Abstract A high capacity cathode is the key to realization of high‐energy‐density lithium‐ion batteries. The anionic oxygen redox induced by activation Li 2 MnO 3 domain has previously afforded an O3‐type layered Li‐rich material used as for batteries with a notably 250–300 mAh g −1 . However, its practical application in been limited due electrodes made from this suffering severe voltage fading and decay during cycling. Here, it shown that O2‐type single‐layer superstructure can deliver...

Bi-functional N -methylurea molecules participate in co-solvating the Li + ions enhancing ionic conductivity, and deactivate non-solvating polymer ethereal groups through amide acceptor, providing a wide electrochemical window.

Layered Li-rich cathode materials with high reversible energy densities are becoming prevalent. However, owing to the activation of low-potential redox couples and progressively irreversible structural transformation caused by local adjustment transition-metal ions in intra/interlayer driven anionic redox, continuous capacity degradation, voltage decay emerge, thus greatly reducing density increasing difficulty battery system management. Herein, layered higher intralayer configuration...

Lithium-rich transition metal oxides (LLOs) can deliver high specific capacity over 250 mAh g-1 , stemming from additional contribution of oxygen redox. However, the formation O(2-n)- (0 < n 2) species and even gas during deep oxidation stage leads to progressive structural transformation that cause voltage decay/hysteresis, sluggish kinetics, poor thermostability, preventing real-world application LLOs. Therefore, substantive key relies on enhancing anionic redox stability in Here, a...

Abstract Lithium-manganese-oxides have been exploited as promising cathode materials for many years due to their environmental friendliness, resource abundance and low biotoxicity. Nevertheless, inevitable problems, such Jahn-Teller distortion, manganese dissolution phase transition, still frustrate researchers; thus, progress in full manganese-based (FMCMs) has relatively slow limited recent decades. Recently, with the fast growth of vehicle electrification large-scale energy-storage grids,...

Lithium-rich Mn-based oxides have gained significant attention worldwide as potential cathode materials for the next generation of high-energy density lithium-ion batteries. Nonetheless, inferior rate capability and voltage decay issues present formidable challenges. Here, a Li-rich material equipped with quasi-three-dimensional (quasi-3D) Li-ion diffusion channels is initially synthesized by introducing twin structures high coefficients into crystal constructing "bridge" between different...

Controlling multimetallic ensembles at the atomic level is significantly challenging, particularly for high-entropy alloys with more than five elements. Herein, we report an innovative ultrasmall (∼2 nm) PtFeCoNiCuZn intermetallic (PFCNCZ-HEI) a well-ordered structure synthesized by using space-confined strategy. By exploiting these combined metals, PFCNCZ-HEI nanoparticles achieve ultrahigh mass activity of 2.403 A mgPt–1 0.90 V vs reversible hydrogen electrode oxygen reduction reaction,...

Layered Li-rich oxides (LROs) that exhibit anionic and cationic redox are extensively studied due to their high energy storage capacities. However, voltage hysteresis, which reduces the conversion efficiency of battery, is a critical limitation in commercial application LROs. Herein, using two Li2RuO3 (LRO) model materials with C2/c P21/m symmetries, we explored relationship between hysteresis electronic structure by neutron diffraction, situ X-ray powder absorption spectroscopy, macro...

Abstract Nickel-rich layered transition metal oxides are leading cathode candidates for lithium-ion batteries due to their increased capacity, low cost and enhanced environmental sustainability compared cobalt formulations. However, the nickel enrichment comes with larger volume change during cycling as well reduced oxygen stability, which can both incur performance degradation. Here we show an ultrahigh-nickel cathode, LiNi 0.94 Co 0.05 Te 0.01 O 2 , that addresses all of these critical...

Abstract To improve the interface stability between Li-rich Mn-based oxide cathodes and electrolytes, it is necessary to develop new polymer electrolytes. Here, we report an entanglement association electrolyte (PVFH-PVCA) based on a poly (vinylidene fluoride-co-hexafluoropropylene) (PVFH) matrix copolymer stabilizer (PVCA) prepared from acrylonitrile, maleic anhydride, vinylene carbonate. The entangled structure of PVFH-PVCA imparts excellent mechanical properties eliminates stress arising...

Abstract Li‐rich NMCs layered oxides, with the general formula of Li[Li x Ni y Mn z Co 1− − ]O 2 , are known for their exceptionally high capacities but remain yet to be practicalized in real world. They have attracted enormous research attention due complex structure and intriguing redox mechanisms, a particular focus on anionic over past decade. While fundamental understandings fruitful, practical considerations emphasized here by providing perspectives how limited roadblocks guidelines...

Anion dimerization poses a significant challenge for the application of Li-rich cathode materials (LCMs) in high-energy-density Li-ion batteries because its deleterious effects, including rapid capacity and voltage decay, sluggish reaction kinetics, large hysteresis. Herein, we propose metal–ligand spin-lock strategy to inhibit anion dimerization, which involves introducing an Fe–Ni couple having antiferromagnetic superexchange interaction into LCM lock spin orientations unpaired electrons...

High energy density Li-S batteries are highly attractive. However, their use in practical applications has been greatly affected by poor cycle life and low rate performance, which can be partly attributed to the dissolution of polysulfides from S cathode migration Li anode through separator. While much effort devoted designing structure cathodes for suppressing polysulfides, relatively little emphasis placed on modifying Herein, we demonstrate a new approach separator with polyvinylidene...

The search for new high-performance and low-cost cathode materials Li-ion batteries is a challenging issue in research. Commonly used cobalt- or nickel-based cathodes suffer from limited resources safety problems that greatly restrict their large-scale application, especially electric vehicles energy storage. Here, novel Li-Mn-O Li-rich material with R3¯m symmetry developed via intralayer Li/Mn disordering the Mn-layer. Due to special atomic arrangement higher respect C2/m symmetry, oxygen...

Abstract Li-rich layered oxide cathode materials show high capacities in lithium-ion batteries owing to the contribution of oxygen redox reaction. However, structural accommodation this reaction usually results O–O dimerization, leading release and poor electrochemical performance. In study, we propose a new response mechanism inhibiting dimerization for by tuning local symmetry around ions. Compared with regular Li 2 RuO 3 , as-prepared local-symmetry-tuned involves telescopic O–Ru–O...

Abstract Nano-ordered intermetallic compounds have generated great interest in fuel cell applications. However, the synthesis of non-preciousearly transition metal nanoparticles remains a formidable challenge owing to extremely oxyphilic nature and very negative reduction potentials. Here, we successfully synthesized non-precious Co 3 Ta nanoparticles, with uniform size 5 nm. Atomic structural characterizations X-ray absorption fine structure measurements confirm atomically ordered...

Developing highly active, low-cost, and durable catalysts for efficient oxygen reduction reactions remain a challenge, hindering the commercial viability of proton exchange membrane fuel cells (PEMFCs). In this study, an ordered PtZnFeCoNiCr high-entropy intermetallic electrocatalyst with Pt antisite point defects (PD-PZFCNC-HEI) is synthesized. The shows high mass activity 4.12 A mgPt-1 toward reaction (ORR), which 33 times that Pt/C. PEMFC, assembled PD-PZFCNC-HEI as cathode (0.05 mgPt...

Abstract Anionic redox processes are vital to realize high capacity in lithium‐rich electrodes of lithium‐ion batteries. However, the activation mechanism these remains ambiguous, hampering further implementation new electrode design. This study demonstrates that electrochemical activity inert cubic‐Li 2 TiO 3 is triggered by Fe 3+ substitution, afford considerable oxygen activity. Coupled with first principles calculations, it found electron holes tend be selectively generated on ions...

Recently, more and new high-capacity lithium-rich layered oxides involving both metal oxygen redox have been proposed. However, the structural stability was influenced by irreversible redox, which leads to instability of framework. Here, we propose that reversibility in Li2RuO3 can be controlled tuning its electronic structure via incorporating boron atoms into interstitial sites obtain higher-stability oxides. Using situ X-ray diffraction absorption fine structure, conclude tuned a...

Continued improvement in the electrochemical performance of Li-Mn-O oxide cathode materials is key to achieving advanced low-cost Li-ion batteries with high energy densities. In this study, O2-type Li0.78[Li0.24Mn0.76]O2 nanowires were synthesized by a solvothermal reaction produce P2-type Na5/6[Li1/4Mn3/4]O2 nanowires, which then subjected molten salt exchange. The resulting have diameters less than 20 nm and lengths several micrometers. full-Mn-based material delivers reversible capacity...

Lithium-rich layered oxides are promising cathode materials for high-energy-density lithium-ion batteries. However, the development of based on these has been limited by voltage fading, poor rate performance, and low tap density materials. In this work, we prepared a material consisting micrometer-scale spherical lithium-rich oxide particles with three-dimensional conductivity network design modified surface primary ruthenium. The as-obtained product maximum 2.1 g cm–3 shows superior high...

Abstract Li‐rich oxide (LRO) cathodes that exhibit anionic redox activity can boost the energy density of Li‐ion batteries. Oxygen in LROs originate from charge compensation pure O 2p nonbonding (NB) states; however, high charging voltages cause much safety concerns practical applications. Exploiting new modes be used at low is thus imperative. In view this, a further understanding behavior with respect to metal‐ligand interactions highly desired. this study, by analyzing orbital...