like outer carbon coating encapsulated silicon/carbon microspheres which are composed of interconnected carbon framework supported CVS nanobeads is reported. The silicon granadillas are prepared via a modified templating method in which calcium carbonate was selected as a sacrificial layer and acetylene as a carbon precursor. Therefore, the void space inside and among these CVS nanobeads can be formed by removing CaCO₃ with diluted hydrochloric acid. As prepared, silicon granadillas having 30% silicon content deliver a reversible capacity of around 1100 mAh g^?1 at a current density of 250 mA g^?1 after 200 cycles. Besides, this composite exhibits an excellent rate performance of about 830 and 700 mAh g^?1 at the current densities of 1000 and 2000 mA g^?1, respectively.     

High‐Performance,Low‐Cost,and Dense‐Structure Electrodes with High Mass Loading for Lithium‐Ion Batteries

Lithium‐ion batteries have undergone a remarkable development in the past 30 years. However, conventional electrodes are insufficient for the ever‐increasing demand of high‐energy batteries. Here, reported is a thick electrode with a dense structure, as an alternative to the commonly recognized porous framework. A low‐temperature sintering technology with the aid of aqueous solvent, high pressure, and an ion‐conductive additive is originally developed for preparing the LiCoO₂ (LCO)/Li₄Ti₅O₁₂ (LTO) dense‐structure electrode as the representative cathode/anode material. The 400 µm thick cathode with 110 mg cm^?2 mass loading achieves a high specific capacity of 131.2 mAh g^?1 with a good capacity retention of 96% over 150 cycles, far exceeding the commercial counterpart (≈40 µm) of 54.1 mAh g^?1 with 39%. The ultrathick electrode of 1300 µm thickness presents a remarkable area capacity of 28.6 mAh cm^?2 that is 16 times that of the commercial electrode. The full cell based on the dense electrodes delivers an extremely high areal capacity of 14.4 mAh cm^?2. The ion‐diffusion coefficients of the densely sintered electrodes increase by nearly three orders of magnitude. This design opens up a new avenue for scalable and sustainable material manufacturing towards various practical applications.     

Multicore–Shell Bi@N‐doped Carbon Nanospheres for High Power Density and Long Cycle Life Sodium‐ and Potassium‐Ion Anodes

Bismuth (Bi) is an attractive material as anodes for both sodium‐ion batteries (NIBs) and potassium‐ion batteries (KIBs), because it has a high theoretical gravimetric capacity (386 mAh g^?1) and high volumetric capacity (3800 mAh L^?1). The main challenges associated with Bi anodes are structural degradation and instability of the solid electrolyte interphase (SEI) resulting from the huge volume change during charge/discharge. Here, a multicore–shell structured Bi@N‐doped carbon (Bi@N‐C) anode is designed that addresses these issues. The nanosized Bi spheres are encapsulated by a conductive porous N‐doped carbon shell that not only prevents the volume expansion during charge/discharge but also constructs a stable SEI during cycling. The Bi@N‐C exhibits unprecedented rate capability and long cycle life for both NIBs (235 mAh g^?1 after 2000 cycles at 10 A g^?1) and KIBs (152 mAh g^?1 at 100 A g^?1). The kinetic analysis reveals the outstanding electrochemical performance can be attributed to significant pseudocapacitance behavior upon cycling.     

Silicon‐Based Self‐Assemblies for High Volumetric Capacity Li‐Ion Batteries via Effective Stress Management

Silicon nanoparticles (Si NPs) have been considered as promising anode materials for next‐generation lithium‐ion batteries, but the practical issues such as mechanical structure instability and low volumetric energy density limit their development. At present, the functional energy‐storing architectures based on Si NPs building blocks have been proposed to solve the adverse effects of nanostructures, but designing ideal functional architectures with excellent electrochemical performance is still a significant challenge. This study shows that the effective stress evolution management is applied for self‐assembled functional architectures via cross‐scale simulation and the simulated stress evolution can be a guide to design a scalable self‐assembled hierarchical Si@TiO₂@C (SA‐SiTC) based on core–shell Si@TiO₂ nanoscale building blocks. It is found that the carbon filler and TiO₂ layer can effectively reduce the risk of cracking during (de)lithiation, ensuring the stability of the mechanical structure of SA‐SiTC. The SA‐SiTC electrode shows long cycling stability (842.6 mAh g^?1 after 1000 cycles at 2 A g^?1), high volumetric capacity (174 mAh cm^?3), high initial Coulombic efficiency (80.9%), and stable solid‐electrolyte interphase (SEI) layer. This work provides insight into the development of the structural stable Si‐based anodes with long cycle life and high volumetric energy density for practical energy applications.     

Solid‐State Plastic Crystal Electrolytes: Effective Protection Interlayers for Sulfide‐Based All‐Solid‐State Lithium Metal Batteries

All‐solid‐state lithium metal batteries (ASSLMBs) have attracted significant attention due to their superior safety and high energy density. However, little success has been made in adopting Li metal anodes in sulfide electrolyte (SE)‐based ASSLMBs. The main challenges are the remarkable interfacial reactions and Li dendrite formation between Li metal and SEs. In this work, a solid‐state plastic crystal electrolyte (PCE) is engineered as an interlayer in SE‐based ASSLMBs. It is demonstrated that the PCE interlayer can prevent the interfacial reactions and lithium dendrite formation between SEs and Li metal. As a result, ASSLMBs with LiFePO₄ exhibit a high initial capacity of 148 mAh g^?1 at 0.1 C and 131 mAh g^?1 at 0.5 C (1 C = 170 mA g^?1), which remains at 122 mAh g^?1 after 120 cycles at 0.5 C. All‐solid‐state Li‐S batteries based on the polyacrylonitrile‐sulfur composite are also demonstrated, showing an initial capacity of 1682 mAh g^?1. The second discharge capacity of 890 mAh g^?1 keeps at 775 mAh g^?1 after 100 cycles. This work provides a new avenue to address the interfacial challenges between Li metal and SEs, enabling the successful adoption of Li metal in SE‐based ASSLMBs with high energy density.     

Highly Connected Silicon–Copper Alloy Mixture Nanotubes as High‐Rate and Durable Anode Materials for Lithium‐Ion Batteries

Seeking high‐capacity, high‐rate, and durable anode materials for lithium‐ion batteries (LIBs) has been a crucial aspect to promote the use of electric vehicles and other portable electronics. Here, a novel alloy‐forming approach to convert amorphous Si (a‐Si)‐coated copper oxide (CuO) core–shell nanowires (NWs) into hollow and highly interconnected Si–Cu alloy (mixture) nanotubes is reported. Upon a simple H₂ annealing, the CuO cores are reduced and diffused out to alloy with the a‐Si shell, producing highly interconnected hollow Si–Cu alloy nanotubes, which can serve as high‐capacity and self‐conductive anode structures with robust mechanical support. A high specific capacity of 1010 mAh g^?1 (or 780 mAh g^?1) has been achieved after 1000 cycles at 3.4 A g^?1 (or 20 A g^?1), with a capacity retention rate of ≈84% (≈88%), without the use of any binder or conductive agent. Remarkably, they can survive an extremely fast charging rate at 70 A g^?1 for 35 runs (corresponding to one full cycle in 30 s) and recover 88% capacity. This novel alloy‐nanotube structure could represent an ideal candidate to fulfill the true potential of Si‐loaded LIB applications.     

Safe,Stable Cycling of Lithium Metal Batteries with Low‐Viscosity,Fire‐Retardant Locally Concentrated Ionic Liquid Electrolytes

Ionic liquid (IL) electrolytes with concentrated Li salt can ensure safe, high‐performance Li metal batteries (LMBs) but suffer from high viscosity and poor ionic transport. A locally concentrated IL (LCIL) electrolyte with a non‐solvating, fire‐retardant hydrofluoroether (HFE) is presented. This rationally designed electrolyte employs lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), 1‐methyl‐1‐propyl pyrrolidinium bis(fluorosulfonyl)imide (P13FSI) and 1,1,2,2‐tetrafluoroethyl 2,2,3,3‐tetrafluoropropyl ether (TTE) as the IL and HFE, respectively (1:2:2 by mol). Adding TTE enables a Li‐concentrated IL electrolyte with low viscosity and good separator wettability, facilitating Li‐ion transport to the Li metal anode. The non‐flammability of TTE contributes to excellent thermal stability. Furthermore, synergy between the dual (FSI/TFSI) anions in the LCIL electrolyte can help modify the solid electrolyte interphase, increasing Li Coulombic efficiency and decreasing dendritic Li deposition. LMBs (Li||LiCoO₂) employing the LCIL electrolyte exhibit good rate capability (≈89 mAh g^?1 at 1.8 mA cm^?2, room temperature) and long‐term cycling (≈80% retention after 400 cycles).     

Li‐CO2 Batteries Efficiently Working at Ultra‐Low Temperatures

Lithium‐carbon dioxide (Li‐CO₂) batteries are considered promising energy‐storage systems in extreme environments with ultra‐high CO₂ concentrations, such as Mars with 96% CO₂ in the atmosphere, due to their potentially high specific energy densities. However, besides having ultra‐high CO₂ concentration, another vital but seemingly overlooked fact lies in that Mars is an extremely cold planet with an average temperature of approximately ?60 °C. The existing Li‐CO₂ batteries could work at room temperature or higher, but they will face severe performance degradation or even a complete failure once the ambient temperature falls below 0 °C. Herein, ultra‐low‐temperature Li‐CO₂ batteries are demonstrated by designing 1,3‐dioxolane‐based electrolyte and iridium‐based cathode, which show both a high deep discharge capacity of 8976 mAh g^?1 and a long lifespan of 150 cycles (1500 h) with a fixed 500 mAh g^?1 capacity per cycle at ?60 °C. The easy‐to‐decompose discharge products in small size on the cathode and the suppressed parasitic reactions both in the electrolyte and on the Li anode at low temperatures together contribute to the above high electrochemical performances.     

A Soft Lithiophilic Graphene Aerogel for Stable Lithium Metal Anode

The lithium metal anode is one of the most promising anodes for next‐generation high‐energy‐density batteries. However, the severe growth of Li dendrites and large volume expansion leads to rapid capacity decay and shortened lifetime, especially in high current density and high capacity. Herein, a soft 3D Au nanoparticles@graphene hybrid aerogel (Au? GA) as a lithiophilic host for lithium metal anode is proposed. The large surface area and interconnected conductive pathways of the Au? GA significantly decrease the local current density of the electrode, enabling uniform Li deposition. Furthermore, the 3D porous structure effectively accommodates the large volume expansion during Li plating/stripping, and the Li_xAu alloy serves as a solid solution buffer layer to completely eliminate the Li nucleation over‐potential. Symmetric cells can stably cycle at 8 mA cm^?2 for 8 mAh cm^?2 and exhibit ultra‐long cycling: 1800 h at 2 mA cm^?2 for 2 mAh cm^?2, and 1200 h at 4 mA cm^?2 for 4 mAh cm^?2, with low over‐potential. Full cells assemble with a Cu@Au? GA? Li anode and LiFePO₄ cathode, can sustain a high rate of 8 C, and retain a high capacity of 59.6 mAh g^?1 after 1100 cycles at 2 C.     

Amorphous GaN@Cu Freestanding Electrode for High‐Performance Li‐Ion Batteries

GaN is demonstrated to be an ideal anode for Li‐ion batteries (LIBs) for the first time. Amorphous GaN@Cu nanorods (a‐GaN@Cu) freestanding electrode is designed via a low‐temperature pulsed laser deposition method, which exhibits prominent rate capability and untralong lifespan as an anode for LIBs. With porous interconnected metal nanorods substrate to improve the structure integrity and electronic conductivity, the a‐GaN@Cu electrode delivers a capacity recovery of 980 mAh g^?1 after 150 cycles from 0.25 to 6.25 A g^?1 and a high discharge capacity of 509 mAh g^?1 after 3000 cycles at 10.0 A g^?1. The lithium storage in the a‐GaN is also systematically studied, which suggests a redox reaction mechanism.     

Engineering Wavy‐Nanostructured Anode Interphases with Fast Ion Transfer Kinetics: Toward Practical Li‐Metal Full Batteries

Fast Li‐metal depletion and severe anode pulverization are the most critical obstacles for the energy‐dense Li‐metal full batteries using thin Li‐metal anodes (<50 µm). Here, a wavy‐nanostructured solid electrolyte interphase (SEI) with fast ion transfer kinetics is reported, which can promote high‐efficiency Li‐metal plating/stripping (>98% at 4 mAh cm^?2) in conventional carbonate electrolyte. Cryogenic transmission electron microscopy (cryo‐TEM) further reveals the fundamental relationship between wavy‐nanostructured SEI, function, and the electrochemical performance. The wavy SEI with greatly decreased surface diffusion resistance can realize grain coarsening of Li‐metal deposition and exhaustive dissolution of active Li‐metal during the stripping process, which can effectively alleviate “dead Li” accumulation and anode pulverization problems in practical full cells. Under highly challenging conditions (45 µm Li‐metal anodes, 4.3 mAh cm^?2 high capacity LiNi_0.8Mn_0.1Co_0.1O₂ cathodes), full cells exhibit significantly improved cycling lifespan (170 cycles; 20 cycles for control cells) via the application of wavy SEI.     

Engineering MoS2 Nanosheets on Spindle‐Like α‐Fe2O3 as High‐Performance Core–Shell Pseudocapacitive Anodes for Fiber‐Shaped Aqueous Lithium‐Ion Capacitors

Fiber‐shaped aqueous lithium‐ion capacitors (FALICs) featured with high energy and power densities together with outstanding safety characteristics are emerging as promising electrochemical energy‐storage devices for future portable and wearable electronics. However, the lack of high‐capacitance fibrous anodes is a major bottleneck to achieve high performance FALICs. Here, hierarchical MoS₂@α‐Fe₂O₃ core–shell heterostructures consisting of spindle‐shaped α‐Fe₂O₃ cores and MoS₂ nanosheet shells on a carbon nanotube fiber (CNTF) are successfully fabricated. Originating from the unique core/shell architecture and prominent synergetic effects for multi‐components, the resulting MoS₂@α‐Fe₂O₃/CNTF anode delivers a remarkable specific capacitance of 2077.5 mF cm^?2 (554.0 F cm^?3) at 2 mA cm^?2, substantially outperforming most of the previously reported fibrous anode materials. Further density functional theory calculations reveal that the MoS₂@α‐Fe₂O₃ nano‐heterostructure possesses better electrical conductivity and stronger adsorption energy of Li⁺ than those of the individual MoS₂ and α‐Fe₂O₃. By paring with the self‐standing LiCoO₂/CNTF battery‐type cathode, a prototype quasi‐solid‐state FALIC with a maximum operating voltage of 2.0 V is constructed, achieving impressive specific capacitance (253.1 mF cm^?2) and admirable energy density (39.6 mWh cm^?3). Additionally, the newly developed FALICs can be woven into the flexible textile to power wearable electronics. This work presents a novel effective strategy to design high‐performance anode materials for next‐generation wearable ALICs.     

Liquid Polydimethylsiloxane Grafting to Enable Dendrite‐Free Li Plating for Highly Reversible Li‐Metal Batteries

Li‐metal is considered as the most promising anode material to advance the development of next‐generation energy storage devices owing to its unparalleled theoretical specific capacity and extremely low redox electrochemical potential. However, safety concerns and poor cycling retention of Li‐metal batteries (LMBs) caused by uncontrolled Li dendrite growth still limit their broad application. Herein, liquid polydimethylsiloxane (PDMS) terminated by –OCH₃ groups is proposed as a graftable additive to reinforce the anode dendrite suppression for LMBs. Such a grafting triggers the formation of a conformal hybrid solid electrolyte interphase (SEI) with increased fractions of LiF and Li–Si–O‐based moieties, which serve as a rigid barrier and ionic conductor for uniform Li‐ion flow and Li‐mass deposition. The grafting protected anode endows Li/Li symmetric cells with a long lifetime over 1800 h with a much smaller voltage gap (≈25 mV) between Li plating and stripping, than the naked anode. The coulombic efficiency values for Li/Cu asymmetric cells in carbonate electrolyte can reach up to 97% even at a high current density of 3 mA cm^?2 or high capacity up to 4 mAh cm^?2. The liquid PDMS additive shows advantage over solid siloxane additives with poor grafting ability in terms of Li surface compaction and SEI stabilization.