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The rechargeable magnesium battery (RMB) is regarded as a high-energy, safe, and cost-effective alternative for conventional batteries. Unfortunately, the passivation and uneven Mg growth not only raise the voltage hysteresis but also shorten the cycle life of RMBs. In this review, Mg passivation induced by electrolytes/contaminants, growth patterns of high dimensional Mg 0 , and mechanisms of Mg anode degradation are discussed. The recent efforts on suppressing electrolyte decomposition and uneven Mg growth including electrolyte/interphase modifications through additives, weakly coordinating anions, artificial interphases, and 3D magnesiophilic hosts are summarized. Finally, the future directions in stabilizing Mg anode and realizing high-performance RMBs are highlighted., (© 2022 Wiley-VCH GmbH.)

In this Full Paper we show that the use of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as conducting salt in commercial lithium-ion batteries is made possible by introducing fluorinated linear carbonates as electrolyte (co)solvents. Electrolyte compositions based on LiTFSI and fluorinated carbonates were characterized regarding their ionic conductivity and electrochemical stability towards oxidation and with respect to their ability to form a protective film of aluminum fluoride on the aluminum surface. Moreover, the investigation of the electrochemical performance of standard lithium-ion anodes (graphite) and cathodes (Li[Ni1/3 Mn1/3 Co1/3 ]O2 , NMC) in half-cell configuration showed stable cycle life and good rate capability. Finally, an NMC/graphite full-cell confirmed the suitability of such electrolyte compositions for practical lithium-ion cells, thus enabling the complete replacement of LiPF6 and allowing the realization of substantially safer lithium-ion batteries., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

To ensure optimal operation of electrochemical energy storage devices, a precise design of the interfaces formed between the electrodes and the electrolyte is essential. Si is a promising anode active material for Li-ion batteries owing to its high theoretical capacity; however, the large volume change associated with Li absorption and release hinders its practical applications. The development of high-performance storage batteries depends on the construction of an electrode-electrolyte interface that facilitates Li+ movement. To this aim, the authors have developed Si-specific interface observation methods. In this feature article, we review and discuss recent advances in the reaction behavior of Si-based anodes, particularly at the Si electrode-electrolyte interface. [ABSTRACT FROM AUTHOR]

[Display omitted] Alloying-type anode materials are considered promising candidates for next-generation alkali-ion batteries. However, they face significant challenges owing to severe volume variations and sluggish kinetics, which hinder their practical applications. To address these issues, we propose a universal synthetic strategy, which can realize the facile synthesis of various alloying-type anode materials composed of a porous carbon matrix with uniformly embedded nanoparticles (Sb, Bi, or Sn). Besides, we construct the interactions among active materials, electrolyte compositions, and the resulting interface chemistries. This understanding assists in establishing balanced kinetics and stability. As a result, the fabricated battery cells based on the above strategy demonstrate high reversible capacity (515.6 mAh g−1), long cycle life (200 cycles), and excellent high-rate capability (at 5.0 C). Additionally, it shows improved thermal stability at 45 and 60 °C. Moreover, our alloying-type anodes exhibit significant potential for constructing a 450 Wh kg−1 battery system. This proposed strategy could boost the development of alloying-type anode materials, aligning with the future demands for low-cost, high stability, high safety, wide-temperature, and fast-charging battery systems. [ABSTRACT FROM AUTHOR]

Uncontrolled dendrite growth and electrolyte‐induced intricate parasitic reactions are two great challenges that hinder the commercial applications of aqueous zinc‐ion batteries. Herein, a synchronous modulation strategy for Zn2+ interfacial migration behavior and electrolyte microenvironment is proposed by constructing a functional lanthanum hydroxide aerogel (LAG) interface layer on Zn anode surface. The in situ derivation of ion‐conducting zinc hydroxide sulfate (ZHS) from LAG layer results in the spontaneous generation of a hierarchic interface layer during the plating process, where the high Zn2+ selectivity of the upper dense ZHS layer can limit SO42− migration and allow for fast Zn2+ interfacial migration kinetics, while the aerogel layer with well‐defined nanochannels near the anode side can homogenize Zn2+ distribution, thus leading to the effective suppression of both dendrites and side reactions. Additionally, the pH microenvironment of the acidic electrolyte can be synchronously regulated by slightly soluble La(OH)3 aerogel, further inhibiting electrolyte corrosion and HER. Consequently, the modified Zn anode delivers highly reversible Zn plating/stripping and low‐voltage hysteresis, and the high areal‐capacity Zn||MnO2 full cells demonstrate considerable electrochemical performances under high Zn utilization conditions. This functional aerogel‐driven synchronous modulation strategy of Zn2+ migration behavior and electrolyte microenvironment provides new insight for stabilizing Zn metal anodes. [ABSTRACT FROM AUTHOR]

[Display omitted] • The H 2 under organic acid regulates the reaction rate and protects the (0 0 2) crystal planes, initiating ultrathin SEI within 1 min. • The exposed (0 0 2) planes induce uniform deposition and enhance corrosion-resistance. • This SEI with organic groups exhibits excellent compatibility, low resistance and isolation of electrolyte/anode. • The ZAC1@Zn possesses practical application value due to the rapid preparation within 1 min and resistance to high current shock. Organic acid treatment can facilitate the in-situ formation of a solid electrolyte interface (SEI) on Zn foil protecting the anode from corrosion. However, the generation of hydrogen (H 2) during this process is inevitable, which is often considered detrimental to getting compact SEI. Herein, a H 2 film-assisted method is proposed under concentrated Amino-Trimethylene-Phosphonic-Acid to construct ultrathin and dense SEI within 1 min. Specifically, the (0 0 2) crystal planes survive from the etching process of 1 min due to the adhered H 2 , inducing uniform deposition and enhanced corrosion-resistance. Moreover, the H 2 can effectively regulate the reaction rate, leading to ultrathin SEI and initiating a morphology preservation behavior, which has been neglected by the previous reports. The quick-formed SEI has excellent compatibility, low resistance and effective isolation of electrolyte/anode, whose advantages work together with exposed (0 0 2) planes to get accustomed to high-current surge, leading to the ZAC1@Zn//ZAC1@Zn consistently cycling over 800 h at 15 mA cm−2 and 15 mAh cm−2, the ZAC1@Zn//Cu preserves high reversibility (CE 99.7 %), and the ZAC1@Zn//MVO exhibits notable capacity retention at 191.7 mAh/g after 1000 cycles. [ABSTRACT FROM AUTHOR]

The integration of Si‐based anodes within sulfide‐based solid electrolyte (SSE) Li‐ion batteries (LIB) has emerged as a promising avenue of research and development, attracting increasing interest in recent years. This work comprehensively examines the latest research directions and major strides in this field. It covers the key advances in the design and engineering of nano‐ and micro‐structured Si anode architectures, and strategies of surface modification. Additionally, it explores the impacts of external pressure, the role of binders and conductive additives, and the implications of varying Si particle size. Beyond providing a detailed account of the evolution of Si anodes within SSE LIBs, this work also identifies critical research challenges that urgently need addressing. These include the electrochemical‐mechanical evolution behavior and failure mechanism of Si anodes in SSE LIBs, strategies for structural and interface modifications, methods for preparing Si electrodes, advancements in high‐performance SSEs, and the development of scalable technologies for SSE thin films. Moreover, it discusses high‐energy cathodes tailored for Si‐based SSE LIBs. The identified research priorities are set to offer crucial guidance and insights, supporting the ongoing investigations and innovations in this dynamic area of research. [ABSTRACT FROM AUTHOR]

Combining high‐voltage nickel‐rich cathodes with lithium metal anodes is among the most promising approaches for achieving high‐energy‐density lithium batteries. However, most current electrolytes fail to simultaneously satisfy the compatibility requirements for the lithium metal anode and the tolerance for the ultra‐high voltage NCM811 cathode. Here, we have designed an ultra‐oxidation‐resistant electrolyte by meticulously adjusting the composition of fluorinated carbonates. Our study reveals that a solid‐electrolyte interphase (SEI) rich in LiF and Li2O is constructed on the lithium anode through the synergistic decomposition of the fluorinated solvents and PF6− anion, facilitating smooth lithium metal deposition. The superior oxidation resistance of our electrolyte enables the Li||NCM811 cell to deliver a capacity retention of 80 % after 300 cycles at an ultrahigh cut–off voltage of 4.8 V. Additionally, a pioneering 4.8 V‐class lithium metal pouch cell with an energy density of 462.2 Wh kg−1 stably cycles for 110 cycles under harsh conditions of high cathode loading (30 mg cm−2), low N/P ratio (1.18), and lean electrolytes (2.3 g Ah−1). [ABSTRACT FROM AUTHOR]

Sulfurized polyacrylonitrile (SPAN) cathodes in high energy‐density Li‐metal batteries have garnered widespread interest owing to their good cycling stability and moderately high capacities. However, their application is hindered by the low prevalence of advanced electrolytes that can simultaneously mitigate polysulfide generation at the cathode and stabilize the Li‐metal anode. Here, a weakly solvating electrolyte is presented, employing a single solvent tetrahydropyran (THP). The solvation structure is effectively tuned by adjusting the salt concentration to stabilize both the Li‐metal anode and SPAN cathode. This approach enables stable cycling with high SPAN loadings (≈5 mg cm−2) and lean electrolyte contents (≈5 µL mgSPAN−1) across a wide temperature range: 0 °C, room temperature, and 50 °C. A pouch cell with a high SPAN loading and a low electrolyte‐to‐SPAN (E/SPAN) ratio of 3 µL mg−1 shows a stable 79.1% capacity retention after 40 cycles. Additionally, THP can be effectively employed in localized high‐concentration electrolyte (LHCE) systems to reduce the diluent‐to‐solvent ratio for greater LHCE viability. The study demonstrates the potential of weakly solvating solvents in Li‐SPAN batteries, offering a pathway for their practical application. [ABSTRACT FROM AUTHOR]

The practical application of silicon (Si)‐based anodes faces challenges due to severe structural and interphasial degradations. These challenges are exacerbated in lithium‐ion batteries (LIBs) employing Si‐based anodes with high‐nickel layered oxide cathodes, as significant transition‐metal crossover catalyzes serious parasitic side reactions, leading to faster cell failure. While enhancing the mechanical properties of polymer binders has been acknowledged as an effective means of improving solid‐electrolyte interphase (SEI) stability on Si‐based anodes, an in‐depth understanding of how the binder chemistry influences the SEI is lacking. Herein, a zwitterionic binder with an ability to manipulate the chemical composition and spatial distribution of the SEI layer is designed for Si‐based anodes. It is evidenced that the electrically charged microenvironment created by the zwitterionic species alters the solvation environment on the Si‐based anode, featuring rich anions and weakened Li+‐solvent interactions. Such a binder‐regulated solvation environment induces a thin, uniform, robust SEI on Si‐based anodes, which is found to be the key to withstanding transition‐metal deposition and minimizing their detrimental impact on catalyzing electrolyte decomposition and devitalizing bulk Si. As a result, albeit possessing comparable mechanical properties to those of commercial binders, the zwitterionic binder enables superior cycling performances in high‐energy‐density LIBs under demanding operating conditions. [ABSTRACT FROM AUTHOR]

All‐solid‐state batteries (ASSBs), particularly those with Li‐free anodes or even anode‐free configurations, have attracted extensive attention due to high safety and energy density. However, chemical‐mechanical degradation typically deteriorates the cycle life and energy of Li‐free anode ASSBs with the absence of Li inventory. Here, the prelithiation agent Li5FeO4 (LFO) coated Ni‐rich layered oxide is developed as the cathode for Li‐free anode ASSBs. The coated LFO acts as an interfacial protective layer to prevent the highly oxidizing Ni‐rich cathode from reacting with sulfide solid‐state electrolytes (SSEs), mitigating the structural degradation of Ni‐rich cathodes and the decomposition of SSE, resulting in excellent cycle life. Beneficial from the coated LFO in the cathode of the Li‐free anode ASSBs, the reversible capacity improves from 174.7 mAh g−1 to 199.7 mAh g−1, and the capacity retention is enhanced from 33.8 % to 84.8 % after 100 cycles. Additionally, an ultrahigh energy density of 440 Wh kg−1, based on the mass of the composite cathode, Li‐free anode, and SSE, is obtained in a Li‐free anode all‐solid‐state pouch cell equipped with the LFO‐coated cathode. [ABSTRACT FROM AUTHOR]

Homogeneous Li‐ion flux is a significant precondition of uniform Li‐ion deposition in Li metal batteries (LMBs). Numerous methodologies have been presented for homogenizing Li‐ion flux before Li deposition based on the features of Li‐ion deposition. Separators that provide Li‐ion transfer channels and are directly exposed to Li metal anodes have attracted rising attention for their role in guiding regular Li‐ion distribution. More novel functional separators have been proposed aiming to achieve dendrite‐free deposition. Herein, the factors and strategies that regulate Li‐ion distribution through functional separators toward LMBs are concentrated on. The current mechanisms of Li‐ion flux regulation by functional separators are first highlighted, including physical properties, interactions with the electrolyte, and modification of the solid‐state electrolyte interphase. According to these mechanisms, functional separator strategies for regulating Li‐ion flux are divided into three methodologies, and typical examples are introduced. Finally, current limitations and suggestions for future functional separator studies are presented, aiming to inspire engaged researchers and newcomers to trigger more exciting works in this area. [ABSTRACT FROM AUTHOR]

Parasitic side reactions and dendrite growth on zinc anodes are formidable issues causing limited lifetime of aqueous zinc ion batteries (ZIBs). Herein, a spontaneous cascade optimization strategy is first proposed to regulate Zn2+ migration‐diffusion behavior. Specifically, PAPE@Zn layer with separation‐reconstruction properties is constructed in situ on Zn anode. In this layer, well‐soluble poly(ethylene oxide) (PEO) can spontaneously separation to bulk electrolyte and weaken the preferential coordination between H2O and Zn2+ to achieve primary optimization. Meanwhile, poor‐soluble polymerized‐4‐acryloylmorpholine (PACMO) is reconstructed on Zn anode as hydrophobic flower‐like arrays with abundant zincophilic sites, further guiding the de‐solvation and homogeneous diffusion of Zn2+ to achieve the secondary optimization. Cascade optimization effectively regulates Zn2+ migration‐diffusion behavior, dendrite growth and side reactions of Zn anode are negligible, and the stability is significantly improved. Consequently, symmetrical cells exhibit stability over 4000 h (1 mA cm−2). PAPE@Zn//NH4+−V2O5 full cells with a high current density of 15 A g−1 maintains 72.2 % capacity retention for 12000 cycles. Even better, the full cell demonstrates excellent performance of cumulative capacity of 2.33 Ah cm−2 at ultra‐low negative/positive (N/P) ratio of 0.6 and a high mass‐loading (~17 mg cm−2). The spontaneous cascade optimization strategy provides novel path to achieve high‐performance and practical ZIBs. [ABSTRACT FROM AUTHOR]

In the pursuit of next‐generation ultrahigh‐energy‐density Li−O2 batteries, it is imperative to develop an electrolyte with stability against the strong oxidation environments. N,N‐dimethylacetamide (DMA) is a recognized solvent known for its robust resistance to the highly reactive reduced oxygen species, yet its application in Li−O2 batteries has been constrained due to its poor compatibility with the Li metal anode. In this study, a rationally selected hydrofluoroether diluent, methyl nonafluorobutyl ether (M3), has been introduced into the DMA‐based electrolyte to construct a localized high concentration electrolyte. The stable −CH3 and C−F bonds within the M3 structure could not only augment the fundamental properties of the electrolyte but also fortify its resilience against attacks from O2− and 1O2. Additionally, the strong electron‐withdrawing groups (−F) presented in the M3 diluent could facilitate coordination with the electron‐donating groups (−CH3) in the DMA solvent. This intermolecular interaction promotes more alignments of Li+‐anions with a small amount of M3 addition, leading to the construction of an anion‐derived inorganic‐rich SEI that enhances the stability of the Li anode. As a result, the Li−O2 batteries with the DMA/M3 electrolyte exhibit superior cycling performance at both 30 °C (359th) and −10 °C (120th). [ABSTRACT FROM AUTHOR]

Aqueous electrolyte additives are considered one of the most promising agents for improving the cycling stability and practicality of aqueous zinc-ion batteries (AZIBs) due to their multiple functions, low cost, and easy operation. The application of these electrolyte additives could significantly suppress the corrosion reaction, dendrite growth, and the hydrogen evolution reaction originating from the zinc anodes. In light of the intensive research of electrolyte additives and the significant progress that have been made in recent years, this review will focus on the mechanism and nature behind the improved performance contributed by the additives. A comprehensive overview of the origins of the challenges above will be presented firstly. Furthermore, the basic function principles of most reported additives are summarized and categorized, aiming to induce a deep and logical consideration of the use of the electrolyte additives in practical or large capacity cells. Finally, this review outlines the prospective advancement of electrolyte additives, inspiring the application of advanced characterization techniques in enhancing the understanding of AZIBs and laying the groundwork for the possibility of commercialization of AZIBs. [ABSTRACT FROM AUTHOR]

Owing to the abundant reserves and low cost, sodium‐ion batteries (SIBs) have garnered unprecedented attention. However, their widespread adoption is hindered by the scarcity of alternative anodes with fast‐charging capability and high stability. To overcome this challenge, a fast‐charging SIB anode, N‐doped Bi/BiOCl embedded in a carbon framework (Bi/BiOCl@NC) with a fast Na+ transport channel and ultra‐high structural stability, is developed. During cycling in ether electrolyte, Bi/BiOCl@NC undergoes a remarkable transformation into a 3D porous skeleton, which significantly reduces the Na+ transport pathway and accommodates volume changes. By employing density functional theory calculations to simulate the storage behavior of Na+ in the structure, Bi/BiOCl@NC is theoretically characterized to have a low Na+ transport barrier (0.056 eV) and outstanding electronic conductivity. Such unique characteristics induce Bi/BiOCl@NC anode to have an ultra‐high Na+ storage capacity of 410 mAh·g−1 at 20 A·g−1 and exhibit outstanding cycling stability with over 2300 cycles at 10 A·g−1. This study provides a rational scenario for the fast‐charging anode design and will enlighten more advanced research to promote the exploitation of SIBs. [ABSTRACT FROM AUTHOR]

Silicon (Si) is considered to be the promising candidate anode for the next generation of high‐energy‐density batteries. However, the poor initial coulombic efficiency (ICE) and rate performance severely hinder its commercial development. Here, fully exploits the 2D structure of photovoltaic silicon waste (PV‐WSi), combining with the advantage of controllable depositing layers offered by fluidized bed atomic layer deposition (FBALD), to simultaneously achieve high ICE and highrate performance of Si‐based anodes. The characteristic of Li+ embedding vertically into the plane direction of the 2D sheet‐like structure of PV‐WSi helps shorten the diffusion distance, alleviating the pulverization problem caused by volume expansion. FBALD is utilized to controllably deposit Li2O (≈1 nm) and TiO2 (≈4 nm) layers to compensate for the loss of Li sources, further suppressing the volume expansion of Si and isolating the side reactions between Si and electrolyte. The prepared Si@Li2O@TiO2 demonstrates ultrahigh ICE (90.9%) and outstanding rate performance (>900 mAh g−1 at a rate of 20 A g−1). Full cells with the Si@Li2O@TiO2 anode and LiFePO4 cathode deliver a stable capacity of 100 mAh g−1 after 300 cycles at 0.5 C. This work provides new ideas for the development of high ICE, high‐rate Si‐based anodes based on low‐cost photovoltaic waste. [ABSTRACT FROM AUTHOR]

Gel electrolyte is one of the key components of flexible energy storage devices. The construction of a three‐dimensional (3D) porous gel electrolyte with high ionic conductivity is a very effective strategy to improve the performance of zinc‐ion batteries (ZIBs). Herein, porous polyvinyl alcohol‐Agar‐sodium dodecyl sulfate‐MXene‐dimethyl sulfoxide (DMSO) (denoted as PVA‐Agar‐SDS‐MXene‐DMSO (PASMD)) gel electrolyte with double network is prepared through one‐pot method by adding two‐dimensional (2D) MXene to improve its ionic conductivity and DMSO to increase its low‐temperature resistance. Meanwhile, the as‐prepared PASMD gel electrolyte with a high ionic conductivity of 50.63 mS cm−1 realizes the gradient induction and redistribution of Zn2+, which drives oriented Zn (002) plane deposition of Zn2+ and then achieves uniform Zn deposition and dendrite‐free anode. The specific capacity of the assembled flexible Zn//PASMD//β‐MnO2 battery can reach 205 mAh g−1 at 0.2 A g−1. It also exhibits good performance both at room temperature and −20 °C with stable cyclic stability for more than 1000 h. After 1000 cycles at 1 A g−1, the assembled flexible battery stabilizes at 67 mAh g−1. This work provides an alternative pathway for the development of high‐performance gel electrolytes with low‐temperature resistance and high‐ionic conductivity for flexible ZIBs. [ABSTRACT FROM AUTHOR]

Achieving good compatibility between anodes and cathodes with electrolytes still faces great challenges in Mg metal batteries (MMBs). Recently developed amine‐based electrolytes have enabled reversible Mg anodes with conventional Mg salts through solvation structure regulations but still suffer from low conductivity and poor cathode compatibility. Herein, a Li/Mg double‐salt strategy is proposed to achieve the bulk phase‐interface‐electrode multi‐scale optimization for the amine‐based electrolyte, including ionic conductivity, anode stability, and cathode compatibility. Lithium triflate (LiOTf) serves as a multifunctional additive to compensate for the limitations of single Mg salt electrolyte (MgCl2/3‐methoxypropylamine). Li+ ions accelerate the ions transport in the bulk phase and ions insertion at the cathode side, benefitting to the conductivity and the cathode compatibility. Attributed to the high reduction stability of OTf− anions, the stable Mg anode/interface is also retained. Therefore, the Mg//SS cell achieves an ultralong cycling life for 2100 cycles with the coulombic efficiency of 99.8% at 1.0 mA cm−2 and the full cell also exhibits a superior cycling performance for 1000 cycles at 5 C. Additionally, the batteries with the optimized electrolyte are verified as a proof‐of‐concept for the air‐assembled MMBs. This work emphasizes the crucial role of multifunctional additives in enhancing amine‐based electrolyte performances. [ABSTRACT FROM AUTHOR]

Layered silicon (L–Si) anodes are celebrated for their high theoretical capacity but face significant challenges regarding safety and material purity during preparation. This study addresses these challenges by employing NH4Cl–CaSi2 as the raw material in a gas-solid de-alloying process, which enhances both safety and purity compared to traditional methods. The L–Si anodes produced demonstrate outstanding electrochemical performance, delivering a high reversible lithium storage capacity of 1497.7 mA h g−1 at a current density of 0.5 A g−1, and exhibiting stable performance over 1200 charge–discharge cycles. In situ and ex situ characterizations reveal that electrolyte decomposition products effectively fill the voids within the electrode, while the gradual disintegration of the L–Si structure contributes to the formation of a dense, conductive network. This process enhances lithium ion transport and exploits the capacitive storage benefits of layered silicon. [ABSTRACT FROM AUTHOR]

Stabilizing the electrode interphases is urgently required to enhance the lifetime of high‐voltage sodium‐ion batteries (SIBs). However, the continuous anode solid–electrolyte interphase (SEI) growth associated with electron leakage and the fragile cathode–electrolyte interphase (CEI) lead to capacity fade at high voltage; and yet the solvation‐interphase‐performance relationship is inadequately addressed. Herein, a cooperative Na+‐solvation strategy is reported to stabilize the interphases by a holistic design of electrolytes combining soft and moderate co‐solvents. The rationally regulated Na+‐solvation leads to CEI/SEI with the desired thickness and component stability. As such, remarkable cycling stability is achieved for 4.3‐V Na3V2O2(PO4)2F (NVOPF) cathodes with 83.3% capacity retention over 3000 cycles at 1 C, significantly outperforming the carbonate counterpart (41.6% capacity retention). Meanwhile, the restrained SEI growth via reducing the formation of electron‐leaking Na2CO3 stabilizes the long‐term cycling of the hard carbon (HC) anode. The assembled NVOPF||HC full cells achieve superior rate capability (up to 15 C) and stable cycling stability over 500 cycles. The demonstrated engineering of electrolyte chemistry, Na+‐solvation, and interphase structure/component contributes toward the rational establishment of design rules for high‐voltage SIBs and possibly other similar chemistries. [ABSTRACT FROM AUTHOR]

Silicon (Si), stands out for its abundant resources, eco‐friendliness, affordability, high capacity, and low operating potential, making it a prime candidate for high‐energy‐density lithium‐ion batteries (LIBs). Notably, the breakthrough use of nanostructured Si (nSi) has paved the way for the commercialization of Si anodes. Despite this, challenges like high processing costs, severe side reactions, and low volumetric energy density have impeded widespread industrial adoption. Micron‐scale Si (µSi) has always faced setbacks compared to nSi due to its greater volume expansion. However, recent years have witnessed a resurgence of interest in µSi‐based anodes. Capitalizing on its inherent advantages, including low cost and high tap density, µSi has once again captured the attention of both academic and industrial communities. This review begins by contrasting the strengths and weaknesses of µSi and nSi, then outline potential solutions to enhance µSi performance, covering aspects like structural regulation, composite anodes, binder design, and electrolyte exploration. Additionally, this work explores the application of machine learning‐assisted high‐throughput screening. Concluding the review, this work provides insights into the future prospects of µSi in LIBs, outlining challenges and proposing integrated coping strategies. This review anticipates that it will provide valuable perspectives for the commercial application of high‐energy‐density Si‐based anodes. [ABSTRACT FROM AUTHOR]

Fluorinated‐ethers are promising electrolyte solvents in lithium metal batteries, for their high antioxidant and excellent reductive stability on Li anode. However, fluorinated‐ethers with high fluorination degree suffer from low ionic conductivity and narrow temperature adaptibility. Herein, we synthesize a mono‐fluorinated linear ether of bis(2‐fluoroethoxy) methane (BFME) with enhanced solvated ability. The −OCH2O− structure and fluoride substitution on the β‐C position endows the BFME electrolyte with moderate affinity to Li+, thereby improving the ionic conductivity and decreasing the Li+‐desolvation energy barrier at a wide temperature range of −60–60 °C. Additionally, the electrolyte with anion‐participated solvation structure demonstrates high film‐forming ability by forming LiF‐rich interfacial film on the electrode surfaces, rendering the graphite anode with an initial Coulombic efficiency (CE) of 94.9 % and a Li plating/stripping CE of 99.8 % by Aurbach method. Consequently, the Graphite||LiFePO4 pouch cells delivered 83.2 %, 92.5 % and 81.2 % capacity retention after 1250, 200 and 300 cycles at 25, −20 °C and 60 °C, respectively. Moreover, the Li||LFP pouch cell with 3 Ah capacity can operate for 65 cycles with 99 % capacity retention, verifying the effectiveness of the BFME electrolyte in stabilizing the interfaces and broadening the temperature adaptibility of lithium‐ion and lithium metal batteries. [ABSTRACT FROM AUTHOR]

Fe2NiSe4@holey-graphene (FNS@HG) has been prepared by in situ growth and simultaneous perforation via a carbothermal reaction. The generation of nanoholes on the graphene sheets significantly reduced the diffusion distance of electrolyte ions, enhancing the rate capability of FNS@HG as an anode material for sodium-ion batteries. [ABSTRACT FROM AUTHOR]

Hard carbon (HC) is the most commonly used anode material in sodium‐ion batteries. However, the solid‐electrolyte‐interface (SEI) layer formed in carbonate ester‐based electrolytes has an imperceptible dissolution tendency and a sluggish Na+ diffusion kinetics, resulting in an unsatisfactory performance of HC anode. Given that electrode/electrolyte interface property is highly dependent on the configuration of Helmholtz plane, we filtrated proper solvents by PFBE (PF6− anion binding energy) and CAE (carbon absorption energy) and disclosed the function of chosen TFEP to reconstruct the Helmholtz plane and regulate the SEI film on HC anode. Benefiting from the preferential adsorption tendency on HC surface and strong anion‐dragging interaction of TFEP, a robust and thin anion‐derived F‐rich SEI film is established, which greatly enhances the mechanical stability and the Na+ ion diffusion kinetics of the electrode/electrolyte interface. The rationally designed TFEP‐based electrolyte endows Na||HC half‐cell and 2.8 Ah HC||Na4Fe3(PO4)2P2O7 pouch cell with excellent rate capability, long cycle life, high safety and low‐temperature adaptability. It is believed that this insightful recognition of tuning interface properties will pave a new avenue in the design of compatible electrolyte for low‐cost, long‐life, and high‐safe sodium‐ion batteries. [ABSTRACT FROM AUTHOR]

Rechargeable magnesium‐ion batteries (RMBs) have garnered increasing research interest in the field of post‐lithium‐ion battery technologies owing to their potential for high energy density, enhanced safety, cost‐effectiveness, and material resourcefulness. Despite substantial advancements in RMB research, a number of intrinsic challenges remain unresolved, such as the strong Coulombic interaction between Mg2+ and the host crystal structure of cathode materials, sluggish Mg2+ diffusion kinetic, poor electrolyte compatibility, and the formation of passivation films on the Mg anode interface. These issues hinder the commercial applications of RMBs. This review provides a comprehensive overview of the progress in key areas of RMB research, including representative magnesium‐ion storage cathode/anode materials and magnesium‐ion conducting electrolytes. Additionally, recent developments in electrode‐electrolyte interface regulations and pouch‐cell fabrication are outlined, highlighting current challenges and the implementation of effective solutions. Finally, future research directions are proposed to guide the development of high‐performance RMBs with practical applications. [ABSTRACT FROM AUTHOR]

Understanding and controlling parasitic reactions on the Zn metal anode (ZMA) surface is essential to enhance the energy capabilities of aqueous zinc‐ion batteries (ZIBs). However, the accurate regulation scheme is often obscured due to the lack of fundamental understanding concerning the ZMA/electrolyte interface. Herein, the descriptor of interfacial parasitic reactions is revealed through a systematic comparative study of three model trace adsorption‐type pyridinesulfonic acid‐based additives with structural variations. Using in situ spectroscopies coupled with density functional theory calculations, direct spectroscopic evidence of interfacial H2O evolution during Zn2+ deposition process is obtained. It is proposed that, beyond the traditional cognitions, the distance between solvated Zn(H2O)62+ and ZMA surface highly dictates the stability of ZMAs. Consequently, the trace 3‐Pyridinesulfonic acid with most effective capacity to drive solvated Zn(H2O)62+ away from the ZMA surface, enables a robust cycle life over 420 h for the Zn||Zn symmetric cell at 10 mA cm−2/10 mAh cm−2 (depth of discharge of 45%), a high Coulombic efficiency of 99.78% and an extended cycling life of 1500 cycles for the Zn//NH4V4O10 full battery. The work sheds light on the underlying mechanism of parasitic reactions on ZMA surface and provides fundamental insights into the design of trace additives for better ZIBs. [ABSTRACT FROM AUTHOR]

Lithium‐ion batteries (LIBs) built on inorganic anodes have achieved great commercial success. By contrast, the practical application of organic anode materials encounters key bottlenecks including electronic insulation, high solubility, and poor initial coulombic efficiency (ICE). Among them, improving ICEs (normally 30–60%) faces enormous challenges in both theory and technology, and there has been no substantial breakthrough yet. Herein, a wet chemical pretreatment technology to increase the ICE of maleic acid (MA)‐based anodes from 43.2% to nearly 100% is proposed for the first time, and this strategy demonstrates universal applicability. Typically, the wet chemical pretreatment involves reacting with lithium‐biphenyl to form LixMA intermediates (x = 4–6) and further forming a compact artificial solid‐electrolyte interphase (SEI) film through the spontaneous reaction between active LixMA and battery organic electrolytes. This wet chemically‐constructed artificial SEI layer can almost completely suppress lithium loss in the initial cycle of the MA electrode and significantly boost the actual output energy density, rate capability, and cycling durability of MA anode‐based full batteries. Significantly, the study further demonstrated that a series of organic anode materials with high ICEs can be achieved through similar wet chemical pretreatment. This work will open up the true application of high‐ICE organic anodes in LIBs. [ABSTRACT FROM AUTHOR]

In this study, the impact of microstructural properties of the anode support layer (ASL) composed of catalyst, electrolyte and pore phases on the performance of solid oxide fuel cell (SOFC) is investigated. Synthetic SOFC anode microstructures, comprising two layers including the anode functional layer (AFL), where electrochemical reactions take place, are generated using an open-source software. Different configurations of the anode support layer with various particle sizes and volume fractions of the catalyst and electrolyte phases for different porosities are combined with a consistent AFL to isolate the effect of ASL microstructural parameters. The triple phase boundary (TPB) density, chosen as a useful metric monitoring the anode performance, is then quantitively determined for each anode layer and entire anode in all reconstructed microstructures. The results demonstrate that the microstructure of ASL significantly influences the anode and thus cell performance by impacting reactant gas supply and current collection, emphasizing the necessity for meticulous design. Specifically, ASL microstructures with low volume fractions of Ni and the pore phase, and/or substantial differences between the volume fractions of the phases, are observed to result in discontinuous phase networks, which deactivate TPBs in AFL. • Impact of microstructural properties of the anode support layer is investigated. • Synthetic SOFC anode microstructures, comprising two layers, are reconstructed. • Triple phase boundary density is quantitatively determined. • Low volume fractions of catalyst/pore phase result in discontinuous phase networks. • Anode support should have pore and catalyst phases with close volume fractions. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐iodine (Zn─I2) battery is a promising energy storage system due to its inherent safety, high theoretical capacity, sustainability, and cost‐effectiveness. However, the shuttle effect of polyiodide severely affects the stable loading of active iodine and even accelerates the corrosion of the Zn anode, thus impeding its further advancement. Herein, a unique trimethylsulfonium cation (TMS+) with strong adsorption is proposed to stabilize both the iodine cathode and Zn anode. Benefiting from the robust interaction between TMS+ and polyiodide, the electrolyte can effectively immobilize large‐capacity iodine in the form of oily precipitate, thus avoiding the shuttle effect of polyiodide and the Zn corrosion. Additionally, TMS+ can be preferentially adsorbed on various Zn facets, inducing an electrostatic shielding effect to inhibit Zn dendrite growth. Consequently, Zn anode can be stably cycled over 3400 h at 5 mA cm−2/5 mAh cm−2, and a large areal capacity of 2.71 mAh cm−2 as well as long‐life stability over 6400 cycles is achieved for Zn─I2 battery. Furthermore, cation adsorption engineering is practically utilized in pouch cells, realizing superior fast‐charging stability over 790 cycles. This electrolyte modification with dual stabilizations is anticipated to be applied to other metal‐iodine batteries as a cost‐effective, facile, and safe strategy. [ABSTRACT FROM AUTHOR]

The commercialization of all‐solid‐state Li batteries (ASSLBs) demands solid electrolytes with strong cost‐competitiveness, low density (for enabling satisfactory energy densities), and decent anode compatibility (the need for cathode compatibility can be circumvented by the cathode coating techniques that are widely applied in sulfide‐based ASSLBs). However, none of the reported oxide, sulfide, or chloride solid electrolytes meets these requirements simultaneously. Here, we design a Li7P3S7.5O3.5 (LPSO) solid electrolyte, which shows a combination of all the aforementioned characteristics. The synthesis of this material does not need the expensive Li2S, so the raw materials cost is only $14.42/kg, which, unlike most solid electrolytes, lies below the $50/kg threshold for commercialization. The density of LPSO is 1.70 g cm−3, considerably lower than those of the oxide (typically above 5 g cm−3) and chloride (around 2.5 g cm−3) solid electrolytes. Besides, LPSO also shows excellent anode compatibility. The Li|LPSO|Li cell cycles stably with a potential of ~50 mV under 0.1 mA cm−2 for over 4200 h at 25 °C, and the all‐solid‐state pouch cell with the Si anode shows a capacity retention of 89.29 % after 200 cycles under 88.6 mA g−1 at 60 °C. [ABSTRACT FROM AUTHOR]

A biomass-derived "zincophilic-hydrophobic" SEI layer is constructed on the Zn anode for dendrite-free, side reaction-free, and fast Zn electrodeposition. [Display omitted] Aqueous zinc ion batteries (AZIBs) face significant challenges stemming from Zn dendrite growth and water-contact attack, primarily due to the lack of a well-designed solid electrolyte interphase (SEI) to safeguard the Zn anode. Herein, we report a bio-mass derived polymer of chitin on Zn anode (Zn@chitin) as a novel and robust artificial SEI layer to boost the Zn anode rechargeability. The polymeric chitin SEI layer features both zincophilic and hydrophobic characteristics to target the suppressed dendritic Zn formation as well as the water-induced side reactions, thus harvesting a dendrite-free and corrosion-resistant Zn anode. More importantly, this polymeric interphase layer is strong and flexible accommodating the volume changes during repeated cycling. Based on these benefits, the Zn@chitin anode demonstrates prolonged cycling performance surpassing 1300 h under an ultra-large current density of 20 mA cm−2, and a long cycle life of 680 h with a record-high zinc utilization rate of 80 %. Besides, the assembled Zn@chitin/V 2 O 5 full batteries reveal excellent capacity retention and rate performance under practical conditions, proving the reliability of our proposed strategy for industrial AZIBs. Our research offers valuable insights for constructing high-performance AZIBs, and simultaneously realizes the high-efficient use of cheap biomass from a "waste-to-wealth" concept. [ABSTRACT FROM AUTHOR]

The cycling performance of zinc‐ion batteries is greatly affected by dendrite formation and side reactions on zinc anode, particularly in scenarios involving high depth of discharge (DOD) and low negative/positive capacity (N/P) ratios in full cells. Herein, drawing upon principles of host–guest interaction chemistry, we investigate the impact of molecular structure of electrolyte additives, specifically the −COOH and −OH groups, on the zinc negative electrode through molecular design. Our findings reveal that molecules containing these groups exhibit strong adsorption onto zinc anode surfaces and chelate with Zn2+, forming a H2O‐poor inner Helmholtz plane. This effectively suppresses side reactions and promotes dendrite‐free zinc deposition of exposed (002) facets, enhancing stability and reversibility of an average coulombic efficiency of 99.89 % with the introduction of Lactobionic acid (LA) additive. Under harsh conditions of 92 % DOD, Zn//Zn cells exhibit stable cycling at challenging current densities of 15 mA ⋅ cm−2. Even at a low N/P ratio of 1.3, Zn//NH4V4O10 full cells with LA electrolyte exhibit high‐capacity retention of 73 % after 300 cycles, significantly surpassing that of the blank electrolyte. Moreover, in a conversion type Zn//Br static battery with a high areal capacity (~5 mAh ⋅ cm−2), LA electrolyte sustains an improved cycling stability of 700 cycles. [ABSTRACT FROM AUTHOR]

The plating/stripping behavior of Zn ions on the Zn anode, driven by an electric field, is a key process in determining the performance of aqueous zinc ion batteries (AZIBs). Process‐induced unevenness of commercial Zn foils results in poor reversibility of Zn anodes. Herein, a self‐healing dynamic anode/electrolyte interface is constructed by incorporating hydroxyl‐rich alcohols with high charge density and zincophilicity into the original electrolyte. These alcohols selectively anchor on electron‐poor sites in the charging state, inducing domain‐limited deposition of Zn2+ to achieve a dense, uniform, and flat deposition state. As a result, a durable Zn anode with excellent electrochemical reversibility can be realized in practical cycling (average Coulombic efficiency of 99.5%). Even under deep plating/stripping conditions (5 mA cm−2 and 5mAh cm−2), the modified electrolyte exhibits a remarkable repair effect on corroded Zn anodes that have been cycled in base electrolyte, extending the lifespan to over 1,020 h. This represents a 15.6‐fold enhancement in lifespan compared to recycling in the base electrolyte. This strategy for electrolyte additive directly influences the design of ultra‐long‐life AZIBs and provides concrete concepts for the recovery of zinc anodes. [ABSTRACT FROM AUTHOR]

Rechargeable zinc batteries are promising choices for eco‐friendly, safe and cost‐effective energy storage solutions. However, their commercial adoption faces challenges such as low Coulombic efficiency (CE) and poor reversibility of Zn anodes. To address these issues, a new green electrolyte based on N,N'‐Dimethylpropyleneurea (DMPU) has been developed, affording a robust, dendrite‐free Zn anode with over 5000 h of cycle stability and a high average CE of 98.49%. Zn anode in DMPU‐electrolyte significantly outperforms aqueous electrolyte with 67 times longer cycle life, demonstrating excellent anode stability. Moreover, ultra‐stable Zn anode in DMPU‐electrolyte cycled for over 10 000 cycles at 1.0 mA cm−2 showcases excellent reversibility. The Dimethylpropyleneurea‐triflate anion generated solid electrolyte interphase enables homogeneous and rapid Zn2+‐diffusion at the electrode interface, leading to a structured hexagonal Zn deposit. Furthermore, as electrolyte additive, DMPU significantly stabilizes Zn anode at severe conditions (5.0 and 10.0 mA cm−2) along with remarkable enhancement in CE (99.12%). This study offers valuable insights into the development of hybrid and organic electrolytes to advance Zn battery technology. [ABSTRACT FROM AUTHOR]

Zn‐I2 batteries suffer from uncontrollable shuttle effects of polyiodine ions (I3− and I5−) at the cathode/electrolyte interface and side reactions induced by reactive H2O at the anode/electrolyte interface. In this study, a hydrated eutectic electrolyte is designed that synergizes the eutectic network and functional interfacial adsorbed layer to develop high‐performance Zn‐I2 batteries. The eutectic network can restrain active H2O molecules in the electrolyte to inhibit the side reaction at the anode/electrolyte interface and shuttle effect at the cathode/electrolyte interface. Additionally, the functional interfacial adsorbed layer guides the nucleation behavior of Zn2+ to inhibit the growth of dendrites and also separates the zinc anode from direct contact with active H2O molecules and polyiodine ions to inhibit corrosion. Theoretical calculation, in situ Ultraviolet–visible spectroscopy (UV‐vis) and Raman characterizations, and visualization experiments demonstrate that the hydrated eutectic electrolyte effectively inhibits the shuttling effect and improves the reversibility of zinc deposition/stripping behavior. Consequently, the Zn‐I2 battery can maintain a capacity of 133 mAh g−1 after 5000 cycles at 5 C. This highly efficient synergistic strategy offers a practical approach to the development of advanced Zn‐I2 batteries. [ABSTRACT FROM AUTHOR]

A fluorinated quasi-solid electrolyte (QSE) with a high conductivity of 2.3 mS cm−1 is meticulously designed for Li metal batteries. It facilitates the formation of a LiF-rich solid electrolyte interface that effectively enhances the reversibility of Li anodes. The assembled Li‖QSE‖LiFePO4 batteries exhibit 92.3% capacity retention after 1500 cycles and an impressive capacity of up to 45 mA h g−1 at 20C. [ABSTRACT FROM AUTHOR]

The instability of the solid electrolyte interface (SEI) is a critical challenge for the zinc metal anodes, leading to an erratic electrode/electrolyte interface and hydrogen evolution reaction (HER), ultimately resulting in anode failure. This study uncovers that the fluorine species dissolution is the root cause of SEI instability. To effectively suppress the F− dissolution, an introduction of a low‐polarity molecule, 1,4‐thioxane (TX), is proposed, which reinforces the stability of the fluorine‐rich SEI. Moreover, the TX molecule has a strong affinity for coordinating with Zn2+ and adsorbing at the electrode/electrolyte interface, thereby diminishing the activity of local water and consequently impeding SEI dissolution. The robust fluorine‐rich SEI layer promotes the high durability of the zinc anode in repeated plating/stripping cycles, while concurrently suppressing HER and enhancing Coulombic efficiency. Notably, the symmetric cell with TX demonstrates exceptional electrochemical performance, sustaining over 500 hours at 20 mA cm−2 with 10 mAh cm−2. Furthermore, the Zn||KVOH full cell exhibits excellent capacity retention, averaging 6.8 mAh cm−2 with 98 % retention after 400 cycles, even at high loading with a lean electrolyte. This work offers a novel perspective on SEI dissolution as a key factor in anode failure, providing valuable insights for the electrolyte design in energy storage devices. [ABSTRACT FROM AUTHOR]

The coupling of high-capacity cathodes and lithium metal anodes promises to be the next generation of high-energy-density batteries. However, the fast-structural degradations of the cathode and anode challenge their practical application. Herein, we synthesize an electrolyte additive, tris(2,2,3,3,3-pentafluoropropyl) borane (TPFPB), for ultra-stable lithium (Li) metal||Ni-rich layered oxide batteries. It can be preferentially adsorbed on the cathode surface to form a stable (B and F)-rich cathode electrolyte interface film, which greatly suppresses the electrolyte-cathode side reactions and improves the stability of the cathode. In addition, the electrophilicity of B atoms in TPFPB enhances the solubility of LiNO3 by 30 times in ester electrolyte to significantly improve the stability of the Li metal anode. Thus, the Li||Ni-rich layered oxide full batteries using TPFPB show high stability and an ultralong cycle life (up to 1500 cycles), which also present excellent performance even under high voltage (4.8 V), high areal mass loading (30 mg cm−2) and wide temperature range (−30∼60°C). The Li||LiNi0.9Co0.05Mn0.05O2 (NCM90) pouch cell using TPFPB with a capacity of 3.1 Ah reaches a high energy density of 420 Wh kg−1 at 0.1 C and presents outstanding cycling performance. [ABSTRACT FROM AUTHOR]

Metal anodes (e.g., Li and Zn) are promising candidates for high-energy and high-power rechargeable batteries. However, the commercialization of metal anodes is hampered by irregular dendrite growth, which severely deteriorates the safety and cyclability of metal anodes. Optimizing the electrolyte by nanostructured additives to regulate the metal deposition shows great potential since the electrochemically nonreactive feature endows the regulation function with good sustainability. In this manuscript, the fundamental dendrite formation models and key parameters for stabilizing metal anode are first discussed. The progress and functional mechanism of nanostructured additives for regulating the metal deposition are summarized in terms of regulatory model, i.e., deposition-, adsorption- and dispersion-type. Finally, we also provide a detailed concluding outlook, pointing out the future trend of selecting new nanostructured additive candidates and elucidating synergistic effects and underlying mechanisms with the key attention being given to the assessments of practicality. [ABSTRACT FROM AUTHOR]

The formation process of lithium‐ion batteries commonly uses low current densities, which is time‐consuming and costly. Experimental studies have already shown that slow formation may neither be necessary nor beneficial for cell lifetime and performance. This work combines an experimental formation variation with physicochemical cell and solid electrolyte interphase (SEI) modeling to reveal formation‐induced changes within the cells. Formation at C/2 without full discharge compared to a standard C/10 formation at 20 °C notably improves the discharge and charge capacities at 2C by up to 41 % and 63 %, respectively, while reducing the formation time by over 80 %. Model‐based cell diagnostics reveal that these performance gains are driven by improved transport in the anode electrolyte phase, which is affected by SEI formation, and by enhanced transport on the cathode side. Hence, the focus on the dense SEI layer is insufficient for a comprehensive understanding and, ultimately, optimization of cell formation. All formation procedures were also tested at temperatures of 35 °C and 50 °C. Despite often surpassing the 2C discharge capacity of the standard formation at 20 °C, these cells showed comparable or lower 2C charge capacities. This suggests a pivotal role of local temperature in the formation of large‐format cells. [ABSTRACT FROM AUTHOR]

Hard carbon (HC) is the most promising anode material for sodium‐ion batteries (SIBs). The main obstacle to HC's application is its incompatibility with the phosphate flame‐retardant additive, a common SIB additive. This incompatibility arises from the unstable solid electrolyte interphase (SEI) caused by phosphate molecule decomposition. For the first time, in this work, a new type of highly adaptive flame‐retardant electrolyte is proposed. The electrolyte ensures the stability of the electrode/electrolyte interface by the introduction of pioneering long‐chain nitrile as the SEI‐forming additive and solvated structural regulator. Long‐chain nitriles decompose before phosphate and form a stable SEI containing N element, which prevents the phosphate from inserting into the HC's layers and reduces its sodium‐storage capacity. As a proof of concept, the HC anode demonstrates a higher initial Coulombic efficiency of 80.78% in the as‐designed highly adaptive flame‐retardant electrolyte, which is about 1.8 times than that before regulation. It can cycle stably for 1250 cycles at 3 C with a capacity retention of 60%. Moreover, the electrolyte has good flame retardancy and can extinguish naturally within 1 s. In this work, an innovative method is provided for developing high‐safety SIBs based on HC anodes. [ABSTRACT FROM AUTHOR]

Lithium-ion batteries (LIBs) has extensively utilized in electric vehicles and portable electronics due to their high energy density and prolonged lifespan. However, the current commercial LIBs are plagued by relatively low energy density. High-entropy materials with multiple components have emerged as an efficient strategic approach for developing novel materials that effectively improve the overall performance of LIBs. This article provides a comprehensive review the recent advancements in rational design of innovative high-entropy materials for LIBs, as well as the exceptional lithium ion storage mechanism for high-entropy electrodes and considerable ionic conductivity for high-entropy electrolytes. This review also analyses the prominent effects of individual components on the high-entropy materials' exceptional capacity, considerable structural stability, rapid lithium ion diffusion, and excellent ionic conductivity. Furthermore, this review presents the synthesis methods and their influence on the morphology and properties of high-entropy materials. Ultimately, the remaining challenges and future research directions are outlined, aimed at developing more effective high-entropy materials and improving the overall electrochemical performance of LIBs. [ABSTRACT FROM AUTHOR]

An intermolecular hydrogen bond between 2,5-dihydroxyterephthalic acid and the anions in the Li+ solvation shell is constructed to promote the formation of a LiF-rich SEI on a metallic Li electrode. Li metal batteries with improved cyclability (140 cycles under an N/P ratio of 4.9) and high capacity retention (90%) are eventually obtained. [ABSTRACT FROM AUTHOR]

Building a lithium–sulfur (Li–S) battery with lean electrolytes is essential to far exceed the energy density of today's Li‐ion. However, earlier electrolyte depletion triggered by Li‐metal anodes (LMAs) causes sluggish Li–S redox kinetics and poor S utilization, resulting in a short cycle lifespan. To retard the electrolyte loss effectively, sustainable protection of LMAs is necessary against the dynamic interfacial evolution between LMA and protective layers (PLs). This study elucidates two critical parameters in securing the interfacial adaptivity of PLs upon local Li pitting: surface free energy (SFE) and Young's modulus through solid‐mechanic simulations and experiments using three different PL models. To alleviate the PL delamination at the early stage, a dual‐layer structured, adaptive protective layer (APL) is introduced to adapt the Li pitting‐driven structural evolution of the PL|LMA interfaces. The APL consists of a high‐ SFE polymer as an inner layer, reducing the interfacial energy in contact with LMA surface, and a highly stretchable polymer for outer shield, serving as a physical barrier for the electrolyte and Li polysulfides. APL‐coated LMA demonstrates stable cycling of Li–S cells, achieving a twofold extension of cycle‐life compared to unprotected LMA, even superior to other single‐layer PLs. [ABSTRACT FROM AUTHOR]

Zinc ion batteries (ZIBs) have emerged as promising candidates for renewable energy storage owing to their affordability, safety, and sustainability. However, issues with Zn metal anodes, such as dendrite growth, hydrogen evolution reaction (HER), and corrosion, significantly hinder the practical application of ZIBs. To address these issues, organic solid electrolyte interface (SEI) layers have gained traction in the ZIB community as they can, for instance, help achieve uniform Zn plating/stripping and suppress side reactions. This article summarizes recent advances in organic artificial SEI layers for ZIB anodes, including their fabrication methods, electrochemical performance, and degradation suppression mechanisms. [ABSTRACT FROM AUTHOR]

The silicon (Si) anode is prone to forming a high electric field gradient and concentration gradient on the electrode surface under high‐rate conditions, which may destroy the surface structure and decrease cycling stability. In this study, a ferroelectric (BaTiO3) interlayer and field polarization treatment are introduced to set up a built‐in field, which optimizes the transport mechanisms of Li+ in solid and liquid phases and thus enhances the rate performance and cycling stability of Si anodes. Also, a fast discharging and slow charging phenomenon is observed in a half‐cell with a high reversible capacity of 1500.8 mAh g−1 when controlling the polarization direction of the interlayer, which means a fast charging and slow discharging property in a full battery and thus is valuable for potential applications in commercial batteries. Simulation results demonstrated that the built‐in field plays a key role in regulating the Li+ concentration distribution in the electrolyte and the Li+ diffusion behavior inside particles, leading to more uniform Li+ diffusion from local high‐concentration sites to surrounding regions. The assembled lithium‐ion battery with a BaTiO3 interlayer exhibited superior electrochemical performance and long‐term cycling life (915.6 mAh g−1 after 300 cycles at a high current density of 4.2 A g−1). The significance of this research lies in exploring a new approach to improve the performance of lithium‐ion batteries and providing new ideas and pathways for addressing the challenges faced by Si‐based anodes. [ABSTRACT FROM AUTHOR]

Magnesium metal batteries (MMBs) currently face challenges suffering from severe Mg metal passivation and extremely high overpotential in conventional electrolytes. Herein, a strategy of using a low‐cost deep eutectic solution (DES) is proposed to modify Mg anode with the monolithic and compact coating of a MgCl2‐Al‐MgCl2 sandwich structure, enabling the stable and reversible Mg plating–stripping behavior. An organic/nanocrystal hybrid interphase is in‐situ built through a facile Mg‐Al displacement reaction between aluminum‐chloro clusters and Mg in AlCl3/Et3NHCl solution, and it can effectively minimize the adverse interfacial passivation reaction and surface diffusion barrier, affording the high ion‐conduction and electronic insulation. This DES‐assisted method guarantees a highly reversible cycling of Mg metal anode (over 5000 h at 0.1 mA cm−2 and 400 h at 2.0 mAh cm−2) in Mg(TFSI)2/DME electrolyte with the improved interfacial kinetics and low overpotential. Even at a much higher current density of 1 mA cm−2, the overpotential only undergoes a slight increase from 0.2 V (at 0.1 mA cm−2) to 0.23 V. The corresponding full cells with CuS and phenanthraquinone cathodes deliver satisfactory cyclic performance. The DES modification strategy provides a new solution to the design of robust and conductive solid electrolyte interphase for achieving high‐voltage and durable MMBs. [ABSTRACT FROM AUTHOR]

Ammonia has garnered recognition as a zero-carbon fuel due to its high-density hydrogen storage capacity and its convenience for storage and transportation. To address the challenges associated with the direct usage of ammonia, the development of NH3-to-H2 conversion technologies has emerged as a promising and effective approach. Herein, we present for the first time that crystallized Sm2O3−x electrodes demonstrate high and stable electrocatalytic activities, including N2 evolution rate and Faradaic efficiency, for ammonia electrolysis in a non-aqueous electrolyte. It was observed that Sm2+ ions in samarium oxide play an indispensable role in the ammonia electrooxidation reaction on the anodes. Furthermore, the mechanism of ammonia electrooxidation has also been elucidated, laying the foundation for a better understanding of the relationship between local structure and electrochemical properties in order to facilitate research on Pt-free electrocatalysts for the electrolysis of ammonia into H2. [ABSTRACT FROM AUTHOR]

Carbon‐based materials have been found to accelerate the sluggish kinetic reaction and are largely subject to the overall Zn‐air batteries (ZABs) property, while their full catalytic mechanism is still not excavated because of the indistinct internal structure and immature in‐situ technology. Up to now, systematic methods have been utilized to study and design promising high‐performance carbon‐based catalysts. To resolve the real active units and catalytic mechanism, developing molecular catalyst is a significant strategy. Herein, the review will initiate to briefly introduce the working principle and composition of ZABs. An important statement is correspondingly provided about the typical structure and catalytic mechanisms for the air cathode material. It also presents the tremendous endeavors on the catalytic performance and stability of carbon‐based material. Furthermore, combined with theoretical calculation, the self‐defined active sites are analyzed to understand the catalytic character, where the molecular catalyst is subsequently summarized and discussed through highlighting the unambiguous and controllable structure, in the hope of surfacing the optimum catalyst. Building on the fundamental understanding of carbon‐based and molecular catalysts, this review is expected to provide guidance and direction toward designing future mechanistic studies and ORR electrocatalysts. [ABSTRACT FROM AUTHOR]