Hierarchical Engineering of Porous P2‐Na2/3Ni1/3Mn2/3O2 Nanofibers Assembled by Nanoparticles Enables Superior Sodium‐Ion Storage Cathodes

Layered transition metal oxides (TMOs) are appealing cathode candidates for sodium‐ion batteries (SIBs) by virtue of their facile 2D Na⁺ diffusion paths and high theoretical capacities but suffer from poor cycling stability. Herein, taking P2‐type Na_2/3Ni_1/3Mn_2/3O₂ as an example, it is demonstrated that the hierarchical engineering of porous nanofibers assembled by nanoparticles can effectively boost the reaction kinetics and stabilize the structure. The P2‐Na_2/3Ni_1/3Mn_2/3O₂ nanofibers exhibit exceptional rate capability (166.7 mA h g^?1 at 0.1 C with 73.4 mA h g^?1 at 20 C) and significantly improved cycle life (≈81% capacity retention after 500 cycles) as cathode materials for SIBs. The highly reversible structure evolution and Ni/Mn valence change during sodium insertion/extraction are verified by in operando X‐ray diffraction and ex situ X‐ray photoelectron spectroscopy, respectively. The facilitated electrode process kinetics are demonstrated by an additional study using the electrochemical measurements and density functional theory computations. More impressively, the prototype Na‐ion full battery built with a Na_2/3Ni_1/3Mn_2/3O₂ nanofibers cathode and hard carbon anode delivers a promising energy density of 212.5 Wh kg^?1. The concept of designing a fibrous framework composed of small nanograins offers a new and generally applicable strategy for enhancing the Na‐storage performance of layered TMO cathode materials.     

High‐Performance Manganese Hexacyanoferrate with Cubic Structure as Superior Cathode Material for Sodium‐Ion Batteries

Sodium manganese hexacyanoferrate (Na_xMnFe(CN)₆) is one of the most promising cathode materials for sodium‐ion batteries (SIBs) due to the high voltage and low cost. However, its cycling performance is limited by the multiple phase transitions during Na⁺ insertion/extraction. In this work, a facile strategy is developed to synthesize cubic and monoclinic structured Na_xMnFe(CN)₆, and their structure evolutions are investigated through in situ X‐ray diffraction (XRD), ex situ Raman, and X‐ray photoelectron spectroscopy (XPS) characterizations. It is revealed that the monoclinic phase undergoes undesirable multiple two‐phase reactions (monoclinic ? cubic ? tetragonal) due to the large lattice distortions caused by the Jahn–Teller effects of Mn³⁺, resulting in poor cycling performances with 38% capacity retention. The cubic Na_xMnFe(CN)₆ with high structural symmetry maintains the structural stability during the repeated Na⁺ insertion/extraction process, demonstrating impressive electrochemical performances with specific capacity of ≈120 mAh g^?1 at 3.5 V (vs Na/Na⁺), capacity retention of ≈70% over 500 cycles at 200 mA g^?1. In addition, the TiO₂//C‐MnHCF full battery is fabricated with an energy density of 111 Wh kg^?1, suggesting the great potential of cubic Na_xMnFe(CN)₆ for practical energy storage applications.     

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.     

Biphase Cobalt–Manganese Oxide with High Capacity and Rate Performance for Aqueous Sodium‐Ion Electrochemical Energy Storage

Manganese‐based metal oxide electrode materials are of great importance in electrochemical energy storage for their favorable redox behavior, low cost, and environmental friendliness. However, their storage capacity and cycle life in aqueous Na‐ion electrolytes is not satisfactory. Herein, the development of a biphase cobalt–manganese oxide (Co? Mn? O) nanostructured electrode material is reported, comprised of a layered MnO₂?H₂O birnessite phase and a (Co_0.83Mn_0.13Va_0.04)_tetra(Co_0.38Mn_1.62)_octaO_3.72 (Va: vacancy; tetra: tetrahedral sites; octa: octahedral sites) spinel phase, verified by neutron total scattering and pair distribution function analyses. The biphase Co? Mn? O material demonstrates an excellent storage capacity toward Na‐ions in an aqueous electrolyte (121 mA h g^?1 at a scan rate of 1 mV s^?1 in the half‐cell and 81 mA h g^?1 at a current density of 2 A g^?1 after 5000 cycles in full‐cells), as well as high rate performance (57 mA h g^?1 a rate of 360 C). Electrokinetic analysis and in situ X‐ray diffraction measurements further confirm that the synergistic interaction between the spinel and layered phases, as well as the vacancy of the tetrahedral sites of spinel phase, contribute to the improved capacity and rate performance of the Co? Mn? O material by facilitating both diffusion‐limited redox and capacitive charge storage processes.     

Manipulating the Electronic Structure of Li‐Rich Manganese‐Based Oxide Using Polyanions: Towards Better Electrochemical Performance

Lithium‐rich manganese‐based layered oxides show great potential as high‐capacity cathode materials for lithium ion batteries, but usually exhibit a poor cycle life, gradual voltage drop during cycling, and low thermal stability in the highly delithiated state. Herein, a strategy to promote the electrochemical performance of this material by manipulating the electronic structure through incorporation of boracic polyanions is developed. As‐prepared Li[Li_0.2Ni_0.13Co_0.13Mn_0.54](BO₄)_0.015(BO₃)_0.005O_1.925 shows a decreased M‐O covalency and a lowered O 2p band top compared with pristine Li[Li_0.2Ni_0.13Co_0.13Mn_0.54]O₂. As a result, the modified cathode exhibits a superior reversible capacity of 300 mA h g^?1 after 80 cycles, excellent cycling stability with a capacity retention of 89% within 300 cycles, higher thermal stability, and enhanced redox couple potentials. The improvements are correlated to the enhanced oxygen stability that originates from the tuned electronic structure. This facile strategy may further be extended to other high capacity electrode systems.     

Functional Passivation Interface of LiNi0.8Co0.1Mn0.1O2 toward Superior Lithium Storage

The fast capacity/voltage fading with a low rate capability has challenged the commercialization of layer-structured Ni-rich cathodes in lithium-ion batteries. In this study, an ultrathin and stable interface of LiNi_0.8Mn_0.1Co_0.1O₂ (NCM) is designed via a passivation strategy, dramatically enhancing the capacity retention and operating voltage stability of cathode at a high cut-off voltage of 4.5 V. The rebuilt interface as a stable path for Li⁺ transport, would strengthen the cathode–electrolyte interface stability, and restrain the detrimental factors for cathode–electrolyte interfacial reactions, intergranular cracking and irreversible phase transformation from layered to spinel, even salt-rock phase. The as-optimized NCM displays a higher cyclability (i.e., 206.6 mA h g⁻¹ at 0.25 C (50 mA g⁻¹) with 92.0% capacity retention over 100 cycles) and a better rate capability (141.0 and 112.6 mA h g⁻¹ at 12.5 and 25 C, respectively) than pristine NCM (205.0 mA h g⁻¹ with 73.0% capacity retention at 0.25 C; 120.9 and 93.1 mA h g⁻¹ at 12.5 and 25 C, respectively).     

Catalytic Conversion of Polysulfides on Single Atom Zinc Implanted MXene toward High‐Rate Lithium–Sulfur Batteries

Although lithium–sulfur (Li–S) batteries are one of the most promising energy storage devices owing to their high energy densities, the sluggish reaction kinetics and severe shuttle effect of the sulfur cathodes hinder their practical applications. Here, single atom zinc implanted MXene is introduced into a sulfur cathode, which can not only catalyze the conversion reactions of polysulfides by decreasing the energy barriers from Li₂S₄ to Li₂S₂/Li₂S but also achieve strong interaction with polysulfides due to the high electronegativity of atomic zinc on MXene. Moreover, it is found that the homogenously dispersed zinc atoms can also accelerate the nucleation of Li₂S₂/Li₂S on MXene layers during the redox reactions. As a result, the sulfur cathode with single atom zinc implanted MXene exhibits a high reversible capacity of 1136 mAh g^?1. After electrode optimization, a high areal capacity of 5.3 mAh cm^?2, high rate capability of 640 mAh g^?1 at 6 C, and good cycle stability (80% capacity retention after 200 cycles at 4 C) can be achieved.     

Faster Activation and Slower Capacity/Voltage Fading: A Bifunctional Urea Treatment on Lithium‐Rich Cathode Materials

Li‐rich layered oxides are promising cathode materials for next‐generation Li‐ion batteries because of their extraordinary specific capacity. However, the activation process of the key active component Li₂MnO₃ in Li‐rich materials is kinetically slow, and the complex phase transformation with electrode/electrolyte side reactions causes fast capacity/voltage fading. Herein, a simple thermal treatment strategy is reported to simultaneously tackle these challenges. The introduction of a urea thermal treatment on Li‐rich material Li_1.87Mn_0.94Ni_0.19O₃ leads to oxygen deficiencies and partially reduced Mn ions on the oxide surface for activating the Li‐rich phase. In situ synchrotron study confirms that the urea‐treated cathode shows much faster Li extraction from both Li and transition metal layers with less oxygen evolution upon charging than that of untreated counterparts. Moreover, the decomposition products of urea during thermal treatment subsequently deposit on the surface of cathode material, leading to a unique passivation layer against side reactions between electrode and electrolyte. Soft X‐ray absorption spectroscopy reveals the structural evolution mechanism with a significantly suppressed dissolution of Mn species over cycling measurement. The urea‐treated Li_1.87Mn_0.94Ni_0.19O₃ shows accelerated activation kinetics to reach high capacity of 270 mA h g^–1 and demonstrates excellent capacity retention of 98.49% over 300 cycles with slower voltage decay.     

Inhibition of Manganese Dissolution in Mn2O3 Cathode with Controllable Ni2+ Incorporation for High-Performance Zinc Ion Battery

Manganese-based materials are considered potential cathode materials for aqueous zinc ion batteries (ZIBs). However, the dissolution of manganese leading to an abrupt decline of capacity and the sluggish electrochemical reaction kinetics are still the main bottlenecks restricting their further development. Herein, a NiMn-layered double hydroxide-derived Ni-doped Mn₂O₃ (NM) is developed to suppress the dissolution of manganese. The incorporation of Ni²⁺ can promote electronic rearrangement and enhance the conductivity, ultimately improving the reaction kinetics and electrochemical performance of the NM. Moreover, the doped Ni²⁺ can effectively stabilize the Mn O bond of Mn₂O₃ by reducing the formation energy. In addition, the storage mechanism based on the simultaneous insertion and transformation of H⁺ and Zn²⁺ is demonstrated. Interestingly, the Ni-doped Mn₂O₃ shows a high specific capacity of 252 mAh g^–1 (0.1 A g^–1), three times more than the pure Mn₂O₃ (72 mAh g^–1). The capacity retention (≈85.6% over 2500 cycles at 1.0 A g^–1) is also more excellent when comparing with the Mn₂O₃ cathode (≈49.7%). Significantly, an ultra-high energy density of 327.6 Wh kg^–1 has been achieved using Ni-doped Mn₂O₃ cathode, which suggests that the synergistic effect of manganese and other transition metal ions provide a promising strategy for future development of ZIBs.     

Sulfurized Polyacrylonitrile Cathodes with High Compatibility in Both Ether and Carbonate Electrolytes for Ultrastable Lithium–Sulfur Batteries

Sulfurized polyacrylonitrile (SPAN) is a promising material capable of suppressing polysulfide dissolution in lithium–sulfur (Li–S) batteries with carbonate electrolyte. However, undesirable spontaneous formation of soluble polysulfides may arise in the ether electrolyte, and the conversion of sulfur in SPAN during the lithiation/delithiation processes is yet to be understood. Here, a highly reliable Li–S system using a freestanding fibrous SPAN cathode, as well as the sulfur conversion mechanism involved, is demonstrated. The SPAN shows high compatibility in both ether and carbonate electrolytes. The sulfur atoms existing in the form of short ? S₂? and ? S₃? chains are covalently bonded to the pyrolyzed PAN backbone. The electrochemical reduction of the SPAN by Li⁺ is a single‐phase solid–solid reaction with Li₂S as the sole discharge product. Meanwhile, the parasitic reaction between Li⁺ and C?N bonds exists upon the first discharge, and the residual Li⁺ enhances the conductivity of the backbone. The recharge ability and rate capability are kinetically dominated by the activation of Li₂S nanoflakes generated during discharge. At 800 mA g^?1, a specific capacity of 1180 mAh g^?1 is realized without capacity fading in the measured 1000 cycles, which makes SPAN promising for practical application.     

Synergistically Assembled Li2S/FWNTs@Reduced Graphene Oxide Nanobundle Forest for Free‐Standing High‐Performance Li2S Cathodes

Lithium sulfide (Li₂S) has attracted increasing attention as a promising cathode because of its compatibility with more practical lithium‐free anode materials and its high specific capacity. However, it is still a challenge to develop Li₂S cathodes with low electrochemical overpotential, high capacity and reversibility, and good rate performance. This work designs and fabricates a practical Li₂S cathode composed of Li₂S/few‐walled carbon nanotubes@reduced graphene oxide nanobundle forest (Li₂S/FWNTs@rGO NBF). Hierarchical nanostructures are obtained by annealing the Li₂SO₄/FWNTs@GO NBF, which is prepared by a facile and scalable solution‐based self‐assembly method. Systematic characterizations reveal that in this unique NBF nanostructure, FWNTs act as axial shafts to direct the structure, Li₂S serves as the internal active material, and GO sheets provide an external coating to minimize the direct contact of Li₂S with the electrolyte. When used as a cathode, the Li₂S/FWNTs@rGO NBF achieve a high capacity of 868 mAh g^?1_Li2S at 0.2C after 300 cycles and an outstanding rate performance of 433 mAh g^?1_Li2S even at 10C, suggesting that this Li₂S cathode is a promising candidate for ultrafast charge/discharge applications. The design and synthetic strategies outlined here can be readily applied to the processing of other novel functional materials to obtain a much wider range of applications.     

A New Strategy to Build a High‐Performance P′2‐Type Cathode Material through Titanium Doping for Sodium‐Ion Batteries

Herein, Ti⁴⁺ in P′2‐Na_0.67[(Mn_0.78Fe_0.22)_0.9Ti_0.1]O₂ is proposed as a new strategy for optimization of Mn‐based cathode materials for sodium‐ion batteries, which enables a single phase reaction during de‐/sodiation. The approach is to utilize the stronger Ti–O bond in the transition metal layers that can suppress the movements of Mn–O and Fe–O by sharing the oxygen with Ti by the sequence of Mn–O–Ti–O–Fe. It delivers a discharge capacity of ≈180 mAh g^?1 over 200 cycles (86% retention), with S‐shaped smooth charge–discharge curves associated with a small volume change during cycling. The single phase reaction with a small volume change is further confirmed by operando synchrotron X‐ray diffraction. The low activation barrier energy of ≈541 meV for Na⁺ diffusion is predicted using first‐principles calculations. As a result, Na_0.67[(Mn_0.78Fe_0.22)_0.9Ti_0.1]O₂ can deliver a high reversible capacity of ≈153 mAh g^?1 even at 5C (1.3 A g^?1), which corresponds to ≈85% of the capacity at 0.1C (26 mA g^?1). The nature of the sodium storage mechanism governing the ultrahigh electrode performance in a full cell with a hard carbon anode is elucidated, revealing the excellent cyclability and good retention (≈80%) for 500 cycles (111 mAh g^?1) at 5C (1.3 A g^?1).     

Comprehensively Strengthened Metal-Oxygen Bonds for Reversible Anionic Redox Reaction

Introducing anionic redox in layered oxides is an effective approach to breaking the capacity limit of conventional cationic redox. However, the anionic redox reaction generally suffers from excessive oxidation of lattice oxygen to O₂ and O₂ release, resulting in local structural deterioration and rapid capacity/voltage decay. Here, a Na_0.71Li_0.22Al_0.05Mn_0.73O₂ (NLAM) cathode material is developed by introducing Al³⁺ into the transition metal (TM) sites. Thanks to the strong Al–O bonding strength and small Al³⁺ radius, the TMO₂ skeleton and the holistic TM–O bonds in NLAM are comprehensively strengthened, which inhibits the excessive lattice oxygen oxidation. The obtained NLAM exhibits a high reversible capacity of 194.4 mAh g^-1 at 20 mA g^-1 and decent cyclability with 98.6% capacity retention over 200 cycles at 200 mA g⁻¹. In situ characterizations reveal that the NLAM experiences phase transitions with an intermediate OP4 phase during the charge–discharge. Theoretical calculations further confirm that the Al substitution strategy is beneficial for improving the overlap between Mn 3d and O 2p orbitals. This finding sheds light on the design of layered oxide cathodes with highly reversible anionic redox for sodium storage.     

High‐Voltage LiNi0.45Cr0.1Mn1.45O4 Cathode with Superlong Cycle Performance for Wide Temperature Lithium‐Ion Batteries

Spinel LiNi_0.45Cr_0.1Mn_1.45O₄ synthesized by a scalable solution route combined by high temperature calcination is investigated as cathode for ultralong‐life lithium‐ion batteries in a wide operating temperature range. Scanning electron microscopy reveals homogeneous microsized polyhedral morphology with highly exposed {100} and {111} surfaces. The most highlighted result is that LiNi_0.45Cr_0.1Mn_1.45O₄ has extremely long cycle performance and high capacity retention at various temperatures (0, 25, 50 °C), indicating that Cr doping is a prospective approach to enable 5 V LiNi_0.5Mn_1.5O₄ (LNMO)‐based cathode materials with excellent cycling performances for commercial applications. After 1000 cycles, the capacity retention of LiNi_0.45Cr_0.1Mn_1.45O₄ is 100.30% and 82.75% at 0 °C and 25 °C at 1 C rate, respectively. Notably, over 350 cycles at 50 °C, the capacity retention of LiNi_0.45Cr_0.1Mn_1.45O₄ can maintain up to 91.49% at 1 C. All the values are comparable to pristine LNMO, which can be attributed to the elimination of Li_yNi_1?yO impurity phase, highly exposed {100} surfaces, less Mn³⁺ ions, and enhancement of ion and electron conductivity by Cr doping. Furthermore, an assembled LiNi_0.45Cr_0.1Mn_1.45O₄/Li₄Ti₅O₁₂ full cell delivers an initial discharge capacity of 101 mA h g^?1, meanwhile the capacity retention is 82.07% after 100 cycles.     

Tuning Anionic Redox Activity and Reversibility for a High‐Capacity Li‐Rich Mn‐Based Oxide Cathode via an Integrated Strategy

When fabricating Li‐rich layered oxide cathode materials, anionic redox chemistry plays a critical role in achieving a large specific capacity. Unfortunately, the release of lattice oxygen at the surface impedes the reversibility of the anionic redox reaction, which induces a large irreversible capacity loss, inferior thermal stability, and voltage decay. Therefore, methods for improving the anionic redox constitute a major challenge for the application of high‐energy‐density Li‐rich Mn‐based cathode materials. Herein, to enhance the oxygen redox activity and reversibility in Co‐free Li‐rich Mn‐based Li_1.2Mn_0.6Ni_0.2O₂ cathode materials by using an integrated strategy of Li₂SnO₃ coating‐induced Sn doping and spinel phase formation during synchronous lithiation is proposed. As an Li⁺ conductor, a Li₂SnO₃ nanocoating layer protects the lattice oxygen from exposure at the surface, thereby avoiding irreversible oxidation. The synergy of the formed spinel phase and Sn dopant not only improves the anionic redox activity, reversibility, and Li⁺ migration rate but also decreases Li/Ni mixing. The 1% Li₂SnO₃‐coated Li_1.2Mn_0.6Ni_0.2O₂ delivers a capacity of more than 300 mAh g^?1 with 92% Coulombic efficiency. Moreover, improved thermal stability and voltage retention are also observed. This synergic strategy may provide insights for understanding and designing new high‐performance materials with enhanced reversible anionic redox and stabilized surface lattice oxygen.     

Mn-Rich Phosphate Cathode for Sodium-Ion Batteries: Anion-Regulated Solid Solution Behavior and Long-Term Cycle Life

As a sodium superionic conductor, Mn-rich phosphate of Na_3.4Mn_1.2Ti_0.8(PO₄)₃ is considered as one of the promising cathodes for sodium-ion batteries owing to its good thermodynamic stability and high working voltage. However, Na_3.4Mn_1.2Ti_0.8(PO₄)₃ is faced with low electronic conductivity, poor cycling stability and complex phase transition caused by multi-electron transfers, which limits its practical application. Herein, an anion-regulated strategy is proposed to optimize the Mn-rich Na_3.4Mn_1.2Ti_0.8(PO₄)₃ phosphate cathode. After introducing F anions into the lattice, the rate performance is improved from 60.5 to 72.8 mAh g⁻¹ at 20 C. Ascribed to unique structure design, the reaction kinetics of Na_3.4Mn_1.2Ti_0.8(PO₄)₃ are significantly improved, as demonstrated by cyclic voltammetry at varied scan rates and galvanostatic intermittent titration technique. The generated M-F bond inhibits Jahn–Teller effect with an improved cycle stability (85.8 mAh g⁻¹ after 1000 cycles at 5 C with 94.3% capacity retention). Interestingly, reaction mechanism of Na_3.4Mn_1.2Ti_0.8(PO₄)₃ with the complex two-phase and solid solution reactions changes to the whole solid solution reaction after fluorine substitution, and leads to a smaller volume change of 5.41% during reaction processes, which is verified by in situ X-ray diffraction. This anion regulation strategy provides a new method for designing the high-performance phosphate cathode materials of sodium-ion batteries.     

Layered P2‐Type K0.44Ni0.22Mn0.78O2 as a High‐Performance Cathode for Potassium‐Ion Batteries

Potassium‐ion batteries (KIBs) are emerging as one of the most promising candidates for large‐scale energy storage owing to the natural abundance of the materials required for their fabrication and the fact that their intercalation mechanism is identical to that of lithium‐ion batteries. However, the larger ionic radius of K⁺ is likely to induce larger volume expansion and sluggish kinetics, resulting in low specific capacity and unsatisfactory cycle stability. A new Ni/Mn‐based layered oxide, P2‐type K_0.44Ni_0.22Mn_0.78O₂, is designed and synthesized. A cathode designed using this material delivers a high specific capacity of 125.5 mAh g^?1 at 10 mA g^?1, good cycle stability with capacity retention of 67% over 500 cycles and fast kinetic properties. In situ X‐ray diffraction recorded for the initial two cycles reveals single solid‐solution processes under P2‐type framework with small volume change of 1.5%. Moreover, a cathode electrolyte interphase layer is observed on the surface of the electrode after cycling with possible components of K₂CO₃, RCO₂K, KOR, KF, etc. A full cell using K_0.44Ni_0.22Mn_0.78O₂ as the cathode and soft carbon as the anode also exhibits exceptional performance, with capacity retention of 90% over 500 cycles as well as superior rate performance. These findings suggest P2‐K_0.44Ni_0.22Mn_0.78O₂ is a promising candidate as a high‐performance cathode for KIBs.     

Approaching the Downsizing Limit of Maricite NaFePO4 toward High‐Performance Cathode for Sodium‐Ion Batteries

Maricite NaFePO₄ nanodots with minimized sizes (≈1.6 nm) uniformly embedded in porous N‐doped carbon nanofibers (designated as NaFePO₄@C) are first prepared by electrospinning for maximized Na‐storage performance. The obtained flexible NaFePO₄@C fiber membrane adherent on aluminum foil is directly used as binder‐free cathode for sodium‐ion batteries, revealing that the ultrasmall nanosize effect as well as a high‐potential desodiation process can transform the generally perceived electrochemically inactive maricite NaFePO₄ into a highly active amorphous phase; meanwhile, remarkable electrochemical performance in terms of high reversible capacity (145 mA h g^?1 at 0.2 C), high rate capability (61 mA h g^?1 at 50 C), and unprecedentedly high cyclic stability (≈89% capacity retention over 6300 cycles) is achieved. Furthermore, the soft package Na‐ion full battery constructed by the NaFePO₄@C nanofibers cathode and the pure carbon nanofibers anode displays a promising energy density of 168.1 Wh kg^?1 and a notable capacity retention of 87% after 200 cycles. The distinctive 3D network structure of very fine NaFePO₄ nanoparticles homogeneously encapsulated in interconnected porous N‐doped carbon nanofibers, can effectively improve the active materials' utilization rate, facilitate the electrons/Na⁺ ions transport, and strengthen the electrode stability upon prolonged cycling, leading to the fascinating Na‐storage performance.     

Targeted Synergy between Adjacent Co Atoms on Graphene Oxide as an Efficient New Electrocatalyst for Li–CO2 Batteries

Li–CO₂ batteries are an attractive technology for converting CO₂ into energy. However, the decomposition of insulating Li₂CO₃ on the cathode during discharge is a barrier to practical application. Here, it is demonstrated that a high loading of single Co atoms (≈5.3%) anchored on graphene oxide (adjacent Co/GO) acts as an efficient and durable electrocatalyst for Li–CO₂ batteries. This targeted dispersion of atomic Co provides catalytically adjacent active sites to decompose Li₂CO₃. The adjacent Co/GO exhibits a highly significant sustained discharge capacity of 17 358 mA h g^?1 at 100 mA g^?1 for >100 cycles. Density functional theory simulations confirm that the adjacent Co electrocatalyst possesses the best performance toward the decomposition of Li₂CO₃ and maintains metallic‐like nature after the adsorption of Li₂CO₃.     

All-Climate Iron-Based Sodium-Ion Full Cell for Energy Storage

The anode materials for sodium-ion batteries (SIBs) such as soft carbon, hard carbon, or alloys suffer from low specific capacity, poor rate capability, and high cost. Various transition metal oxides materials possess high specific capacity and suitable working potential, however, huge volume change and unstable electrode/electrolyte interfaces limit their practical applications. Herein, an ultrathin carbon-coated iron-based borate, (Fe₃BO₅), as an anode material for SIBs is reported. The carbon coated Fe₃BO₅ composite as an anode material possesses a reversible specific capacity of 548 mAh g⁻¹ with a high initial coulombic efficiency of 72.6% at a current density of 50 mA g⁻¹, and maintains a capacity retention ratio of 99% after 1000 cycles at 2000 mA g⁻¹. Moreover, this anode can work well over a wide temperature range (-40–60 °C). Furthermore, a sodium-ion full cell using this anode coupling with iron-based cathode (Na₃Fe₂(PO₄)₂(P₂O₇)@rGO) cathode is fabricated, which exhibits a wide operating temperature range from −40 to 60 °C with a maximum energy density of 175 Wh Kg⁻¹ and a maximum power density of 1680 W Kg⁻¹. Most importantly, this full-cell configuration is low-cost due to its inexpensive iron based raw material for both anode and cathode.