The compact design of an environmentally adaptive battery and effectors forms the foundation for wearable electronics capable of time-resolved, long-term signal monitoring. Herein, we present a one-body strategy that utilizes a hydrogel as the ionic conductive medium for both flexible aqueous zinc-ion batteries and wearable strain sensors. The poly(vinyl alcohol) hydrogel network incorporates nano-SiO2 and cellulose nanofibers (referred to as PSC) in an ethylene glycol/water mixed solvent, balancing the mechanical properties (tensile strength of 6 MPa) and ionic diffusivity at -20 degrees C (2 orders of magnitude higher than 2 M ZnCl2 electrolyte). Meanwhile, cathode lattice breathing during the solvated Zn2+ intercalation and dendritic Zn protrusion at the anode interface are mitigated. Besides the robust cyclability of the Zn parallel to PSC parallel to V2O5 prototype within a wide temperature range (from -20 to 80 degrees C), this microdevice seamlessly integrates a zinc-ion battery with a strain sensor, enabling precise monitoring of the muscle response during dynamic body movement. By employing transmission-mode operando XRD, the self-powered sensor accurately documents the real-time phasic evolution of the layered cathode and synchronized strain change induced by Zn deposition, which presents a feasible solution of health monitoring by the miniaturized electronics.

The paradigm shift toward the closed-loop recycling of spent lithium-ion batteries necessitates the direct, efficient cathode recovery that goes beyond the traditional pyrometallurgy and hydrometallurgy techniques, meanwhile avoiding substantial energy consumption, tedious procedures, or chemical contamination. In this study, a straightforward, dual-functional upcycling approach is presented for the spent nickel-rich cathodes to boost their high-rate performance. Specifically, the protocol rationally employs the Li vacancy within the degraded oxide to minimize the La diffusion barrier, expanding the lattice spacing of the layered structure; the Li+ conductive, conformal LiLaO2 encapsulation further suppresses the interfacial acid corrosion and structural deterioration into the rock-salt phase. Transmission-mode X-ray diffraction tracks the reversible lattice breathing of the regenerated cathode in operando, suggesting the continuous, kinetically boosted solid-solution process with all the microcracks repaired. The as-assembled regenerated LiNi0.8Co0.1Mn0.1O2/Graphite pouch cell (1.4Ah) thus achieves 91.0% capacity retention for 500 cycles, the energy density of 277 Wh kg-1 as well as extreme power output of 1030 W kg-1 at the cell level. This upcycling strategy paves the way for value-added utilization of the retired Ni-rich cathodes in practical high-rate battery prototypes. A straightforward, dual-functional upcycling approach is presented for the spent Ni-rich cathodes to boost their high-rate performance. Specifically, the protocol rationally employs the Li vacancy within the degraded oxide to minimize the La diffusion barrier, expanding the lattice spacing of the layered structure; the Li+ conductive, conformal LiLaO2 encapsulation further suppresses the interfacial acid corrosion and structural deterioration into the rock-salt phase. image

The unregulated metallic deposition and continuous cracking of the fragile solid electrolyte interphase are considered the critical barriers that compromise the cyclability of lithium metal batteries (LMB), especially under low N/P ratio (<3) pairing modes. Herein, an ultra-thin (5 m), lightweight (0.25 mg cm(-2)), and moisture-proof interfacial layer composed of the high-entropy alloys (denoted as HEAs) and interweaved carbon nanotubes (CNTs) scaffold is constructed to modify the current collector, moreover, the thermally-induced Li22Si5 alloy blended with the hydrophobic ethylene-vinyl acetate copolymer (EVA) is infiltrated into the scaffold pores as the moisture-proof cation reservoir. The HEA@CNT/Li22Si5@EVA interfacial layer not only maximizes the Li-utilization degree with minimal voltage divergence in symmetric cells but also compensates for irreversible Li depletion in the pouch-format anode-less models. As the HEA@CNT/Li22Si5@EVA-Cu substrate paired with the LiNi0.8Mn0.1Co0.1O2 cathode in a 200 mAh prototype, the phase evolution of oxide cathode and efficient Li utilization at the anode substrate can be real-time monitored by the transmission-mode operando X-ray diffraction. This interfacial layer strategy affords multifunctionality to enable the LMB prototyping without excessive Li abuse. Consequently, cycling endurance and the balanced energy densities (420.1 Wh kg(-1)) are obtained on the whole cell.

Featuring the straightforward assembly of fully lithiated cathodes with bared current collectors, anode-free lithium metal batteries (AFLMBs) nominally achieve the highest gravimetric/volumetric energy densities with minimum Li host in excess, simplified anode processing, as well as the reduced labor/cost of cell manufacturing and maintenance. Nevertheless, issues of parasitic interfacial reactions, high-voltage cathode collapse and the irreversible Li+ plating on the deposition substrate, collectively deplete the cation reservoir of cell models. This study thus proposes a separator strategy to enable the multiscale interfacial stabilization for Ah-level AFLMB model. Specifically, the sacrificial Li2S@C prelithiation layer loaded on the polyolefin separator (Li2S@C|PE), not only supplements the customized Li+ inventory during the formation cycle, but also establishes the lithium polysulfides containing cathode interface with the high-voltage tolerance (till 4.5V). Through the combined analysis of in-situ electrochemical impedance spectroscopy and transmission-mode operando X-ray diffraction, the enhanced Li+ diffusivity and reversible phase evolution of LiNi0.8Co0.1Mn0.1O2 cathode as in contact with the prelithiation separator are real-time documented. Upon the cell assembly of Li2S@C|PE separator with the Ag modified Cu foil (Ag-Cu) and densely-packed LiNi0.8Co0.1Mn0.1O2 cathode (25.0 mg cm− 2) under lean electrolyte condition (E/C 1.8 g Ah− 1), the 1.22 Ah pouch-format prototype balances the robust cycling endurance, gravimetric/volumetric energy densities of 450 Wh kg− 1/1355 Wh L− 1, as well as extreme power output up to 830.6 W kg− 1. This prelithiation protocol demonstrates upscaling potential and generic applicability to secure the interfacial chemistries for anode-less/-free LMB configurations.

The implementation of solid polymer electrolytes (SPEs) in energy-dense batteries faces severe challenges including sluggish ionic diffusion, oxidation tendency at the cathode interface, dendrite protrusion from the metallic anode, as well as the technological incompatibility with the layer stack-up cell assembly. Herein, an in-situ polymerization strategy is presented to deal with above dilemma for the solid battery prototyping. The in situ cross-linked poly(ethylene glycol) diglycidyl ether is embedded within the nanocellulose framework, endowing SPE membrane with the reinforced mechanical strength (11.31 MPa) at the thickness of 10 mu m as well as superior ionic conductance (150 mS). After a rigorous selection, the sacrificial triphenylphosphine additive preferentially oxidizes on the LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode to form the cathode electrolyte interface during the formation charging. Concurrently, the solvated zinc(II) bis(trifluoromethylsulfonyl)imide constructs the polyether/LiZn mosaic layer on the Li foil, which effectively promotes interfacial cation diffusion and horizontal deposits propagation. By pairing the polymerized SPE with the thin-layer Li foil (50 mu m) and the NCM811 cathode (25 mg cm-2), the 94 mAh pouch-format cell can realize a gravimetric/volumetric energy density of 397.5 Wh kg-1 and 1197.6 Wh L-1, high-voltage tolerance till 4.5 V, and robust cyclability (95.1% capacity retention for 200 cycles). A facile in situ polymerization strategy is proposed to formulate a thin-layer, mechanically robust, high ionic conductive poly (ethylene glycol) diglycidyl ether (PEGDE)-based solid polymer electrolyte, in which the dual-functional, sacrificial additives of triphenylphosphine (TPP) and zinc(II) bis(trifluoromethylsulfonyl)imide (Zn(TFSI)2) exhibit strong electron-losing/accepting capabilities to stabilize both high-voltage LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode and high-reactive Li anode interfaces. image

Lattice oxygen redox reactions dedicate the extra retrievable capacities from the lithium-rich layered oxides (LLOs) cathodes, however, the widespread adoption of which in the energy-dense batteries faces a series of obstacles, such as oxygen loss during the initial activation, cycling-induced structural degradation as well as the retard Li+ diffusivity impeded by the interfacial impurities. Here, a Lewis acid gas treatment of LLOs is proposed, namely the PF5 etching to enhance the cycling endurance and high-temperature tolerance of the electrode. The multiscale modifications involve the F- doping in the bulk lattice, the phosphate coating to kinetically suppress the O2 release as well as the removal of surface impurities in a single step. The gas-phase treatment constructs a continuous pathway across the densely-packed LLO electrode, enhancing Li+ diffusivity by fivefold compared to the untreated electrode. Notably, the transmission-mode operando X-ray diffraction of the modified LLOs cathode confirms a 71.4% reduction of self-discharge rate during the idle charged state at 55 degrees C, as well as the 16% mitigation of lattice contraction (Delta c/a) during the dynamic galvanostatic cycling. By pairing the lithium foil (50 mu m) with the modified LLO cathode (12.75 mg cm-2) in a pouch-format cell model, the 0.2 Ah prototype achieves the gravimetric energy/power densities as well as cycling endurance across a wide temperature range. This scalable, Lewis-acid gas modification strategy presents a practical approach for deploying LLOs in energy-dense cell prototyping. This work presents a one-step, gas-phase treatment, namely the heat-induced Lewis-acid PF5 gas to reinforce the cycling endurance and high-temperature adaptability of the LLO cathode. The multiscale modifications range from the fluorine doping of the bulk lattice to mitigate the energy barrier of Li diffusion in the layered oxide, phosphate surface coating to suppress the O2 release as well as the removal of the carbonate or alkali impurities. image

Rechargeable aqueous zinc batteries (RAZBs) suffer from the structural degradation of the layered oxide cathode, parasitic side reaction on the Zn foil as well as often-overlooked self-discharge phenomenon at the elevated temperatures. Herein, this study presents a thin-layer (9 mu m) molecular-engineered separator strategy to achieve the concurrent shelf life, cycling endurance, as well as the practical energy density for the RAZBs prototype. On the face-to-cathode side, the biphthalic anhydride is anchored onto the polyethylene separator substrate (PE) via a robotic arm-controlled spray-coating method, inhibiting the spontaneous vanadium dissolution and shuttle at both the dynamic cycling or static high-temperature storage; meanwhile the 3,3 '-diamino-4,4 '-dihydroxydiphenyl sulfone molecular tailoring on the face-to-anode side provides ion-sieving capability to repel detrimental SO42-, yet guiding uniform Zn2+ influx and preferential deposits accumulation along the (002) crystallographic orientation even at the extreme deposition scenario (20 mA cm(-2), 20 mAh cm(-2)). Upon the layer-stacked assembly of the V2O5 cathode (2.0 mAh cm(-2)), molecular-engineered separator as well as the Zn foil (20 mu m), the 0.78 Ah pouch-format prototype exhibits the superior volumetric/gravimetric energy densities of 133.3 Wh L-1/71.4 Wh kg(-1) and extreme power output (444.3 W L-1/238.0 W kg(-1)).

The substantial manufacturing of lithium-ion batteries (LIBs) requires sustainable, circular, and decarbonized recycling strategies. While efforts are concentrated on extracting valuable metals from cathodes using intricate chemical process, the direct, efficient cathode regeneration remains a technological challenge. More urgently, the battery supply chain also requires the value-added exploitation of retired anodes. Here, a "closed-loop" approach is proposed to upcycle spent graphite into the prelithiation catalyst, namely the fewer-layer graphene flakes (FGF), upon the exquisite tuning of interlayer spacing and defect concentration. Since the catalytic FGF mitigates the delithiation energy barrier from calcinated Li5FeO4 nanocrystalline, the composite layer of which cast on the polyolefin substrate thus enables a customized prelithiation capability (98% Li+ utilization) for the retired LiFePO4 recovery. Furthermore, the hydrophobic polymeric modification guarantees the moisture tolerance of Li5FeO4 agents, aligning with commercial battery manufacturing standards. The separator strategy well regulates the interfacial chemistry in the anode-free pouch cell (LiFePO4||Cu), the prototype of which balances the robust cyclability, energy density up to 386.6 Wh kg-1 as well as the extreme power output of 1159.8 W kg-1. This study not only fulfills the sustainable supply chain with graphite upcycling, but also establishes a generic, viable protocol for the anode-free cell prototyping.

Coupling the Si-based anodes with nickel-rich LiNixMnyCo1−x−yO2 cathodes (x ≥ 0.8) in the energy-dense cell prototype suffers from the mechanical instability of the Li-Si alloys, cathode collapse upon the high-voltage cycling, as well as the severe leakage current at elevated temperatures. More seriously, the cathode-to-anode cross-talk effect of transitional metal aggravates the depletion of the active Li reservoir. To reconcile the cation utilization degree, stress dissipation, and extreme temperature tolerance of the Si-based anode||NMC prototype, we propose a gel polymer electrolyte to reinforce the mechanical integrity of Si anode and chelate with the transitional cations towards the stabilized interfacial property. As coupling the conformal gel polymer electrolyte encapsulation with the spatial arranged Si anode and NMC811 cathode, the 2.7 Ah pouch-format cell could achieve the high energy density of 325.9 Wh kg−1 (based on the whole pouch cell), 88.7% capacity retention for 2000 cycles, self-extinguish property as well as a wide temperature tolerance. Therefore, this proposed polymerization strategy provides a leap toward the secured Li batteries.

The practical use of polyethylene oxide polymer electrolyte in the solid‐state sodium metallic batteries (SSMBs) suffers from the retard Na + diffusion at the room temperature, mechanical fragility as well as the oxidation tendency at high voltages. Herein, a hetero‐layered composite polymeric electrolyte (CPE) is proposed to enable the simultaneous interfacial stability with the high voltage cathodes (till 4.2 V) and Na metallic anode. Being incorporated within the polymer matrix, the sand‐milled Na 3 Zr 2 Si 2 PO 12 nanofillers and nanocellulose scaffold collectively endow the thin‐layer (25 µm), ultralightweight (1.65 mg cm −2 ) CPE formation with an order of magnitude enhancement of the mechanical strength (13.84 MPa) and ionic conductivity (1.62 × 10 −4 S cm −1 ) as compared to the pristine polymer electrolyte, more importantly, the improved dimension stability up to 180 °C. Upon the integration of the hetero‐layered CPE with the iron hexacyanoferrate FeHCF cathode (1 mAh cm −2 ) and the Na foil, the cell model can achieve the room‐temperature cycling stability (93.73% capacity retention for 200 cycles) as well as the high temperature tolerance till 80 °C, which inspires a quantum leap toward the surface‐wetting‐agent‐free, energy‐dense, wide‐temperature‐range SSMB prototyping.

The lightweight solid electrolyte design in replacement of the flammable liquid electrolyte and polyolefin separator is the key of the energy-dense all-solid-state batteries (ASSBs) construction. However, the technological barriers of scalable manufacturing, retarded ionic conductivity at room temperature as well as the mechanical fragility upon the high-temperature operation restrict the ASSB deployment of practical relevance. In this study, an ultra-lightweight (1.67 mg cm-2), thin (25 mu m), high strength and thermally robust (stability up to 180 degrees C) composite solid electrolyte (CSE) has been designed to address the dilemma by the rational integration of polyethylene glycol monomethyl ethers coated Li6.4La3Zr1.4Ta0.6O12 nanofillers (MPEG@LLZTO) with light-weight nanocellulose scaffold. The MPEG coating layer enhances the interfacial compatibility and homogeneous dispersibility of LLZTO nanofiller within the poly (ethylene oxide) (PEO) matrix, while the mechanically flexible and thermally stable nanocellulose scaffold guarantees the formation of the high-temperature endurance and structural robustness for the as-formed CSE layer. Upon the solvent-free, layer stacked-up assembly of the PEO/ MPEG@LLZTO-Nanocellulose (PLCN) CSE film with the high-mass-loading LiFePO4 cathode and thin-layer lithium anode, the ASSB prototype could simultaneously realize the high gravimetric energy density (323 Wh kg -1), cycling stability as well as operation reliability within a wider temperature range (25 degrees C similar to 130 degrees C).

Helical structure in catalysts has attracted attention and been recently investigated for various catalytic reactions. However, helical transition metal oxides suffer from uncontrollable crystallization processes at high temperatures when being transformed from an amorphous phase into a crystalline structure. Herein, we report a helical anatase TiO2 nanotube for the first time, which has been prepared using a protected crystallization strategy in the confined space of silica. A single chirality of helical TiO2 has been used to track the ordering of the twisted structure. The twisted structure in helical anatase TiO2 nanotube is maintained after a vigorous crystallization process. Helical anatase TiO2 nanotubes possess more accessible active sites and abundant defects of oxygen vacancy and Ti3+ species owing to the twisted structure. The obtained helical anatase TiO2 nanotube exhibits superior photocatalytic activity for hydrogen production without adding any co-catalysts. This work provides new insights into the role of helical structure in transition metal-based catalysts.

Poly(ethylene oxide) (PEO)‐based solid polymer electrolyte promises interfacial compatibility with the high‐capacity metallic anodes in all‐solid‐state batteries (ASSBs). However, the prototype construction is severely hindered by the parasitic ohmic resistance at the electrode‐electrolyte interface, insufficient ionic pathway of the high loading cathode, as well as the PEO oxidation tendency at the high voltage. Herein, a laser‐assisted strategy is presented toward ultra‐efficient cathode modification (completes within 240 s) by constructing continuous, multi‐scale artificial cathode/electrolyte interface (CEI). The tailorable, yet localized temperature gradient induced by the pulsed laser beam can customize the CEI species from the target precursor salts for the on‐demand protection purpose. Derived from the tris(trimethylsilyl)phosphate, the proof‐of‐concept model achieves phosphorus‐rich, ion‐diffusion network across the high‐mass‐loading LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode, which enables the high‐rate operation of the ASSBs prototype as well as the extended shelf life at the oxidized idling state. Transmission‐mode operando X‐ray phase tracking unravels the electrochemical stability origin at the cathode/PEO interface due to the insulation of electron shuttling, where the layered to spinel phase transition and the lattice oxygen release are alleviated. This generic, readily tailorable, highly‐efficient laser processing strategy thus provides unprecedented opportunities to secure the varieties of energy‐dense, polymer‐based ASSBs.

Hard carbons (HCs) are extensively investigated as the potential anodes for commercialization of sodium-ion batteries (SIBs). However, the practical deployment of HC anode suffers from the retarded Na+ diffusion at the high-rate or low-temperature operation scenarios. Herein, a multiscale modification strategy by tuning HC microstructure on the particle level as well as replenishing extra Na+ reservoir for the electrode through a homogeneous presodiation therapy is presented. Consequently, the coulombic efficiency of HC anode can be precisely controlled till the close-to-unit value. Detailed kinetics analysis observes that the Na+ diffusivity can be drastically enhanced by two orders of magnitude at the low potential region (< 0.1 V vs. Na+ /Na), which accelerates the rate-limiting step. As pairing the presodiated HC anode (≈5.0 ± 0.2 mg cm-2 ) with the NaVPO4 F cathode (≈10.3 mg cm-2 ) in the 200 mAh pouch cell, the optimal balance of the cyclability (83% over 1000 cycles), low-temperature behavior till -40 °C as well as the maximized power output of 1500 W kg-1 can be simultaneously achieved. This synergistic modification strategy opens a new avenue to exploit the reversible, ultrafast Na+ storage kinetics of HC anodes, which thus constitutes a quantum leap forward toward high-rate SIB prototyping.

Electrode exploration with the appropriate equilibrium voltage and facile cation diffusion kinetics is the key enabler towards realizing the extreme power output of the battery formats. With the aid of the stepwise lattice tailoring, herein, we present an alternative fast-charging anode of the rock-salt lithium vanadium oxide. Specifically, the pre-insertion of polyaniline (PANI) molecules unlocks the basal plane of the layered V2O5 precursor, while subsequent Na+ doping at the octahedral sites could stabilize the lattice breathing and mitigate Li-ion diffusion barrier along the tetrahedron-octahedron-tetrahedron pathway, as confirmed by the operando X-ray diffraction and kinetics simulation. The Na0.6Li2.4V2O5@PANI//LiFePO4 full cell prototype (3 mAh cm−2) exhibits 82% capacity retention at 20 C for 2000 cycles, as well as the cycling endurance within a wider temperature range of 0-60°C. This stepwise lattice engineering strategy opens a fresh impetus of the electrode innovations for the high-power energy storage devices.

The practical deployment of metallic anodes in the energy-dense batteries is impeded by the thermodynamically unstable interphase in contact with the aprotic electrolyte,structural collapse of the substrates as well as their insufficient affinity toward the metallic deposits.Herein,the mechanical flexible,lightweight(1.2 mg cm-2)carbon nanofiber scaffold with the monodispersed,ultrafine Sn4P3 nanoparticles encapsulation(Sn4P3NPs@CNF)is proposed as the deposition substrate toward the high-areal-capacity sodium loadings up to 4 mAh cm-2.First-principles calculations manifest that the alloy intermediates,namely the Na15Sn4 and Na3P matrix,exhibit the intimate Na affinity as the"sodiophilic"sites.Meanwhile,the porous CNF regulates the heterogeneous alloying process and confines the deposit propagation along the nanofiber orientation.With the precise control of pairing mode with the NaVPO4F cathode(8.7 mg cm-2),the practical feasibility of the Sn4P3 NPs@CNF anode(1*Na excess)is demonstrated in 2 mAh single-layer pouch cell prototype,which achieves the 95.7％capacity retention for 150 cycles at various mechanical flexing states as well as balanced energy/power densities.

The scalable development of an environmentally adaptive and homogeneous Li+ supplementary route remains a formidable challenge for the existing prelithiation technologies, restricting the full potential of high-capacity anodes. In this study, we present a moisture-tolerant interfacial prelithiation approach through casting a hydrophobic poly(vinylidene-co-hexafluoropropylene) membrane blended with a deep-lithiated alloy (Li22Si5@C/PVDF-HFP) onto Si based anodes. This strategy could not only extend to various high-capacity anode systems (SiOx@C, hard carbon) but also align with industrial roll-to-roll assembly processes. By carefully adjusting the thickness of the prelithiation layer, the densely packed Si@C electrode (4.5 mAh cm-2) exhibits significantly improved initial Coulombic efficiency until a close-to-unit value, as well as extreme moisture tolerance (60% relative humidity). Furthermore, it achieves more than 10-fold enhancement of ionic conductivity across the electrode. As pairing the prelithiated Si@C anode with the LiNi0.8Co0.1Mn0.1O2 cathode, the 2 Ah pouch-format prototype balances an energy density of ∼371 Wh kg-1 and an extreme power output of 2450 W kg-1 as well as 83.8% capacity retention for 1000 cycles. The combined operando phase tracking and spatial arrangement analysis of the intermediate alloy elucidate that the enhanced Li utilization derives from the gradient stress dissipation model upon a spontaneous Li+ redistribution process.

The alarming resource shortage of the lithium battery supply chain has triggered new vitality to the close-loop recycling of retired batteries. As compared to hydrometallurgy or pyrometallurgy strategies for the cathode recovery, the proper use of degraded graphite anodes, featuring with the solvated Li+ intercalation and in-plane defect formation, is hitherto neglected. In this work, we propose a facile "green route" to extract values from spent graphite anode. Through elucidating the dynamic Li occupancy in graphite lattice, an up-scaling delamination protocol is developed with the aid of in-situ generated H-2 bubbles in the protic mixed solvent, to weaken van der Waals (vdW) bonding of the graphite interlayers and generate few-layer graphene flakes (similar to 2 nm); meanwhile high-purity Li salt could be simultaneously extracted from the residue solvent (similar to 98% Li leaching efficiency). Upon exquisite interfacial modification, the as-exfoliated graphene flakes tend to assemble with the Na2Ti6O13 (NTO) nanosheets as a layer-stacked, mechanical-flexible anode, which further demonstrates a robust cycling at various flexing states and extreme power output of 1142 Wkg(-1) as paired with the LiFePO4 cathode (5.3 mg cm(-2)) in the integrated, thin-film battery. This work vividly demonstrates potential add-value market of spent anodes in the flexible power sources.

Single-crystalline Ni-rich cathode active materials (CAMs) are considered as promising candidates for high-energy-density lithium-ion batteries (LIBs) with favorable cycling stability and safety, due to their grain boundaryless characteristics efficiently alleviate the structural degradation of intergranular microcracks in poly-crystalline counterparts. However, their practical application not only suffers from sluggish Li diffusion kinetics, surface reconstruction and parasitic cathode/electrolyte interfacial reactions upon repeated cycling but also encounters chemical instability during storage and slurry processes. Herein, we constructed a uniform LiAlO2/Li3PO4 protective layer with gradient Al doping (LAP modification) on the surface of single-crystalline LiNi0.90Co0.05Mn0.04Al0.01O2 (SCNCMA) CAMs through an in situ modification process to relieve these intrinsic instability issues. This advantageous surface engineering significantly reduces Li+/Ni2+ mixing, inhibits parasitic side reactions and surface phase transformation, and notably improves Li+ diffusion kinetics. Therefore, LAP-modified SCNCMA exhibits superior cycling performance with a capacity retention of 74.4% at a high voltage of 4.5 V after 200 cycles at 1C compared to that of SCNCMA. Moreover, the enhancement of air storage properties after modification was further confirmed by the reduced surface residual lithium, improved rheological properties and well-maintained electrochemical performance. This work provides an effective strategy for the modification of single-crystal Ni-rich cathodes and further accelerates their practical application.

The Si anodes suffer from the repetitive buildup of the solid electrolyte interphase, electrode pulverization upon the lithiation/delithiation process, as well as the Li trapping in the alloy intermediates. Herein, a facile electrostatic self-assembly process of the Si nanosheets (SiNS) and graphite microsheets (GMs) is proposed as a viable high-capacity composite anode. Upon the appropriate interfacial tailoring, the SiNS/GMs composite not only guarantees the intimate contact mode between the sand-milled Si nanosheets and the positively charged graphite sheets but also renders the enhanced electrode conductivity and high-rate performance (886.2 mAh g(-1) at current density of 5 Ag-1 ). In addition, the prelithiated SiNS/GMs (Pre-SiNS/GMs) are fabricated by spraying stabilized lithium metal powder (SLMP) at the predetermined amounts onto the electrodes, contributing to the improved initial Coulombic efficiency (ICE) of the half cell (99%). As the Pre-SiNS/GMs anodes are assembled with the diverse commercial cathodes, the full cell models reveal the balanced cycling endurance and the high gravimetric energy/power densities.