Entropy-Driven Hybrid Gel Electrolyte Enables Practical High-Voltage Lithium Metal Batteries.

Electrolyte engineering plays a crucial role in enhancing the performance of lithium metal batteries (LMBs) featuring high-voltage cathodes and limited lithium anodes, thereby unlocking their potential for high-energy electrochemical storage. Herein, an entropy-driven hybrid gel electrolyte with enhanced diversity in Li-ion solvation structures is designed by incorporating substantial amounts of insoluble LiPO2F2 and LiNO3 salts into LiPF6-based carbonate electrolytes, followed by in situ thermal polymerization. Specifically, the Li+ solvation structures are modulated via ionophilic NO3- and PO2F2- to generate an anion-rich solvation sheath and thus promote anion reduction at the electrode-electrolyte interface. The interfaces enriched in anion-derived inorganic components facilitate rapid ionic transport, thus enabling smooth and dense Li morphology and ultimately enhancing the electrochemical performance of LMBs. As a result, this high-hybrid gel electrolyte confers LMBs employing high-voltage NCM cathodes, as demonstrated by sustained performance in both coin-cell (500 cycles at 4.5 V) and Ah-level pouch cell configurations under practical conditions (60 cycles, N/P: 1.92, and E/C: 2.0 g Ah -1).

Molten-Salt-Assisted Strategy Enables High-Rate Micron-Sized Single-Crystal Li-Rich, Mn-Based Layered Oxide Cathode Materials.

Li-rich Mn-based layered oxides (LMLOs) are expected to be the most promising high-capacity cathodes for the next generation of lithium-ion batteries (LIBs). However, the poor cycling stability and kinetics performance of polycrystalline LMLOs restrict their practical applications due to the anisotropic lattice stress and crack propagation during cycling. Herein, B-doped micron-sized single-crystal Co-free LMLOs were obtained by molten-salt (LiNO3 and H3BO3)-assisted sintering. The results reveal that the low-melting-point molten salt can serve as liquid-phase media to improve the efficiency of atomic mass transfer and crystal nucleation and growth. The modified single-crystal LMLO cathodes can resist the accumulation of anisotropic stress and strain during the cycling and reduce interface side reactions, thus achieving excellent high-voltage stability and kinetics performance. The reversible specific capacity of the single crystals is 210.8 mAh g-1 at 1C with a voltage decay rate of 1.95 mV/cycle and up to 161.1 mAh g-1 at 10C with a capacity retention of 81.06% after 200 cycles.

Nanoflower-like NiCo2O4 Composite Graphene Oxide as a Bifunctional Catalyst for Zinc-Air Battery Cathode.

Developing efficient bifunctional catalysts for nonprecious metal-based oxygen reduction (ORR) and oxygen evolution (OER) is crucial to enhance the practical application of zinc-air batteries. The study harnessed electrostatic forces to anchor the nanoflower-like NiCo2O4 onto graphene oxide, mitigating the poor inherent conductivity in NiCo2O4 as a transition metal oxide and preventing excessive agglomeration of the nanoflower-like structures during catalysis. Consequently, the resulting composite, NiCo2O4-GO/C, exhibited notably superior ORR and OER catalytic performance compared to pure nanoflower-like NiCo2O4. Notably, it excelled in OER catalytic activity of the OER relative to the precious metal RuO2. As a bifunctional catalyst for ORR and OER, NiCo2O4-GO/C displayed a potential difference of 0.88 V between the ORR half-wave potential and the OER potential at 10 mA·cm-2, significantly lower than the 1.08 V observed for pure flower-like NiCo2O4 and comparable to the 0.88 V exhibited by precious metal catalysts Pt/C + RuO2. The NiCo2O4-GO/C-based zinc-air battery demonstrated a discharge capacity of 817.3 mA h·g-1, surpassing that of precious metal-based zinc-air batteries. Moreover, charge-discharge cycling tests indicated the superior stability of the NiCo2O4-GO/C-based zinc-air battery compared to its precious metal-based counterparts.

Diagnostic procedure for localized constrictive pericarditis leading to bilateral pleural effusion: two case reports.

Constrictive pericarditis is a rare disease. Localized constrictive pericarditis leading to bilateral pleural effusion is more difficult to recognize, and the diagnostic procedure can be ambiguous. Here, we report two patients diagnosed with localized constrictive pericarditis who presented with bilateral pleural effusion. A thorough work-up showed that the pleural effusion was nonspecific, as was the pathology of the pleura. One patient had a history of pericardial effusion 2 years ago, and the other had undergone surgery for an anterior mediastinum teratoma. Pericardial scarring was found on their chest CT scans. The patients underwent pericardiectomy, and localized pericardial thickening was excised. The bilateral pleural effusion was effectively cured, and the patients showed satisfactory recovery on follow-up. Physicians should be aware of localized pericarditis leading to bilateral pleural effusion, and pericardiectomy is an effective diagnostic and therapeutic procedure.

Orderly Arranged Dipoles Regulate Anion-Derived Solid-Electrolyte Interphase for Stable Lithium Metal Chemistry.

Lithium (Li) metal batteries are considered the most promising high-energy-density electrochemical energy storage devices of the next generation. However, the unstable solid-electrolyte interphase (SEI) derived from electrolytes usually leads to high impedance, Li dendrites growth, and poor cyclability. Herein, the ferroelectric BaTiO3 with orderly arranged dipoles (BTOV) is integrated into the polypropylene separator as a functional layer. Detailed characterizations and theoretical calculations indicate that surface oxygen vacancies drive the phase transition of BaTiO3 materials and promote the ordered arrangement of dipoles. The strong dipole moments in BTOV can adsorb TFSI- and NO3 - anions selectively and promote their preferential reduction to form a SEI film enriched with inorganic LiF and LiNxOy species, thus facilitating the rapid transfer of Li+ and restraining the growth of Li dendrites. As a result, the Li-Li cell with the BTOV functional layer exhibits enhanced Li plating/stripping cycling with an ultra-long life of over 7000 h at 0.5 mA cm-2/1.0 mAh cm-2. The LiFePO4 || Li (50 µm) full cells display excellent cycling performance exceeding 1760 cycles and superior rate performance. This work provides a new perspective for regulating SEI chemistry by introducing ordered dipoles to control the distribution and reaction of anions.

Hydrogen Bond Boosted Ferroelectric Polarization Enables High Rate Capability Lithium Metal Batteries.

Lithium metal is considered as a promising anode material for next generation lithium-based batteries due to its highest specific capacity and lowest reduction potential. However, irreversible lithium stripping/depositing gives rise to severe dendritic growth and countless dead lithium, which lead to rapid electrochemical performance degradation and increased safety hazards, and thus limit its large-scale application. Herein, this work demonstrates a universal hydrogen-bond-induced strategy to in situ form a highly polarized ferroelectric polyvinylidene fluoride (PVDF) coating on the anode current collector. The localized electric field induced by the polarized ferroelectric PVDF can accelerate the migration of lithium ions and alleviate the shortage of lithium ions and uneven ion/electron distribution and transfer at the anode/electrolyte interface, thus promoting uniform deposition and stripping of Li+ at high-rate situations. As a result, the symmetrical Li || Li batteries with polarized PVDF coating exhibit a long cycling lifespan over 900 h under 2 mA cm-2 with marginal voltage polarization, and an ultra-high-rate performance up to 8.85 mA cm-2 . The full cells using LiFePO4 cathode also display enhanced electrochemical performance. The innovative strategy of ferroelectric polarization sheds light on interface engineering to circumvent Li dendrite growth in lithium metal batteries (LMBs).

Crosslinked solubilizer enables nitrate-enriched carbonate polymer electrolytes for stable, high-voltage lithium metal batteries.

High-voltage lithium metal batteries (LMBs) have been considered promising next-generation high-energy-density batteries. However, commercial carbonate electrolytes can scarcely be employed in LMBs owing to their poor compatibility with metallic lithium. N,N-dimethylacrylamide (DMAA)-a crosslinkable solubilizer with a high Gutmann donor number-is employed to facilitate the dissolution of insoluble lithium nitrate (LiNO3) in carbonate-based electrolytes and to form gel polymer electrolytes (GPEs) through in situ polymerization. The Li+ solvation structure of the GPEs is regulated using LiNO3 and DMAA, which suppresses the decomposition of LiPF6 and facilitates the formation of an inorganic-rich solid electrolyte interface. Consequently, the Coulombic efficiency (CE) of the Li||Cu cell assembled with a GPE increases to 98.5% at room temperature, and the high-voltage Li||NCM622 cell achieves a capacity retention of 80.1% with a high CE of 99.5% after 400 cycles. The bifunctional polymer electrolytes are anticipated to pave the way for next-generation high-voltage LMBs.

In Situ Formed Tribofilms as Efficient Organic/Inorganic Hybrid Interlayers for Stabilizing Lithium Metal Anodes.

The practical application of Li metal anodes (LMAs) is limited by uncontrolled dendrite growth and side reactions. Herein, we propose a new friction-induced strategy to produce high-performance thin Li anode (Li@CFO). By virtue of the in situ friction reaction between fluoropolymer grease and Li strips during rolling, a robust organic/inorganic hybrid interlayer (lithiophilic LiF/LiC6 framework hybridized -CF2-O-CF2- chains) was formed atop Li metal. The derived interface contributes to reversible Li plating/stripping behaviors by mitigating side reactions and decreasing the solvation degree at the interface. The Li@CFO||Li@CFO symmetrical cell exhibits a remarkable lifespan for 5,600 h (1.0 mA cm-2 and 1.0 mAh cm-2) and 1,350 cycles even at a harsh condition (18.0 mA cm-2 and 3.0 mAh cm-2). When paired with high-loading LiFePO4 cathodes, the full cell lasts over 450 cycles at 1C with a high-capacity retention of 99.9%. This work provides a new friction-induced strategy for producing high-performance thin LMAs.

Stabilizing Lithium Metal Batteries by Synergistic Effect of High Ionic Transfer Separator and Lithium-Boron Composite Material Anode.

The development of lithium (Li) metal batteries (LMBs) has been limited by problems, such as severe dendrite growth, drastic interfacial reactions, and large volume change. Herein, an LMB (8AP@LiB) combining agraphene oxide-poly(ethylene oxide) (PEO) functionalized polypropylene separator (8AP) with a lithium-boron (LiB) anode is designed to overcome these problems. Raman results demonstrate that the PEO chain on 8AP can influence the Li+ solvation structure in the electrolyte, resulting in Li+ homogeneous diffusion and Li+ deposition barrier reduction. 8AP exhibits good ionic conductivity (4.9 × 10-4 S cm-1), a high Li+ migration number (0.88), and a significant electrolyte uptake (293%). The 3D LiB skeleton can significantly reduce the anode volume changes and local current density during the charging/discharging process. Therefore, 8AP@LiB effectively regulates the Li+ flux and promotes the uniform Li deposition without dendrites. The Li||Li symmetrical cells of 8AP@LiB exhibit a high electrochemical stability of up to 1000 h at 1 mA cm-2 and 5 mAh cm-2. Importantly, the Li||LiFePO4 full cells of 8AP@LiB achieve an impressive 2000 cycles at 2C, while maintaining a high-capacity retention of 86%. The synergistic effect of the functionalized separator and LiB anode might provide a direction for the development of high-performance LMBs.

Interfacial friction enabling ≤ 20 µm thin free-standing lithium strips for lithium metal batteries.

A practical high-specific-energy Li metal battery requires thin (≤20 µm) and free-standing Li metal anodes, but the low melting point and strong diffusion creep of lithium metal impede their scalable processing towards thin-thickness and free-standing architecture. In this paper, thin (5 to 50 µm) and free-standing lithium strips were achieved by mechanical rolling, which is determined by the in situ tribochemical reaction between lithium and zinc dialkyldithiophosphate (ZDDP). A friction-induced organic/inorganic hybrid interface (~450 nm) was formed on Li with an ultra-high hardness (0.84 GPa) and Young's modulus (25.90 GPa), which not only enables the scalable process mechanics of thin lithium strips but also facilitates dendrite-free lithium metal anodes by inhibiting dendrite growth. The rolled lithium anode exhibits a prolonged cycle lifespan and high-rate cycle stability (in excess of more than 1700 cycles even at 18.0 mA cm-2 and 1.5 mA cm-2 at 25 °C). Meanwhile, the LiFePO4 (with single-sided load 10 mg/cm2) ||Li@ZDDP full cell can last over 350 cycles with a high-capacity retention of 82% after the formation cycles at 5 C (1 C = 170 mA/g) and 25 °C. This work provides a scalable approach concerning tribology design for producing practical thin free-standing lithium metal anodes.

In Situ Formed Heterostructure Interface and Well-Tuned Electronic Structure Ensuring Long Cycle Stability for 4.9 V High-Voltage Li-Rich Layered Oxide Cathodes.

High-voltage lithium-rich manganese-based layered oxides (LMLOs) are considered as the most competitive cathode materials for next-generation high-energy-density lithium-ion batteries (LIBs). However, LMLOs still suffer from irreversible lattice oxygen release, uncontrollable interface side reactions, and surface structural degradation. Herein, we propose an integration strategy combining La/Al codoping and LixCoPO4 nanocoating to improve the electrochemical performance of LMLOs comprehensively. La/Al codoping regulates the electronic structure to enhance the redox activity of anions and cations and inhibit structural degradation. The LixCoPO4 nanocoating formed by in situ reaction with the surface residual lithium can not only promote Li-ion migration but also reduce interfacial side reactions. The induced Layered@Rocksalt@LixCoPO4 heterostructure suppresses lattice volume variation and structural degradation during cycling. Under the synergistic effect of the heterostructure interface and well-tuned electronic structure, the capacity retention rate of comodified LMLO materials reaches 80.06% after 500 cycles (2.0-4.65 V) and 75.1% after 340 cycles at 1C under a high cut-off voltage of 4.9 V.

Reactive Polymer as Artificial Solid Electrolyte Interface for Stable Lithium Metal Batteries.

Lithium (Li) metal anodes have the highest theoretical capacity and lowest electrochemical potential making them ideal for Li metal batteries (LMBs). However, Li dendrite formation on the anode impedes the proper discharge capacity and practical cycle life of LMBs, particularly in carbonate electrolytes. Herein, we developed a reactive alternative polymer named P(St-MaI) containing carboxylic acid and cyclic ether moieties which would in situ form artificial polymeric solid electrolyte interface (SEI) with Li. This SEI can accommodate volume changes and maintain good interfacial contact. The presence of carboxylic acid and cyclic ether pendant groups greatly contribute to the induction of uniform Li ion deposition. In addition, the presence of benzyl rings makes the polymer have a certain mechanical strength and plays a key role in inhibiting the growth of Li dendrites. As a result, the symmetric Li||Li cell with P(St-MaI)@Li layer can stably cycle for over 900 h under 1 mA cm-2 without polarization voltage increasing, while their Li||LiFePO4 full batteries maintain high capacity retention of 96 % after 930 cycles at 1C in carbonate electrolytes. The innovative strategy of artificial SEI is broadly applicable in designing new materials to inhibit Li dendrite growth on Li metal anodes.

Organoboron- and Cyano-Grafted Solid Polymer Electrolytes Boost the Cyclability and Safety of High-Voltage Lithium Metal Batteries.

Solid-state polymer electrolytes (SPEs) are deemed as a class of sought-after candidates for high-safety and high-energy-density solid-state lithium metal batteries, but their low ionic conductivity, narrow electrochemical windows, and severe interfacial deterioration limit their practical implementations. Herein, an organoboron- and cyano-grafted polymer electrolyte (PVNB) was designed using vinylene carbonate as the polymer backbone and organoboron-modified poly(ethylene glycol) methacrylate and acrylonitrile as the grafted phases, which may facilitate Li-ion transport, immobilize the anions, and enlarge the oxidation voltage window; therefore, the well-tailored PVNB exhibits a high Li-ion transference number (tLi+ = 0.86), a wide electrochemical window (>5 V), and a high ionic conductivity (σ = 9.24 × 10-4 S cm-1) at room temperature (RT). As a result, the electrochemical cyclability and safety of the Li|LiFePO4 and Li|LiNi0.8Co0.1Mn0.1O2 cells with in situ polymerization of PVNB are substantially improved by forming the stable organic-inorganic composite cathode electrolyte interphase (CEI) and the Li3N-LiF-rich solid electrolyte interphase (SEI).

Evaluation of Chrysanthemi Indici Flos germplasms based on nine bioactive constituents and color parameters.

Chrysanthemi Indici Flos (CIF) is the inflorescence of Chrysanthemum indicum L., which exists in various shades of yellow and has pharmacologically active constituents. It is widely used for medicinal purposes in China, Japan, and South Korea to treat inflammatory diseases. Its external color is usually used to judge its internal quality in trade; however, the correlation between its color and chemical constituents is unknown. Here, we simultaneously determined five phenylpropanoids (neochlorogenic acid, chlorogenic acid, and isochlorogenic acids A, B, and C) and four flavonoids (linarin, luteolin, apigenin, and acacetin) of 70 CIF germplasms using a newly established UPLC method; furthermore, we measured their color parameters (L*, a*, and b*) using a spectrophotometer. Our results showed considerable variations in the bioactive constituent contents and color parameters of CIF. The content of the five phenylpropanoids and the relative correlation degree γi of the nine constituents were positively correlated with color parameters, which could be rapidly predicted based on L* and/or b*. Moreover, we screened out a high-quality germplasm with a high linarin content and bright colors using the hierarchical clustering method. Our results provide comprehensive insight into CIF's quality evaluation process, particularly the methods for procuring high-quality medicinal materials and breeding by color.

A separator modified by barium titanate with macroscopic polarization electric field for high-performance lithium-sulfur batteries.

The detrimental "shuttling effect" of lithium polysulfides and the sluggish kinetics of the sulfur redox reaction in lithium-sulfur batteries (LSBs) impede the practical application. Considering the high polar chemistry facilitates the anchoring of polysulfides, ferroelectric materials have gradually been employed as functionalized separators to suppress the "shuttling effect". Herein, a functional separator coated with BaTiO3 with a macroscopic polarization electric field (poled-BaTiO3) is designed for retarding the problematic shuttle effect and accelerating redox kinetics. Theoretical calculations and experiments revealed that resultant positive charged alignments on the poled-BaTiO3 coating can chemically immobilize polysulfides, effectively improving the cyclic stability of LSBs. Moreover, the simultaneous reinforcement of the built-in electric field in the poled-BaTiO3 coating can also improve Li-ion transportation for accelerating redox kinetics. Benefiting from these attributes, the as-developed LSB attains an initial discharge capacity of 1042.6 mA h g-1 and high cyclic stability of over 400 cycles at 1 C rate. The corresponding LSB pouch cell was also assembled to validate the concept. This work is anticipated to provide new insight into the development of high-performing LSBs through engineering ferroelectric-enhanced coatings.

Theranostic applications of selenium nanomedicines against lung cancer.

The incidence and mortality rates of lung cancer are among the highest in the world. Traditional treatment methods include surgery, chemotherapy, and radiotherapy. Although rapid progress has been achieved in the past decade, treatment limitations remain. It is therefore imperative to identify safer and more effective therapeutic methods, and research is currently being conducted to identify more efficient and less harmful drugs. In recent years, the discovery of antitumor drugs based on the essential trace element selenium (Se) has provided good prospects for lung cancer treatments. In particular, compared to inorganic Se (Inorg-Se) and organic Se (Org-Se), Se nanomedicine (Se nanoparticles; SeNPs) shows much higher bioavailability and antioxidant activity and lower toxicity. SeNPs can also be used as a drug delivery carrier to better regulate protein and DNA biosynthesis and protein kinase C activity, thus playing a role in inhibiting cancer cell proliferation. SeNPs can also effectively activate antigen-presenting cells to stimulate cell immunity, exert regulatory effects on innate and regulatory immunity, and enhance lung cancer immunotherapy. This review summarizes the application of Se-based species and materials in lung cancer diagnosis, including fluorescence, MR, CT, photoacoustic imaging and other diagnostic methods, as well as treatments, including direct killing, radiosensitization, chemotherapeutic sensitization, photothermodynamics, and enhanced immunotherapy. In addition, the application prospects and challenges of Se-based drugs in lung cancer are examined, as well as their forecasted future clinical applications and sustainable development.

Dual Active Sites of Oversaturated Fe-N5 and Fe2 O3 Nanoparticles for Accelerating Redox Kinetics of Polysulfides.

The shuttling effect and sluggish reaction kinetics are the main bottlenecks for the commercial viability of lithium-sulfur (Li-S) batteries. Metal-nitrogen-carbon single atom catalysts have attracted much attention to overcoming these obstacles due to their novel electrocatalytic activity. Herein, a novel cooperative catalytic interface with dual active sites (oversaturated Fe-N5 and polar Fe2 O3 nanocrystals) are co-embedded in nitrogen-doped hollow carbon spheres (Fe2 O3 /Fe-SA@NC) is designed by fine atomic regulation mechanism. Both experimental verifications and theoretical calculations disclose that the dual active sites (Fe-N5 and Fe2 O3 ) in this catalyst (Fe2 O3 /Fe-SA@NC) tend to form "FeS" and "LiN/O" bond, synchronically enhancing chemical adsorption and interface conversion ability of polysulfides, respectively. Specially, the Fe-N5 coordination with 3D configuration and sulfiphilic superfine Fe2 O3 nanocrystals exhibit the strong adsorption ability to facilitate the subsequent conversion reaction at dual-sites. Meanwhile, the nitrogen-doped hollow carbon spheres can promote Li+ /electron transfer and physically suppress polysulfides shuttling. Consequently, Li-S battery with the Fe2 O3 /Fe-SA@NC-modified separator exhibits a high capacity retention of 78% after 800 cycles at 1 C (pure S cathode, S content: 70 wt.%). Furthermore, the pouch cell with this separator shows good performance at 0.1 C for practical application (S loading: 4 mg cm-2 ).

Integrating a Ferroelectric Interface with a Well-Tuned Electronic Structure in Lithium-Rich Layered Oxide Cathodes for Enhanced Lithium Storage.

Li-rich layered oxides (LLOs) are considered promising candidates for new high-energy-density cathode materials for next-generation power batteries. However, their large-scale applications are largely hindered by irreversible Li/O loss, structural degradation, and interfacial side reactions during cycling. Herein, we demonstrate an integration strategy that tunes the electronic structure by La/Al codoping and constructs a ferroelectric interface on the LLOs surface through Bi0.5Na0.5TiO3 (BNT) coating. Experimental characterization reveals that the synergistic effect of the ferroelectric interface and the well-tuned electronic structure can not only promote the diffusion of Li+ and hinder the migration of On- but also suppress the lattice volume changes and reduce interfacial side reactions at high voltages up to 4.9 V vs Li+/Li. As a result, the modified material shows enhanced initial capacities and retention rates of 224.4 mAh g-1 and 78.57% after 500 cycles at 2.0-4.65 V and 231.7 mAh g-1 and 85.76% after 200 cycles at 2.0-4.9 V at 1C, respectively.

[Germplasm resource evaluation of Chrysanthemi Indici Flos based on color and chemical components].

This study explored the correlation between color and chemical components of Chrysanthemi Indici Flos(CIF), aiming at providing a reference for its procurement, evaluation, and breeding. Colorimeter and ultra-performance liquid chromatograph(UPLC) were used to determine the color(lightness-shade chromaticity value L~*, red-green chromaticity value a~*, yellow-blue chromati-city value b~*) and chemical components(cynaroside, linarin, luteolin, apigenin, and chlorogenic acid) of 84 CIF germplasms, respectively. Diversity analysis, correlation analysis, regression analysis, and cluster analysis were performed. The results showed that the color and chemical components of CIF were diversified. Chlorogenic acid was in significantly positive correlation with L~* and b~* and significantly negative correlation with a~*. Cynaroside and grey relational grade γ_i of chemical components were in significantly po-sitive correlation with b~* and L~*, respectively, whereas linarin, luteolin, and apigenin had no significant correlation with L~*, a~*, or b~*. The 84 CIF germplasms were clustered into 4 clades. In addition, germplasms in clade Ⅲ had higher γ_i and total color value(E~*_(ab)) than those in other clades, with the best quality and color, and a germplasm with the highest quality, bright yellow color, and highest content of linarin was screened out in this clade. Thus, CIF with bright yellow color had high content of cymaroside and chlorogenic acid and thereby high quality. In summary, the color can be used to quickly predict the quality of CIF. Our results provided data for the evaluation of CIF quality by color and a reference for its procurement and breeding.

Cationic-potential tuned biphasic layered cathodes for stable desodiation/sodiation.

Sodium layered oxides generally suffer from deep-desodiation instability in P2 structure and sluggish kinetics in O3 structure. It will be great to design P2/O3 biphasic materials that bring the complementary merits of both structures. However, such exploration is hindered by the ambiguous mechanism of material formation. Herein, supported by theoretical simulations and various spectroscopies, we prove that P2/O3 biphasic structures essentially originate from the internal heterogeneity of cationic potential, which can be realized by constraining the temperature-driven ion diffusion during solid-state reactions. Consequently, P2/O3 biphasic Na0.7Ni0.2Cu0.1Fe0.2Mn0.5O2-δ with well-designed quaternary composition is successfully obtained, exhibiting much-improved rate capabilities (62 mAh g-1 at 2.4 A g-1) and cycling stabilities (84% capacity retention after 500 cycles) than its single-phase analogues. Furthermore, synchrotron-based diffraction and X-ray absorption spectroscopy are employed to unravel the underlying sodium-storage mechanism of the P2/O3 biphasic structure. This work presents new insights toward the rational design of advanced layered cathodes for sodium-ion batteries.