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In recent years, sodium-ion batteries (SIBs) have attracted a lot of attention and are considered an ideal alternative to lithium-ion batteries (LIBs). The hard carbon (HC) anode in SIBs presents a unique challenge for studying the formation process of the solid electrolyte interphase (SEI) during initial cycling, owing to its distinctive porous structure. This study employs a combination of ultrasonic scanning techniques and differential electrochemical mass spectrometry to conduct an in-depth analysis of the two-dimensional distribution and composition of gases during the formation process. The findings reveal distinct gas evolution behaviors in SIBs compared to LIBs during formation. Notably, significant gas evolution is observed during the discharge phase of the formation cycle in SIBs, with higher discharge rates leading to increased gas evolution rates. This phenomenon is likely attributed to the adsorption of CO 2 gas by the abundant pores in HC, followed by desorption during discharge. Furthermore, the study demonstrates that the addition of 5A molecular sieves, which competitively adsorb gases, effectively reduces gas adsorption on the anode during formation, thereby significantly enhancing battery performance. This research elucidates the gas adsorption and desorption behavior at the battery interface, providing new insights into the SEI formation process in SIBs., (© 2024 Wiley-VCH GmbH.)

This study aimed to develop and validate a prognostic model for elderly patients with differentiated thyroid carcinoma (DTC) based on various demographic and clinical parameters in order to accurately predict patient outcomes. Patients who were diagnosed with DTC and were over 55 years old between 2010 and 2019 were identified from the Surveillance, Epidemiology, and End Results database. The patients were then randomly divided into a training set and a validation set in a 7:3 ratio, and patients from our center were included as an external validation group. Univariate and multivariate Cox proportional hazards regression analyses were performed to identify independent prognostic factors, which were then utilized to develop nomograms for predicting the prognosis. The discriminative ability of the nomograms was evaluated using the concordance index, and the calibration was assessed using calibration plots. The clinical usefulness and benefits of the predictive models were determined through decision curve analysis. The findings of the stepwise Cox regression analysis revealed that several variables, including age, marital status, sex, multifocality, T stage, N stage, and M stage, were significantly associated with overall survival in elderly patients with DTC. Additionally, age, tumor size, multifocality, T stage, N stage, and M stage were identified as the primary determinants of cancer specific survival in elderly patients with DTC. Using these predictors, nomograms were constructed to estimate the probability of overall survival and cancer specific survival. The nomograms demonstrated a high level of predictive accuracy, as evidenced by the concordance index, and the calibration plots indicated that the predicted outcomes were consistent with the actual outcomes. Furthermore, the decision curve analysis demonstrated that the nomograms provided substantial clinical net benefit, indicating their utility in clinical practice., Competing Interests: The authors have no conflicts of interest to disclose., (Copyright © 2024 the Author(s). Published by Wolters Kluwer Health, Inc.)

Utilizing solid-state polymer electrolytes (SPEs) in high-voltage Li-metal batteries is a promising strategy for achieving high energy density and safety. However, the SPEs face the challenges such as undesirable mechanical strength, low ionic conductivity and incompatible high-voltage interface. Here, a novel crosslinked poly(ether-urethane)-based SPE with a molecular cross-linked structure is fabricated to create high-throughput Li + transport pathway. The amino-modified Zr-porphyrin-based metal-organic frameworks (ZrMOF) are introduced as multisite cross-linking nodes and polymer chain extenders. The abundant ether/ketonic-oxygen and Lewis acid sites in the SPE achieve high Li + conductivity (5.7 × 10 -4 S cm -1 at 30 °C) and Li + transference number (0.84). The interpenetrating cross-linked structure of SPE with robust mechanical strength results in a record cycle life of 8000 h in Li||Li symmetric cell. The high structural stability of ZrMOF and abundant electron-withdrawing urethane/ureido groups in the SPE with high oxidation potential (5.1 V) enables a discharge capacity of 182 mAh g -1 at 0.3 C over 500 cycles in a LiNi 0.8 Co 0.1 Mn 0.1 O 2 ||Li cell. Remarkably, a high energy density of 446 Wh kg -1 in a 1.5-Ah pouch cell is obtained with high loading cathode (≈4 mAh cm -2 ), demonstrating a great prospect of the current SPE for practical application in solid-state, high-voltage Li-metal batteries., (© 2024 Wiley‐VCH GmbH.)

Metallene is considered as an emerging family of electrocatalysts due to its atomically layered structure and unique surface stress. Here we propose a strategy to modulate the Bader charge transfer (BCT) between Pd surface and oxygenated intermediates via p-d electronic interaction by introducing single-atom p-block metal (M=In, Sn, Pb, Bi) into Pd metallene nanosheets towards efficient oxygen reduction reaction (ORR). X-ray absorption and photoelectron spectroscopy suggests that doping p-block metals could facilitate electron transfer to Pd sites and thus downshift the d-band center of Pd and weaken the adsorption energy of O intermediates. Among them, the developed Bi-Pd metallene shows extraordinarily high ORR mass activity of 11.34 A mg Pd -1 and 0.86 A mg Pd -1 at 0.9 V and 0.95 V in alkaline solution, respectively, representing the best Pd-based ORR electrocatalysts ever reported. In the cathode of a Zinc-air battery, Bi-Pd metallene could achieve an open-circuit voltage of 1.546 V and keep stable for 760 h at 10 mA cm -2 . Theoretical calculations suggest that the BCT between Pd surface and *OO intermediates greatly affects the bond length between them (d Pd-*OO ) and Bi doping could appropriately reduce the amount of BCT and stretch the d Pd-*OO, thus enhancing the ORR activity., (© 2024 Wiley-VCH GmbH.)

Lithium-ion battery (LIB) has gained significant recognition for the power cell market owing to its impressive energy density and appealing cost benefit. Among various cathodes, a high-voltage cobalt-poor lithium nickel manganese cobalt oxide cathode (Co-poor NCM cathode) has been considered as a promising strategy to enhance its energy density. Despite these advantages, high-voltage Co-poor NCM cathode-graphite full battery usually suffers from poor rate performance. However, fast charging has been a key indicator for widespread application of power batteries. Although many efforts have been made to improve the charging performance of fresh batteries, few works investigate the charging ability during calendar aging and cycling aging of high-voltage Co-poor NCM cathode-graphite full battery. In this work, we found that the charging ability becomes worse during calendar aging and cycling aging. Results showed that the increasing charge transfer resistance from the cathode is the major obstacle to achieving fast charging during the aging process. To address the problem, high-voltage Al 2 O 3 -coated Co-poor NCM cathode successfully prepared via a simple atomic layer deposition (ALD) method has been developed to reduce the decay of charging performance during calendar aging and cycling aging. Al 2 O 3 -coated NCM cathode can effectively reduce the growth rate of the resistance of cathode, which is benefiting from the conversion of Al 2 O 3 into LiAlO 2 with high ionic conductivity and the restriction formation of rock salt phase. Benefiting from the decreased charge transfer resistance of the NCM cathode, the mismatch of the lithium-ion reaction kinetics is well alleviated, thus effectively reducing the polarization under fast charging. As a result, Al 2 O 3 -coated NCM cathode-graphite full battery shows the slow deterioration of charging performance during the aging process. This work provides a promising strategy for constructing fast-charging batteries during calendar aging and cycling aging.

With the booming development of Li-ion batteries (LIBs), the recycling and reusing of spent graphite (SG) from LIBs is becoming increasingly crucial. Meanwhile, developing low-cost and efficient carbon hosts for lithium-sulfur (Li-S) batteries has gained widespread attention in the past decade. Nevertheless, the processing of carbon materials as sulfur hosts is often energy-consuming and complex. Herein, a simple and environmental-friendly strategy is proposed to reuse the SG to prepare graphene/sulfur composite cathode for Li-S batteries. Due to expanded layer spacing and defects of SG, sulfur molecules can strip it into a graphene-type host via ball milling. By optimizing the S/SG ratio and ball milling time, the as-prepared graphene/sulfur composite cathode with 70 wt.% sulfur content exhibits a high capacity of 1000 mAh g -1 . With a high sulfur loading of 4.68 mg cm -2 , the graphene/sulfur cathode can maintain 526 mAh g -1 after 400 cycles. This work provides a novel waste-to-wealth perspective for recycling spent graphite from LIBs to reuse in Li-S batteries., (© 2024 Wiley‐VCH GmbH.)

O3-type layered oxide cathode exhibits great application potential for practical sodium-ion batteries, due to its cost-effectiveness, abundant sodium and manganese resources, and high theoretical capacity. However, the irreversible phase transition, coupled with rapid capacity decay, which is primarily attributed to the Jahn-Teller effect of Mn 3+ , remains a significant bottleneck for commercial application. Additionally, the sluggish kinetics during the (de)sodiation process require urgent improvement. Herein, an electronic structure regulation strategy is proposed by low-valence Li/Cu co-substitution to address these issues. The roles of Li/Cu on the electronic structure, structural evolution, and electrochemical properties in the Na 0.96 Ni 0.22 Fe 0.2 Mn 0.5 Li 0.04 Cu 0.04 O 2 (NFMLC) cathode are comprehensively explored through systematic in situ/ex situ characterization techniques and theoretical calculations. The results reveal that this strategy effectively activates more Ni 2+/3+ and Fe 3+/4+ redox reactions above 2.5 V, while suppressing Mn 3+/4+ redox activity below 2.5 V, thereby achieving highly structural reversibility. Therefore, the NFMLC electrode displays excellent long-term cycling stability (81.5% capacity retention after 2000 cycles at 5 C), and significantly enhanced rate performance (from 45.5% to 80.4% under a ratio of 5 C to 0.5 C). This work provides a valuable perspective on the design of low-cost, long-life, and high-performance layered oxide cathodes for practical sodium-ion batteries., (© 2024 Wiley‐VCH GmbH.)

The utilization of thin zinc (Zn) anodes with a high depth of discharge is an effective strategy to increase the energy density of aqueous Zn metal batteries (ZMBs), but challenged by the poor reversibility of Zn electrode due to the serious Zn-consuming side reactions at the Zn||electrolyte interface. Here, we introduce 2-bromomethyl-1,3-dioxolane (BDOL) and methanol (MeOH) as electrolyte additive into aqueous ZnSO 4 electrolyte. In the as-formulated electrolyte, BDOL with a strong electron-withdrawing group (-CH 2 Br) tends to pair with the H 2 O-Zn-MeOH complex, leading to the formation of organobromine-partnered H 2 O-Zn-MeOH cluster ions. During the Zn electrodeposition process, the formed ZnO-dominated by-products induce the polymerization of BDOL monomers, which are previously adsorbed on the electrode. As a result, a uniform dual-layer SEI with ZnO-dominated outer layer and polyether-dominated inner layer is built on the surface of Zn electrode. With such an in situ formed dual-layer SEI, the Zn||Mg 0.9 Mn 3 O 7  ⋅ 2.7H 2 O pouch cell using a 10-um Zn anode (corresponding to a low negative to positive areal capacity ratio of 3.56) successfully operated for 300 cycles with a high capacity retention of 86 %, promising a high practical energy density of >120 Wh/kg (based on the total mass of Zn and Mg 0.9 Mn 3 O 7  ⋅ 2.7H 2 O)., (© 2024 Wiley-VCH GmbH.)

The sustainable development of lithium iron phosphate (LFP) batteries calls for efficient recycling technologies for spent LFP (SLFP). Even for the advanced direct material regeneration (DMR) method, multiple steps including separation, regeneration, and electrode refabrication processes are still needed. To circumvent these intricacies, new regeneration methods that allow direct electrode reuse (DER) by rejuvenating SLFP electrodes without damaging its structure are desired. Here, a 0.1 M lithium triethyl borohydride/tetrahydrofuran solution, which has the proper reductive capability to reduce Fe 3+ in SLFP to Fe 2+ without alloying with the aluminum current collector, is selected as the lithiation/regeneration reagent to restock the Li loss and regenerate SLFP electrodes. By soaking the SLFP electrodes in the lithiation solution, we successfully rejuvenated the crystal structure and electrochemical activity of SLFP electrodes with structural integrity within only 6 minutes at room temperature. When being directly reused, the regenerated LFP electrodes deliver a high specific capacity of 162.6 mAh g -1 even after being exposed to air for 3 months. The DER strategy presents significant economic and environmental benefits compared with the DMR method. This research provides a timely and innovative solution for recycling spent blade batteries using large-sized LFP electrodes, boosting the closed-loop development of LFP batteries., (© 2024 Wiley-VCH GmbH.)

The mass-transfer of oxygen in liquid phases (including in the bulk electrolyte and near the electrode surface) is a critical step to deliver oxygen to catalyst sites (especially immersed catalyst sites) and use the full capacity of oxygen reduction reaction (ORR). Despite the extensive efforts of optimizing the complex three-phase reaction interfaces to enhance the gaseous oxygen transfer, strong limitations remain due to oxygen's poor solubility and slow diffusion in electrolytes. Herein, a magnetic method for boosting the directional hydrodynamic pumping of oxygen toward immersed catalyst sites is demonstrated which allows the ORR to reach otherwise inaccessible catalytic regions where high currents normally would have depleted oxygen. For Pt foil electrodes without forced oxygen saturation in KOH electrolytes, the mass-transfer-limited current densities can be improved by 60% under an external magnetic field of 435 mT due to the synergistic effect between bulk- and surface-magnetohydrodynamic (MHD) flows induced by Lorentz forces. The residual magnetic fields are further used at the surface of magnetic materials (such as CoPt alloys and Pt/FeCo heterostructures) to enhance the surface-MHD effect, which helps to retain part of the ORR enhancement permanently without applying external magnetic fields., (© 2024 Wiley‐VCH GmbH.)

Chemical synthesis of unconventional topologically close-packed intermetallic nanocrystals (NCs) remains a considerable challenge due to the limitation of large volume asymmetry between the components. Here, a series of unconventional intermetallic Frank-Kasper C15 phase Ir 2 M (M = rare earth metals La, Ce, Gd, Tb, Tm) NCs is successfully prepared via a molten-salt assisted reduction method as efficient electrocatalysts for hydrogen evolution reaction (HER). Compared to the disordered counterpart (A1-Ir 2 Ce), C15-Ir 2 Ce features higher Ir-Ce coordination number that leads to an electron-rich environment for Ir sites. The C15-Ir 2 Ce catalyst exhibits excellent and pH-universal HER activity and requires only 9, 16, and 27 mV overpotentials to attain 10 mA cm -2 in acidic, alkaline, and neutral electrolytes, respectively, representing one of the best HER electrocatalysts ever reported. In a proton exchange membrane water electrolyzer, the C15-Ir 2 Ce cathode achieves an industrial-scale current density of 1 A cm -2 with a remarkably low cell voltage of 1.7 V at 80 °C and can operate stably for 1000 h with a sluggish voltage decay rate of 50 µV h -1 . Theoretical investigations reveal that the electron-rich Ir sites intensify the polarization of *H 2 O intermediate on C15-Ir 2 Ce, thus lowering the energy barrier of the water dissociation and facilitating the HER kinetics., (© 2024 Wiley‐VCH GmbH.)

'Anode-free' Li metal batteries offer the highest possible energy density but face low Li coulombic efficiency when operated in carbonate electrolytes. Here we report a performance improvement of anode-free Li metal batteries using p-block tin octoate additive in the carbonate electrolyte. We show that the preferential adsorption of the octoate moiety on the Cu substrate induces the construction of a carbonate-less protective layer, which inhibits the side reactions and contributes to the uniform Li plating. In the mean time, the reduction of Sn 2+ at the initial charging process builds a stable lithophilic layer of Cu 6 Sn 5 alloy and Sn, improving the affinity between the Li and the Cu substrate. Notably, anode-free Li metal pouch cells with tin octoate additive demonstrate good cycling stability with a high coulombic efficiency of ~99.1%. Furthermore, this in situ p-block layer plating strategy is also demonstrated with other types of p-block metal octoate, as well as a Na metal battery system, demonstrating the high level of universality., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Aqueous Zinc-sulfur (Zn-S) batteries are promising for the field of energy storage due to their low cost, high theoretical capacity, and safety. However, the large volume expansion and the inherently poor conductivity of sulfur would result in electrode cracking and sluggish reaction kinetics, limiting the practical application of Zn-S batteries. Herein, commercial zinc sulfide (ZnS) is employed instead of S as cathode and proposed a doping modification strategy to solve the above problems. The designed ZnS 0.93 Se 0.07 cathode shows good cycle stability and much-improved reaction kinetics, which is due to the smaller bandgap of ZnS 0.93 Se 0.07 (1.40 eV) compared to ZnS (1.86 eV). As a result, the obtained ZnS 0.93 Se 0.07 cathode exhibits a high specific capacity of 552 mAh g -1 (1672.6 mAh g -1 based on S) at 0.1 A g -1 and 330 mAh g -1 (1000 mAh g -1 based on S) at 2 A g -1 . Moreover, the ZnS 0.93 Se 0.07 cathode can provide a high areal capacity of 3.8 mAh cm -2 at a high mass loading of 10 mg cm -2 and limited electrolyte (4 µL mg -1 ). This work provides a simple and effective cathode modification strategy, which is conducive to promoting the practical application of Zn-S batteries., (© 2024 Wiley‐VCH GmbH.)

Structurally ordered L1 0 -PtM (M = Fe, Co, Ni and so on) intermetallic nanocrystals, benefiting from the chemically ordered structure and higher stability, are one of the best electrocatalysts used for fuel cells. However, their practical development is greatly plagued by the challenge that the high-temperature (>600 °C) annealing treatment necessary for realizing the ordered structure usually leads to severe particle sintering, morphology change and low ordering degree, which makes it very difficult for the gram-scale preparation of desirable PtM intermetallic nanocrystals with high Pt content for practical fuel cell applications. Here we report a new concept involving the low-melting-point-metal (M' = Sn, Ga, In)-induced bond strength weakening strategy to reduce E a and promote the ordering process of PtM (M = Ni, Co, Fe, Cu and Zn) alloy catalysts for a higher ordering degree. We demonstrate that the introduction of M' can reduce the ordering temperature to extremely low temperatures (≤450 °C) and thus enable the preparation of high-Pt-content (≥40 wt%) L1 0 -Pt-M-M' intermetallic nanocrystals as well as ten-gram-scale production. X-ray spectroscopy studies, in situ electron microscopy and theoretical calculations reveal the fundamental mechanism of the Sn-facilitated ordering process at low temperatures, which involves weakened bond strength and consequently reduced E a via Sn doping, the formation and fast diffusion of low-coordinated surface free atoms, and subsequent L1 0 nucleation. The developed L1 0 -Ga-PtNi/C catalysts display outstanding performance in H 2 -air fuel cells under both light- and heavy-duty vehicle conditions. Under the latter condition, the 40% L1 0 -Pt 50 Ni 35 Ga 15 /C catalyst delivers a high current density of 1.67 A cm -2 at 0.7 V and retains 80% of the current density after extended 90,000 cycles, which exceeds the United States Department of Energy performance metrics and represents among the best cathodic electrocatalysts for practical proton-exchange membrane fuel cells., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Hypothesis: Metal-organic frameworks (MOFs) are highly suitable precursors for supercapacitor electrode materials owing to their high porosity and stable backbone structures that offer several advantages for redox reactions and rapid ion transport., Experiments: In this study, a carbon-coated Ni 9 S 8 composite (Ni 9 S 8 @C-5) was prepared via sulfuration at 500 ℃ using a spherical Ni-MOF as the sacrificial template., Finding: The stable carbon skeleton derived from Ni-MOF and positive structure-activity relationship due to the multinuclear Ni 9 S 8 components resulted in a specific capacity of 278.06 mAh·g -1 at 1 A·g -1 . Additionally, the hybrid supercapacitor (HSC) constructed using Ni 9 S 8 @C-5 as the positive electrode and the laboratory-prepared coal pitch-based activated carbon (CTP-AC) as the negative electrode achieved an energy density of 69.32 Wh·kg -1 at a power density of 800.06 W·kg -1 , and capacity retention of 83.06 % after 5000 cycles of charging and discharging at 5 A·g -1 . The Ni-MOF sacrificial template method proposed in this study effectively addresses the challenges associated with structural collapse and agglomeration of Ni 9 S 8 during electrochemical reactions, thus improving its electrochemical performance. Hence, a simple preparation method is demonstrated, with broad application prospects in supercapacitor electrodes., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

O3-type layered oxide cathodes are promising for practical sodium-ion batteries (SIBs) owing to their high theoretical capacity, facile synthesis, and sufficient Na + storage. However, they face challenges such as rapid capacity loss and poor cycling stability, mainly attributed to irreversible phase transitions. To address these challenges, a novel cathode material, Li/Sn co-substituted O3-Na 0.95 Li 0.07 Sn 0.01 Ni 0.22 Fe 0.2 Mn 0.5 O 2 (LSNFM), has been designed by regulating the electronic structure, in which Li + activates more redox reactions of Ni 2+/3+ and Fe 3+/4+ above 2.5 V and suppresses the redox reactivity of Mn 3+/4+ below 2.5 V, while Sn 4+ can prevent the charge delocalization in the transition metal layer, contributing to structural stability. Due to this synergistic effect, the as-prepared LSNFM electrode with high structural reversibility displays a 27.2% capacity increase contributed by the high-voltage transition metal ion redox activity and exhibits excellent long-term cycling stability, an 84.0% capacity retention after 500 cycles at 1 C and an 84.7% capacity retention after 2000 cycles at 5 C. The fundamental mechanism is fully investigated using systematic in situ / ex situ characterization techniques and density functional theory computations. This work provides a paradigm for designing long-term cycle life cathode materials by synergistically regulating the electronic structure in practical SIBs.

Ni-rich LiNi x Co y Mn z O 2 (NCM xyz, x  +  y  +  z  = 1, x  ≥ 0.8) layered oxide materials are considered the main cathode materials for high-energy-density Li-ion batteries. However, the endless cracking of polycrystalline NCM materials caused by stress accelerates the loss of active materials and electrolyte decomposition, limiting the cycle life. Hence, understanding the chemo-mechanical evolution during (de)lithiation of NCM materials is crucial to performance improvement. In this work, an optical fiber with με resolution is designed to in operando detect the stress evolution of a polycrystalline LiNi 0.8 Co 0.1 Mn 0.1 O 2 (P-NCM811) cathode during cycling. By integrating the sensor inside the cathode, the stress variation of P-NCM811 is completely transferred to the optical fiber. We find that the anisotropy of primary particles leads to the appearance of structural stress, inducing the formation of microcracks in polycrystalline particles, which is the main reason for capacity decay. The isotropy of primary particles reduces the structural stress of polycrystalline particles, eliminating the generation of microcracks. Accordingly, the P-NCM811 with an ordered arrangement structure delivered high electrochemical performance with capacity retention of 82% over 500 cycles. This work provides a brand-new perspective with regard to understanding the operando chemo-mechanical evolution of NCM materials during battery operation, and guides the design of electrode materials for rechargeable batteries., (© The Author(s) 2024. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd.)

Extensively-used rechargeable lithium-ion batteries (LIBs) face challenges in achieving high safety and long cycle life. To address such challenges, ultrathin solid polymer electrolyte (SPE) is fabricated with reduced phonon scattering by depositing the composites of ionic-liquid (1-ethyl-3-methylimidazolium dicyamide, EMIM:DCA), polyurethane (PU) and lithium salt on the polyethylene separator. The robust and flexible separator matrix not only reduces the electrolyte thickness and improves the mobility of Li + , but more importantly provides a relatively regular thermal diffusion channel for SPE and reduces the external phonon scattering. Moreover, the introduction of EMIM:DCA successfully breaks the random intermolecular attraction of the PU polymer chain and significantly decreases phonon scattering to enhance the internal thermal conductivity of the polymer. Thus, the thermal conductivity of the as-obtained SPE increases by approximately six times, and the thermal runaway (TR) of the battery is effectively inhibited. This work demonstrates that optimizing thermal safety of the battery by phonon engineering sheds a new light on the design principle for high-safety Li-ion batteries., (© 2024 Wiley‐VCH GmbH.)

Li-rich layered oxide (LRLO) cathodes have been regarded as promising candidates for next-generation Li-ion batteries due to their exceptionally high energy density, which combines cationic and anionic redox activities. However, continuous voltage decay during cycling remains the primary obstacle for practical applications, which has yet to be fundamentally addressed. It is widely acknowledged that voltage decay originates from the irreversible migration of transition metal ions, which usually further exacerbates structural evolution and aggravates the irreversible oxygen redox reactions. Recently, constructing O2-type structure has been considered one of the most promising approaches for inhibiting voltage decay. In this review, the relationship between voltage decay and structural evolution is systematically elucidated. Strategies to suppress voltage decay are systematically summarized. Additionally, the design of O2-type structure and the corresponding mechanism of suppressing voltage decay are comprehensively discussed. Unfortunately, the reported O2-type LRLO cathodes still exhibit partially disordered structure with extended cycles. Herein, the factors that may cause the irreversible transition metal migrations in O2-type LRLO materials are also explored, while the perspectives and challenges for designing high-performance O2-type LRLO cathodes without voltage decay are proposed., (© 2024. The Author(s).)

Graphite-based lithium-ion batteries have succeeded greatly in the electric vehicle market. However, they suffer from performance deterioration, especially at fast charging and low temperatures. Traditional electrolytes based on carbonated esters have sluggish desolvation kinetics, recognized as the rate-determining step. Here, a weakly solvating ether electrolyte with tetrahydropyran (THP) as the solvent is designed to enable reversible and fast lithium-ion (Li + ) intercalation in the graphite anode. Unlike traditional ether-based electrolytes which easily cointercalate into the graphite layers, the THP-based electrolyte shows fast desolvation ability and can match well with the graphite anode. In addition, the weak interconnection between Li + and THP allows more anions to come into the solvating shell of Li + , inducing an inorganic-rich interface and thus suppressing the side reactions. As a result, the lithium iron phosphate/graphite pouch cell (3 Ah) with the THP electrolyte shows a capacity retention of 80.3% after 500 cycles at 2 C charging, much higher than that of the ester electrolyte system (7.6% after 200 cycles). At 4 C charging, the discharging capacity is increased from 2.29 Ah of esters to 2.96 Ah of THP. Furthermore, the cell can work normally over wide working temperatures (-20 to 60 °C). Our electrolyte design provides some understanding of lithium-ion batteries at fast charging and wide temperatures.

Superionic halides have attracted widespread attention as solid electrolytes due to their excellent ionic conductivity, soft texture, and stability toward high-voltage electrode materials. Among them, Li 3 InCl 6 has aroused interest since it can be easily synthesized in water or ethanol. However, investigations into the influence of solvents on both the crystal structure and properties remain unexplored. In this work, Li 3 InCl 6 is synthesized by three different solvents: water, ethanol, and water-ethanol mixture, and the difference in properties has been studied. The results show that the product obtained by the ethanol solvent demonstrates the largest unit cell parameters with more vacancies, which tend to crystallize on the (131) plane and provide the 3D isotropic network migration for lithium-ions. Thus, it exhibits the highest ionic conductivity (1.06 mS cm -1 ) at room temperature and the lowest binding energy (0.272 eV). The assembled all-solid-state lithium metal batteries (ASSLMBs) employing Li 3 InCl 6 electrolytes demonstrate a high initial discharge capacity of 153.9 mA h g -1 at 0.1 C (1 C = 170 mA h g -1 ) and the reversible capacity retention rate can reach 82.83% after 50 cycles. This work studies the difference in ionic conductivity between Li 3 InCl 6 electrolytes synthesized by different solvents, which can provide a reference for the future synthesis of halide electrolytes and enable their practical application in halide-based ASSLMBs with a high energy density.

Reactive metal-support interaction (RMSI) is an emerging way to regulate the catalytic performance for supported metal catalysts. However, the induction of RMSI by the thermal reduction is often accompanied by the encapsulation effect on metals, which limits the mechanism research and applications of RMSI. In this work, a gradient orbital coupling construction strategy was successfully developed to induce RMSI in Pt-carbide system without a reductant, leading to the formation of L1 2 -Pt x M-MC y (M = Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, and W) intermetallic electrocatalysts. Density functional theory (DFT) calculations suggest that the gradient coupling of the d (M)-2 p (C)-5 d (Pt) orbital would induce the electron transfer from M to C covalent bonds to Pt NPs, which facilitates the formation of C vacancy ( C v ) and the subsequent M migration (occurrence of RMSI). Moreover, the good correlation between the formation energy of C v and the onset temperature of RMSI in Pt-MC x systems proves the key role of nonmetallic atomic vacancy formation for inducing RMSI. The developed L1 2 -Pt 3 Ti-TiC catalyst exhibits excellent acidic methanol oxidation reaction activity, with mass activity of 2.36 A mg Pt -1 in half-cell and a peak power density of 187.9 mW mg Pt -1 in a direct methanol fuel cell, which is one of the best catalysts ever reported. DFT calculations reveal that L1 2 -Pt 3 Ti-TiC favorably weakens *CO absorption compared to Pt-TiC due to the change of the absorption site from Pt to Ti, which accounts for the enhanced MOR performance.

Silicon (Si) anode has attracted broad attention because of its high theoretical specific capacity and low working potential. However, the severe volumetric changes of Si particles during the lithiation process cause expansion and contraction of the electrodes, which induces a repeatedly repair of solid electrolyte interphase, resulting in an excessive consuming of electrolyte and rapid capacity decay. Clearly known the deformation and stress changing at µε resolution in the Si-based electrode during battery operation provides invaluable information for the battery research and development. Here, an in operando approach is developed to monitor the stress evolution of Si anode electrodes via optical fiber Bragg grating (FBG) sensors. By implanting FBG sensor at specific locations in the pouch cells with different Si anodes, the stress evolution of Si electrodes has been systematically investigated, and Δσ/areal capacity is proposed for stress assessment. The results indicate that the differences in stress evolution are nested in the morphological changes of Si particles and the evolution characteristics of electrode structures. The proposed technique provides a brand-new view for understanding the electrochemical mechanics of Si electrodes during battery operation., (© 2024 Wiley‐VCH GmbH.)

Aqueous zinc-ion batteries (AZIBs) have emerged as one of the most promising candidates for next-generation energy storage devices due to their outstanding safety, cost-effectiveness, and environmental friendliness. However, the practical application of zinc metal anodes (ZMAs) faces significant challenges, such as dendrite growth, hydrogen evolution reaction, corrosion, and passivation. Fortunately, the rapid rise of nanomaterials has inspired solutions for addressing these issues associated with ZMAs. Nanomaterials with unique structural features and multifunctionality can be employed to modify ZMAs, effectively enhancing their interfacial stability and cycling reversibility. Herein, an overview of the failure mechanisms of ZMAs is presented, and the latest research progress of nanomaterials in protecting ZMAs is comprehensively summarized, including electrode structures, interfacial layers, electrolytes, and separators. Finally, a brief summary and optimistic perspective are given on the development of nanomaterials for ZMAs. This review provides a valuable reference for the rational design of efficient ZMAs and the promotion of large-scale application of AZIBs.

Developing efficient and anti-corrosive oxygen reduction reaction (ORR) catalysts is of great importance for the applications of proton exchange membrane fuel cells (PEMFCs). Herein, we report a novel approach to prepare metal oxides supported intermetallic Pt alloy nanoparticles (NPs) via the reactive metal-support interaction (RMSI) as ORR catalysts, using Ni-doped cubic ZrO 2 (Ni/ZrO 2 ) supported L1 0 -PtNi NPs as a proof of concept. Benefiting from the Ni migration during RMSI, the oxygen vacancy concentrations in the support are increased, leading to an electron enrichment of Pt. The optimal L1 0 -PtNi-Ni/ZrO 2 -RMSI catalyst achieves remarkably low mass activity (MA) loss (17.8 %) after 400,000 accelerated durability test cycles in a half-cell and exceptional PEMFC performance (MA=0.76 A mg Pt -1 at 0.9 V, peak power density=1.52/0.92 W cm -2 in H 2 -O 2 /-air, and 18.4 % MA decay after 30,000 cycles), representing the best reported Pt-based ORR catalysts without carbon supports. Density functional theory (DFT) calculations reveal that L1 0 -PtNi-Ni/ZrO 2 -RMSI requires a lower energetic barrier for ORR than L1 0 -PtNi-Ni/ZrO 2 (direct loading), which is ascribed to a decreased Bader charge transfer between Pt and *OH, and the improved stability of L1 0 -PtNi-Ni/ZrO 2 -RMSI compared to L1 0 -PtNi-C can be contributed to the increased adhesion energy and Ni vacancy formation energy within the PtNi alloy., (© 2024 Wiley-VCH GmbH.)

As a potential catalyst for hydrogen evolution reaction (HER), tungsten nitride (W 2 N) has attracted extensive attention, due to its Pt-like characteristic. Nevertheless, insufficient active sites, slow electron transfer, and lack of scale-up nano-synthesis methods significantly limit its practical application. Constructing multi-component active centers and interface-rich heterojunctions to increase exposed active sites and modulate interface electrons is a very effective modification strategy. Therefore, a nano-heterostructure formed from tungsten nitride, tungsten phosphide and tungsten encapsulated in N, P co-doped carbon nanofiber (W 2 N/WP/W@NPC) was synthesized by a flexible and scalable electrospinning technology. Experimental results reveal that abundant heterojunctions are formed, electron transfer occurs between tungsten nitride and tungsten phosphide, and carbon nanofibers play a confinement role. The optimized W 2 N/WP/W@NPC-3 electrocatalyst demonstrates excellent HER catalytic activity and robust stability in both acidic and base media. Furthermore, the overall water splitting performance is tested using W 2 N/WP/W@NPC as the cathode through a two-electrode electrolyzer, which also exhibits impressive electrochemical performance., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024. Published by Elsevier Inc.)

Constructing large-area artificial solid electrolyte interphase (SEI) to suppress Li dendrites growth and electrolyte consumption is essential for high-energy-density Li metal batteries (LMBs). Herein, chemically exfoliated ultrathin MoS 2 nanosheets (EMoS 2 ) as an artificial SEI are scalable transfer-printed on Li-anode (EMoS 2 @Li). The EMoS 2 with a large amount of sulfur vacancies and 1T phase-rich acts as a lithiophilic interfacial ion-transport skin to reduce the Li nucleation overpotential and regulate Li + flux. With favorable Young's modulus and homogeneous continuous layered structure, the proposed EMoS 2 @Li effectively suppresses the growth of Li dendrites and repeat breaking/reforming of the SEI. As a result, the assembled EMoS 2 @Li||LiFePO 4 and EMoS 2 @Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 batteries demonstrate high-capacity retention of 93.5% and 92% after 1000 cycles and 300 cycles, respectively, at ultrahigh cathode loading of 20 mg cm -2 . Ultrasonic transmission technology confirms the admirable ability of EMoS 2 @Li to inhibit Li dendrites in practical pouch batteries. Remarkably, the Ah-class EMoS 2 @Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch battery exhibits an energy density of 403 Wh kg -1 over 100 cycles with the low negative/positive capacity ratio of 1.8 and electrolyte/capacity ratio of 2.1 g Ah -1 . The strategy of constructing an artificial SEI by sulfur vacancies-rich and 1T phase-rich ultrathin MoS 2 nanosheets provides new guidance to realize high-energy-density LMBs with long cycling stability., (© 2024 Wiley‐VCH GmbH.)

The solid-state battery with a lithium metal anode is a promising candidate for next-generation batteries with improved energy density and safety. However, the current polymer electrolytes still cannot fulfill the demands of solid-state batteries. In this work, we propose a "5H" poly(ethylene oxide) (PEO) electrolyte via introducing a multifunctional additive of tris(pentafluorophenyl)borane (TPFPB) for high-performance lithium metal batteries. The addition of TPFPB improves the ionic conductivity from 6.08 × 10 -5 to 1.54 × 10 -4 S cm -1 via reducing the crystallinity of the PEO electrolyte and enhances the lithium-ion transference number from 0.19 to 0.53 via anion trapping due to its Lewis acid nature. Furthermore, the fluorine and boron segments from TPFPB can optimize the composition of the solid-electrolyte interphase and cathode-electrolyte interphase, providing a high electrochemical stability window over 4.6 V of the PEO electrolyte along with significantly improved interface stability. At last, TPFPB can ensure improved safety through a self-extinguishing effect. As a result, the "5H" electrolyte enables the Li/Li symmetric cells to achieve a stable cycle over 2200 h at the current density of 0.2 mA cm -2 with a capacity of 0.2 mA h cm -2 ; the LiFePO 4 /Li full cells with a high LFP loading of 8 mg cm -2 exhibits decay-free capacity of 140 mA h g -1 (99% capacity retention) after 100 cycles; and the NCM811/Li cells exhibit a high capacity of 160 mA h g -1 after 50 cycles at 0.5 C. This work presents an innovative approach to utilizing a "5H" electrolyte for high-performance solid-state lithium batteries.

Solid electrolyte interface (SEI) is arguably the most important concern in graphite anodes, which determines their achievable Coulombic efficiency (CE) and cycling stability. In spent graphite anodes, there are already-formed (yet loose and/or broken) SEIs and some residual active lithium, which, if can be inherited in the regenerated electrodes, are highly desired to compensate for the lithium loss due to SEI formation. However, current graphite regenerated approaches easily destroy the thin SEIs and residue active lithium, making their reuse impossible. Herein, this work reports a fast-heating strategy (e.g., 1900 K for ≈150 ms) to upcycle degraded graphite via instantly converting the loose original SEI layer (≈100 nm thick) to a compact and mostly inorganic one (≈10-30 nm thick with a 26X higher Young's Modulus) and still retaining the activity of residual lithium. Thanks to the robust SEI and enclosed active lithium, the regenerated graphite exhibited 104.7% initial CE for half-cell and gifted the full cells with LiFePO 4 significantly improved initial CE (98.8% versus 83.2%) and energy density (309.4 versus 281.4 Wh kg -1 ), as compared with commercial graphite. The as-proposed upcycling strategy turns the "waste" graphite into high-value prelithiated ones, along with significant economic and environmental benefits., (© 2024 Wiley‐VCH GmbH.)

Sodium-ion batteries are competitive candidates for large-scale energy storage batteries due to the abundant sodium resource. However, the electrode interface in the conventional electrolyte is unstable, deteriorating the cycle life of the cells. Introducing functional electrolyte additives can generate stable electrode interfaces. Here, pentafluoro(phenoxy)cyclotriphosphazene (FPPN) serves as a functional electrolyte additive to stabilize the interfaces of the layered oxide cathode and the hard carbon anode. The fluorine substituting groups and the π-π conjugated ─PN─ structure decrease the lowest unoccupied molecular orbital and increase the highest occupied molecular orbital of FPPN, respectively, realizing the preferential reduction and oxidization of FPPN on the anode and cathode simultaneously, which results in the formation of a uniform, ultrathin, and inorganic-rich solid electrolyte interlayer and cathode electrolyte interphase. The sodium-ion pouch cells of 5 Ah capacity rather than coin cells are assembled to evaluate the effect of FPPN. It can retain a high capacity of 4.46 Ah after 1000 cycles, corresponding to a low decay ratio of 0.01% per cycle. The pouch cell also achieves a high energy density of 145 Wh kg -1 and a wide operating temperature of -20-60 °C. This work can attract more attention to the rational electrolyte design for practical applications., (© 2024 Wiley‐VCH GmbH.)

Using Li 2 S cathodes instead of S cathodes presents an opportunity to pair them with Li-free anodes (e.g., graphite), thereby circumventing anode-related issues, such as poor reversibility and safety, encountered in Li-S batteries. However, the moisture-sensitive nature of Li 2 S causes the release of hazardous H 2 S and the formation of insulative by-products, increasing the manufacturing difficulty and adversely affecting cathode performance. Here, Li 4 SnS 4 , a Li + conductor that is air-stable according to the hard-soft acid-base principle, is formed in situ and uniformly on Li 2 S particles because Li 2 S itself participates in Li 4 SnS 4 formation. When exposed to air (20% relative humidity), the protective Li 4 SnS 4 layer maintains its components and structure, thus contributing to the enhanced stability of the Li 2 S@Li 4 SnS 4 composite. In addition, the Li 4 SnS 4 layer can accelerate the sluggish conversion of Li 2 S because of its favorable interfacial charge transfer, and continuously confine lithium polysulfides owing to its integrity during electrochemical processes. A graphite-Li 2 S pouch cell containing a Li 2 S@Li 4 SnS 4 cathode is constructed, which shows stable cyclability with 97% capacity retention after 100 cycles. Hence, combining a desirable air-stable Li 2 S cathode and a highly reversible Li-free configuration offers potential practical applications of graphite-Li 2 S full cells., (© 2024 Wiley‐VCH GmbH.)

The cobalt-free layered oxide cathode of LiNi 0.65 Mn 0.35 O 2 is promising for high-energy-density lithium-ion batteries (LIBs). However, under high-voltage conditions, severe side reactions between the Co-free cathode and electrolyte, as well as grain boundary cracks and pulverization of particles, hinder its practical applications. Herein, an electrolyte regulation strategy is proposed by adding fluoroethylene carbonate (FEC) and LiPO 2 F 2 as electrolyte additives in carbonate-based electrolytes to address the above issues. As a result, a homogeneous and dense organic-inorganic hybrid cathode electrolyte interface (CEI) film is formed on the cathode surface. The CEI film consists of C-F, LiF, Li 2 CO 3 , and Li x PO y F z species, which is proven to be highly conductive and effective in suppressing structure damage and alleviating the interfacial reactions between the cathode and electrolyte. With such a CEI film, the interfacial stability of the Co-free cathode and the high-voltage cycling performance of Li||LiNi 0.65 Mn 0.35 O 2 are greatly improved. A reversible capacity of 155.1 mAh g -1 and a capacity retention of 81.3% over 150 cycles are attained at a 4.8 V charge cutoff voltage with the tamed electrolyte, whereas the cell without the additives only retains 76.1% capacity retention. Therefore, our work demonstrates the synergistic effect of FEC and LiPO 2 F 2 in stabilizing the interface of Co-free cathode materials and provides an alternative strategy for the electrolyte design of high-voltage LIBs.

Stable solid electrolytes are essential to high-safety and high-energy-density lithium batteries, especially for applications with high-voltage cathodes. In such conditions, solid electrolytes may experience severe oxidation, decomposition, and deactivation during charging at high voltages, leading to inadequate cycling performance and even cell failure. Here, we address the high-voltage limitation of halide solid electrolytes by introducing local lattice distortion to confine the distribution of Cl - , which effectively curbs kinetics of their oxidation. The confinement is realized by substituting In with multiple elements in Li 3 InCl 6 to give a high-entropy Li 2.75 Y 0.16 Er 0.16 Yb 0.16 In 0.25 Zr 0.25 Cl 6 . Meanwhile, the lattice distortion promotes longer Li-Cl bonds, facilitating favorable activation of Li + . Our results show that this high-entropy halide electrolyte boosts the cycle stability of all-solid-state battery by 250% improvement over 500 cycles. In particular, the cell provides a higher discharge capacity of 185 mAh g -1 by increasing the charge cut-off voltage to 4.6 V at a small current rate of 0.2 C, which is more challenging to electrolytes|cathode stability. These findings deepen our understanding of high-entropy materials, advancing their use in energy-related applications., (© 2024. The Author(s).)

As the classic cathode material, lithium cobalt oxide (LiCoO 2 , LCO) suffers from severe structural and interfacial degradation at voltage >4.5 V, which induces fast capacity decay of the cells. Herein, we adopt a simple and effective method, doping aluminum (Al) cations in precursors, to improve the structural stability of LCO and systematically investigate the effect of Al doping on the electrochemical performances. Doping in precursors rather than bulk particles is beneficial to realize uniform Al ions distribution. Even at 4.5 V charging voltage, the LCO/graphite pouch cells with high Al doping levels (8500 ppm) deliver initial and reversible discharge capacities of 386 and 369 mAh after 500 cycles, respectively. The capacity retention is as high as 95.5%. When the cutoff voltage reaches 4.55 V, the pouch cell maintains 79.0% of the first-cycle discharge capacity after 500 cycles. With optimized electrolyte, the pouch cell realizes 87.3% of the initial discharge capacity after 500 cycles at 45 °C. Moreover, the thermal safety performance of the pouch cells with Al doping is promising. Our work displays an excellent inspiration for developing high-voltage, long-cycle, and safe LCO cathode for commercial lithium-ion batteries.

Anode-free solid-state batteries (AFSSBs) are considered to be one of the most promising high-safety and high-energy storage systems. However, low Coulombic efficiency stemming from severe deterioration on solid electrolyte/current collector (Cu foil) interface and undesirable Li dendrite growth impede their practical application, especially when rigid garnet electrolyte is used. Here, an interfacial engineering strategy between garnet electrolyte and Cu foil is introduced for stable and highly efficient AFSSBs. By utilizing the high Li ion conductivity of LiC 6 layer, interfacial self-adaption ability arising from ductile lithiated polyacrylic acid polymer layer and regulated Li deposition via Li-Ag alloying reaction, the garnet-based AFSSB delivers a stable long-term operation. Additionally, when combined with a commercial LiCoO 2 cathode (3.1 mAh cm -2 ), the cell also exhibits an outstanding capacity retention due to the tailored interface design. The strategies for novel AFSSBs architecture thus offer an alternative route to design next-generation batteries with high safety and high density., (© 2023 Wiley-VCH GmbH.)

Surface polarization under harsh electrochemical environments usually puts catalysts in a thermodynamically unstable state, which strictly hampers the thermodynamic stability of Pt-based catalysts in high-performance fuel cells. Here, we report a strategy by introducing electron buffers (variable-valence metals, M = Ti, V, Cr, and Nb) into intermetallic Pt alloy nanoparticle catalysts to suppress the surface polarization of Pt shells using the structurally ordered L1 0 -M-PtFe as a proof of concept. Operando X-ray absorption spectra analysis suggests that with the potential increase, electron buffers, especially Cr, could facilitate an electron flow to form a electron-enriched Pt shell and thus weaken the surface polarization and tensile Pt strain. The best-performing L1 0 -Cr-PtFe/C catalyst delivers superb oxygen reduction reaction (ORR) activity (mass activity = 1.41/1.02 A mg Pt -1 at 0.9 V, rated power density = 14.0/9.2 W mg Pt -1 in H 2 -air under a total Pt loading of 0.075/0.125 mg Pt cm -2 , respectively) and stability (20 mV voltage loss at 0.8 A cm -2 after 60,000 cycles of accelerated durability test) in a fuel cell cathode, representing one of the best reported ORR catalysts. Density functional theory calculations reveal that the optimized surface strain by introducing Cr on L1 0 -PtFe/C accounts for the enhanced ORR activity, and the durability enhancement stems from the charge transfer contribution of Cr to the Pt shells and the increased kinetic energy barrier for Pt dissolution/Fe diffusion.

Fe/Mn-based layered oxide cathode is regarded as a competitive candidate for sodium-ion batteries (SIBs) because of its high theoretical capacity, earth abundance and low cost. However, its poor cycling stability still remains a major bottleneck. Herein, P2/O3 biphasic Na 0.67 Fe 0.425 Mn 0.425 Cu 0.15 O 2 layered oxide is successfully synthesized via a sol-gel method. It is observed that Cu substitution can facilitate the conversion of P2 to O3 phase, and the P2/O3 composite structure can be obtained with an appropriate amount of Cu. Meanwhile, in-situ XRD reveals that constructing P2/O3 composite structure can realize the highly reversible phase transition process of P2/O3-P2/P3-OP4/OP2 and decrease the lattice mismatch during Na + insertion/extraction. Consequently, the biphasic P2/O3-Na 0.67 Fe 0.425 Mn 0.425 Cu 0.15 O 2 electrode exhibits 87.1 % capacity retention after 100 cycles at 1C, while the single phase P2-Na 0.67 Fe 0.5 Mn 0.5 O 2 electrode has only 36.4 %. Therefore, the constructing biphasic structure is proved to be an effective strategy for designing high-performance Fe/Mn-based layered oxide cathodes., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)

Coupling high-capacity cathode and Li-anode with solid-state electrolyte has been demonstrated as an effective strategy for increasing the energy densities and safety of rechargeable batteries. However, the limited ion conductivity, the large interfacial resistance, and unconstrained Li-dendrite growth hinder the application of solid-state Li-metal batteries. Here, a poly(ether-urethane)-based solid-state polymer electrolyte with self-healing capability is designed to reduce the interfacial resistance and provides a high-performance solid-state Li-metal battery. With its dynamic covalent disulfide bonds and hydrogen bonds, the proposed solid-state polymer electrolyte exhibits excellent interfacial self-healing ability and maintains good interfacial contact. Full cells are assembled with the two integrated electrodes/electrolytes. As a result, the Li||Li symmetric cells exhibit stable long-term cycling for more than 6000 h, and the solid-state Li-S battery shows a prolonged cycling life of 700 cycles at 0.3 C. The use of ultrasound imaging technology shows that the interfacial contact of the integrated structure is much better than those of traditional laminated structure. This work provides an interesting interfacial dual-integrated strategy for designing high-performance solid-state Li-metal batteries., (© 2024. The Author(s).)

The optimal electrolyte for ultrahigh energy density (>400 Wh/kg) lithium-metal batteries with a LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode is required to withstand high voltage (≥4.7 V) and be adaptable over a wide temperature range. However, the battery performance is degraded by aggressive electrode-electrolyte reactions at high temperature and high voltage, while excessive growth of lithium dendrites usually occurs due to poor kinetics at low temperature. Accordingly, the development of electrolytes has encountered challenges in that there is almost no electrolyte simultaneously meeting the above requirements. Herein, a high chaos electrolyte design strategy is proposed, which promotes the formation of weak solvation structures involving multiple anions. By tailoring a Li + -EMC-DMC-DFOB - -PO 2 F 2 - -PF 6 - multiple-anion-rich solvation sheath, a robust inorganic-rich interphase is obtained for the electrode-electrolyte interphase (EEI), which is resistant to the intense interfacial reactions at high voltage (4.7 V) and high temperature (45 °C). In addition, the Li + solvation is weakened by the multiple-anion solvation structure, which is a benefit to Li + desolventization at low temperature (-30 °C), greatly improving the charge transfer kinetics and inhibiting the lithium dendrite growth. This work provides an innovative strategy to manipulate the high chaos electrolyte to further optimize solvation chemistry for high voltage and wide temperature applications.

To better understand why Chinese residents' COVID-19 perceptions of the importance of vaccination change dramatically over time, this research used an online lab-like experiment to test the antecedents of individuals' perception of the importance of COVID-19 vaccines. We find that participants who view themselves as separate from others (i.e. independent self-construal) perceive COVID-19 vaccines as more important than Hepatitis B vaccines (i.e. control group), regardless of how salient mortality is for them. In contrast, among participants who view themselves as a part of their social groups (i.e. interdependent self-construal), awareness of death (i.e. mortality salience) plays a moderating role. Specifically, when mortality is salient, COVID-19 vaccines are considered more important than Hepatitis B vaccines; when morality is not salient, vaccine type does not make a difference on perceptions of vaccine importance.

Recently, sodium-ion batteries (SIBs) have received considerable attention for large-scale energy storage applications. However, the low initial Coulombic efficiency of traditional SIBs severely impedes their further development. Here, a highly active Na 2 S-based composite is employed as a self-sacrificial additive for sodium compensation in SIBs. The in situ synthesized Na 2 S is wrapped in a carbon matrix with nanoscale particle size and good electrical conductivity, which helps it to achieve a significantly enhanced electrochemical activity as compare to commercial Na 2 S. As a highly efficient presodiation additive, the proposed Na 2 S/C composite can reach an initial charge capacity of 407 mAh g -1 . When 10 wt.% Na 2 S/C additive is dispersed in the Na 3 V 2 (PO 4 ) 3 cathode, and combined with a hard carbon anode, the full cell achieves 24.3% higher first discharge capacity, which corresponds to a 18.3% increase in the energy density from 117.2 to 138.6 Wh kg -1 . Meanwhile, it is found that the Na 2 S additive does not generate additional gas during the initial charging process, and under an appropriate content, its reaction product has no adverse impact on the cycling stability and rate performance of SIBs. Overall, this work establishes Na 2 S as a highly effective additive for the construction of advanced high-energy-density SIBs., (© 2023 Wiley-VCH GmbH.)

The rational design of novel high-performance cathode materials for sodium-ion batteries is a challenge for the development of the renewable energy sector. Here, a new sodium-deficient NASICON phosphate, namely Na 3.40 □ 0.60 Co 0.5 Fe 0.5 V(PO 4 ) 3 , demonstrating the excellent electrochemical performance is reported. The presence of Co allows a third Na + to participate in the reaction thus exhibiting a high reversible capacity of ≈155 mAh g -1 in the voltage range of 2.0-4.0 V versus Na + /Na with a reversible single-phase mechanism and a small volume shrinkage of ≈5.97% at 4.0 V. 23 Na solid-state nuclear magnetic resonance (NMR) combined with ex situ X-ray diffraction (XRD) refinements provide evidence for a preferential Na + insertion within the Na2 site. Furthermore, the enhanced sodium kinetics ascribed to Co-substitution is also confirmed in combination with electrochemical impedance spectroscopy (EIS), galvanostatic intermittent titration technique (GITT), and theoretical calculation., (© 2023 Wiley-VCH GmbH.)

Lithium (Li) metal electrodes show significantly different reversibility in the electrolytes with different salts. However, the understanding on how the salts impact on the Li loss remains unclear. Herein, using the electrolytes with different salts (e.g., lithium hexafluorophosphate (LiPF 6 ), lithium difluoro(oxalato)borate (LiDFOB), and lithium bis(fluorosulfonyl)amide (LiFSI)) as examples, we decouple the irreversible Li loss (SEI Li + and "dead" Li) during cycling. It is found that the accumulation of both SEI Li + and "dead" Li may be responsible to the irreversible Li loss for the Li metal in the electrolyte with LiPF 6 salt. While for the electrolytes with LiDFOB and LiFSI salts, the accumulation of "dead" Li predominates the Li loss. We also demonstrate that lithium nitrate and fluoroethylene carbonate additives could, respectively, function as the "dead" Li and SEI Li + inhibitors. Inspired by the above understandings, we propose a universal procedure for the electrolyte design of Li metal batteries (LMBs): (i) decouple and find the main reason for the irreversible Li loss; (ii) add the corresponding electrolyte additive. With such a Li-loss-targeted strategy, the Li reversibility was significantly enhanced in the electrolytes with 1,2-dimethoxyethane, triethyl phosphate, and tetrahydrofuran solvents. Our strategy may broaden the scope of electrolyte design toward practical LMBs., (© 2023. Shanghai Jiao Tong University.)

Aqueous zinc-ion batteries (AZIBs) are receiving widespread attention due to their abundant resources, low material cost, and high safety. However, the susceptibility of Zn metal anodes to corrosion and hydrogen evolution limits their further practical applications. Replacing Zn metal with intercalation-type anode material and constructing rocking-chair-type batteries could be an effective way to significantly prolong the cycle life of AZIBs. Herein, we present copper selenide with different crystal phase structures through a facile redox reaction as an anode for AZIBs. By comparing and analyzing different copper selenide phases, it is found that the cubic Cu 2- x Se shows superior structural stability and highly reversible Zn 2+ storage. Theoretical calculation results further demonstrate that the cubic Cu 2- x Se possesses an increased electrical conductivity, higher Zn 2+ adsorption energy, and reduced diffusion barrier, thereby promoting the storage reversibility and (de)intercalation kinetics of the Zn 2+ ion. Thus, the Cu 2- x Se anode delivers a long-term service life of over 15 000 cycles and impressive cumulative capacity. Furthermore, the full-cells assembled with the MnO 2 /CNT cathode operate stably for over 1500 cycles at 6 mA cm -2 at a negative/positive (N/P) capacity ratio of ∼1.53. This work provides a more ideal Zn-metal-free anode, which helps to push the practical applications of AZIBs.

NaClO 4 and NaPF 6 , the most universally adopted electrolyte salts in commercial sodium-ion batteries (SIBs), have a decisive influence on the interfacial chemistry, which is closely related to electrochemical performance. The complicated and ambiguous interior mechanism of microscopic interfacial chemistry has prevented reaching a consensus regarding the most suitable sodium salt for high-performance SIB electrolytes. Herein, we reveal that the solvation structure induced by different sodium salt anions determines the Na + desolvation kinetics and interfacial film evolution process. Specifically, the weak interaction between Na + and PF 6 - promoted sodium desolvation and storage kinetics. The solvation structure involving PF 6 - induced the anion's preferential decomposition, generating a thin, inorganic compound-rich cathode-electrolyte interphase that ensured interface stability and inhibited solvent decomposition, thereby guaranteeing electrode stability and promoting the charge transfer kinetics. This study provides clear evidence that NaPF 6 is not only more compatible with industrial processes but also more conducive to battery performance. Commercial electrolyte design employing NaPF 6 will undoubtedly promote the industrialization of SIBs.

An ultrasonic method for lithium-ion battery (LIB) state of charge (SoC) estimation is a promising emerging technology which may largely improve the SoC estimation accuracy. Previously, it was unknown whether the SoC change induced ultrasonic signal change originated from the anode or the cathode, because the thicknesses of cathodes, anodes and separators are much smaller than the ultrasonic wavelength, which makes it impossible to decouple the anodic and cathodic influence. To quantitatively solve the above problem, we have designed a special half-cell architecture with an extra-thick separator (675 μm) to study the reflected ultrasonic signal. The thickened separator would significantly delay the reflection of ultrasonic waves from the counter-electrode (Li), so that the influence of the working electrode (LiFePO 4 or graphite) on the ultrasonic wave can be studied separately. As a result, in the Gr anode, the time of flight (ToF) of the ultrasonic wave decreases with SoC, the changing rate coefficient of which is in the range of -110 to -70 ps μm Gr thickness -1 , depending on the compact density. A lower compact density electrode leads to a more significant ultrasonic ToF decrease and intensity increase while in the LFP cathode, the ToF increases with SoC, the changing rate coefficient of which is in the range of 15-43 ps μm LFP thickness -1 . The ToF change of the transmitted ultrasound through multilayered LIB matches very well with the sum of the ToF change in each electrode measured with our half-cells.

Unstable solid electrolyte interface (SEI) layers induced by significant volume changes and subsequent side reactions at the interface have prevented Si anodes from practical application in lithium-ion batteries. The interface stability plays an important role in the electrochemical performance of Si electrodes. Here, we modify the interface of a Si electrode with ion-conductive poly(ethylene glycol) diglycidyl ether (PEGDE), which controls the electrolyte decomposition route and stabilizes the SEI layer. It enables the Si electrode to achieve a capacity of more than 1800 mAh g -1 at a current density of 2 A g -1 , with a capacity retention of 77.25% after 300 cycles. The PEGDE-decorated Si electrode also shows greatly improved rate capability, with specific capacity up to 777 mAh g -1 even at 20 A g -1 . We demonstrate that PEGDE decoration greatly increases the Li 2 CO 3 ratio in the SEI layer, which improves the interface stability and Li + conductivity and hence suppresses continuous electrolyte decomposition. As a result, the structural integrity of the Si particles is maintained and capacity fading is retarded. This work reveals that surface design can effectively regulate the SEI layer composition and improve interface stability, which is a promising strategy for Si-electrode manufacture.

Thin lithium (Li) metal foils have been proved to be indispensable yet elusive for practical high-energy-density lithium batteries. Currently, the realization of such thin foils (<50 μm) is impeded by the inferior mechanical processability of metallic Li. In this work, we demonstrate that the combination of solid solution strengthening and second phase strengthening, achieved by the addition of silver fluoride (AgF) to Li metal, can substantially enhance both the strength and ductility of metallic Li. Benefiting from the improved machinability, we succeed in fabricating an ultrathin (down to 5 μm), freestanding, and mechanically robust Li-AgF composite foil. More interestingly, the in situ-formed Li x Ag-LiF skeleton in the composite facilitates Li diffusion kinetics and uniform Li deposition, where the thin Li-AgF electrode displays a prolonged cycle life over 500 h at 1 mA cm -2 and 1 mAh cm -2 in a carbonate electrolyte. Coupled with a commercial LiCoO 2 cathode (3.4 mAh cm -2 ), the LiCoO 2 ||Li-AgF cell delivers a notable capacity retention of ∼90% over 100 cycles at 0.5 C with a low negative/positive ratio of 2.5.

The "solvent-in-salt" electrolytes for an aqueous system, including "water-in-salt" electrolytes and "bisolvent-in-salt" electrolytes, have shown significantly improved electrochemical stability toward low-voltage anodes and high-voltage cathodes. However, the heavy use of salt raises concerns of high cost, high viscosity, inferior wettability, and poor low-temperature performance. Herein, a "localized bisolvent-in-salt electrolyte" is proposed by introducing 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) as the diluent to the high-concentration water/sulfolane hybrid (BSiS-SL) electrolytes, forming a ternary solvent-based electrolyte, Li(H 2 O) 0.9 SL 1.3 ·TTE 1.3 (HS-TTE). The introduction of TTE dilutes the compact ionic clusters, while the original primary Li + solvation structure remains, and in the meantime, boosts the formation of a robust solid electrolyte interphase. As a result, a wide electrochemically stable window of 4.4 V is achieved. In comparison with the bisolvent BSiS-SL system, the trisolvent HS-TTE electrolyte exhibits a low salt concentration of 2.1 mol kg -1 , resulting in drastically reduced viscosity, superb separator wettability, and largely improved low-temperature performance. The constructed 2.5 V Li 4 Ti 5 O 12 /LiMn 2 O 4 cell shows an excellent capacity retention of 80.7% after 800 cycles, and the cell can even work at -30 °C. With these extraordinary advantages, the fundamental designing strategy of the HS-TTE electrolyte developed in this work can promote the practical applications of solvent-in-salt electrolytes.

Hydrogen produced from neutral seawater electrolysis faces many challenges including high energy consumption, the corrosion/side reactions caused by Cl - , and the blockage of active sites by Ca 2+ /Mg 2+ precipitates. Herein, we design a pH-asymmetric electrolyzer with a Na + exchange membrane for direct seawater electrolysis, which can simultaneously prevent Cl - corrosion and Ca 2+ /Mg 2+ precipitation and harvest the chemical potentials between the different electrolytes to reduce the required voltage. In-situ Raman spectroscopy and density functional theory calculations reveal that water dissociation can be promoted with a catalyst based on atomically dispersed Pt anchored to Ni-Fe-P nanowires with a reduced energy barrier (by 0.26 eV), thus accelerating the hydrogen evolution kinetics in seawater. Consequently, the asymmetric electrolyzer exhibits current densities of 10 mA cm -2 and 100 mA cm -2 at voltages of 1.31 V and 1.46 V, respectively. It can also reach 400 mA cm -2 at a low voltage of 1.66 V at 80 °C, corresponding to the electricity cost of US$1.36 per kg of H 2 ($0.031/kW h for the electricity bill), lower than the United States Department of Energy 2025 target (US$1.4 per kg of H 2 )., (© 2023. The Author(s).)