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A new avenue by transforming the conventional electrochemical domain into an electro‐chemo‐mechanical domain is proposed to achieve less hysteretic fast‐charging based on the three pictures: i) electro‐chemo‐mechanics, ii) phase transition kinetics, and iii) ionic kinetics. Each concept is demonstrated leading to the electrochemical improvement using data‐driven computation and experimental analyses, and its novel framework is generalized based on alkali‐ion chalcogenide models. The mechanical strain lowers and delays the electrochemical yield point, which gives rise to extending the elastic region and enhancing the phase and ionic kinetics. This is experimentally verified with less hysteresis upon (dis)charging for all models. Implementing the electro‐chemo‐mechanical domain is central in alkali‐ion chalcogenide batteries and broadens its application in other rechargeable batteries, ultimately playing a critical role in providing practical fast‐charging solutions. [ABSTRACT FROM AUTHOR]

The application of sodium‐ion batteries (SIBs) within grid‐scale energy storage systems (ESSs) critically hinges upon fast charging technology. However, challenges arise particularly with anodes such as hard carbon (HC), which exhibits a low working plateau (less than 0.1 V vs Na/Na+) and is susceptible to sodium dendrite issues under high current densities. In this study, a cost‐effective SIB system comprising Na2.4Fe1.8(SO4)3 (NFS) cathode, NaTi2(PO4)3 (NTP) anode, and ester‐based electrolyte is assembled to solve the fast‐charging obstacle. Benefiting from the fast sodium‐ion diffusion kinetics and relatively high voltage platform of NTP anode, this full cell can work for 10 000 cycles at 10 C rate with a notable capacity retention of 70.7%. Moreover, this investigation reveals that the full cell can operate safely between ‐50 to 90 °C even with an ester‐based electrolyte, thereby showcasing broad application prospects. This work provides a valuable guidance for designing fast charging and wide temperature SIBs. [ABSTRACT FROM AUTHOR]

Lithium‐ion batteries are currently the most widely used electrochemical energy storage devices. However, the most used graphite anode faces severe lithium plating issues when charging at low temperatures or high rates, leading to battery's capacity decay and even safety concerns. Therefore, visually and quantitatively detecting lithium plating is extremely important to analyze battery's performances. Here a convenient, rapid‐response, visual, and semi‐quantitative technique, namely fluorescence probe, is put forward to visually and quantitatively detect lithium plating on graphite anodes. A commercially available aggregation‐induced emission (AIE) molecule (4′‐hydroxychalcone) is introduced as a probe. The hydroxyl group of 4′‐hydroxychalcone can rapidly and sensitively react with plated lithium, instantaneously emerging an intensive yellow fluorescence within seconds; while 4′‐hydroxychalcone undergoes fluorescence quenching when directly contacting with graphite. Based on this, not only the uneven distribution of plated lithium on graphite anodes can be simply and clearly visualized and detected after being charged at low temperatures or high rates, but also the semi‐quantitative relationship between fluorescence intensity and the amount of plated lithium can be well established. Therefore, this work puts forward a practical solution for analyzing lithium plating on graphite anodes, offering a practical approach for failure analysis of lithium‐ion batteries used in various scenarios. [ABSTRACT FROM AUTHOR]

Fast‐charging lithium‐ion batteries are pivotal in overcoming the limitations of energy storage devices, particularly their energy density. There is a burgeoning interest in boosting energy storage performance through enhanced fast‐charging capabilities. However, the challenge lies in developing batteries that combine high rates, long cycle life, high capacity, and safety. This review emphasizes the importance of fundamentals and design principles of fast charging, identifying the transport of ion/electron within the electrodes/electrolytes' bulk phase and at phase boundaries as the crucial rate‐limiting steps for fast charging. Such as ion transport tunnel regulation, interfacial modification, defect engineering and multiphase systems, various optimization strategies improve the stable and exceptional electrochemical reaction kinetics for electrodes. Constructing stable solid electrolyte interfaces and adjusting solvation structures further enhance the Li+ diffusion kinetics of electrolytes. The review critically assesses the impacts and limitations of these strategies, suggesting future research directions and insights for advancing fast‐charging lithium‐ion batteries. It is anticipated that this review will inspire and guide the systematic evolution of fast‐charging technologies. [ABSTRACT FROM AUTHOR]

The development of fast‐charging lithium‐ion batteries with high energy density is hindered by the sluggish Li+ transport and substantial polarization within graphite electrodes. Herein, this study proposes that the integrated design of liquid electrolyte and solid electrolyte, a dual‐phase electrolyte (DP‐electrolyte), can facilitate Li+ transport within a thick electrode. A 3D Li3PS4 (LPS) network is constructed within the graphite electrode to form the LPS/graphite electrode. This is achieved through the in situ conversion of the P4S16 into the LPS, a process introduced during the slurry processing. Both experimental findings and simulation outcomes indicate that this design mitigates the concentration polarization due to the improved Li+ transport capability with an overall high Li+ transference number within the electrode. With a high capacity of ≈3.1 mAh cm−2 attributed to the graphite electrode, the LiNi0.6Co0.2Mn0.2O2 (NCM622)||LPS/graphite cells demonstrate superior fast‐charging capability (4 C, 15 min, charging to ≈87.7%) and stable cycling performance (4 C, 700 cycles, ≈80% capacity retention). Furthermore, they exhibit commendable low‐temperature performance. The Ah‐level pouch cell achieves 87.5% recharge in 15 min with an energy density of ≈221.5 Wh kg−1. This work offers an alternative avenue for the advancement of fast‐charging lithium‐ion batteries with practical high energy density. [ABSTRACT FROM AUTHOR]

Silicon (Si) anodes hold great promise for enhancing the energy density of lithium‐ion batteries (LIBs). However, issues such as slow intrinsic kinetics and unstable interfaces caused by significant volume changes hinder the practical deployment of Si anodes. Fast charging is desired by Si‐related issues that worsen Li plating and dead Li, making it essential to overcome these for safe, reversible charging. Herein, a novel approach is proposed by combining structural design and solid electrolyte interface (SEI) modulation to enable efficient and safe fast charging of LIBs. 3D porous micro‐particles consisting of Si nanosheets coated with a pitch‐based carbon layer are successfully prepared. This design provides enhanced ion transport pathways while maintaining the material's intrinsic rate performance and tap density. Furthermore, the designed localized high‐concentration electrolyte (LHCE) exhibits a lower Li+ desolvation energy barrier and leads to the formation of a LiF‐rich SEI, mitigating the Li plating "tip effect" during fast charging, maintaining interface stability, and demonstrating high Coulombic efficiency. Overall, this study highlights the synergistic importance of structure design and SEI regulation in enhancing LIB anodes for fast charging, aiding in developing superior, safe energy storage. [ABSTRACT FROM AUTHOR]

Thick and dense graphite anodes used in lithium‐ion batteries (LIBs) suffer from sluggish reaction kinetics at the electrode level, causing Li metal plating on their surfaces and significant capacity decay at high charging currents. Thus, it is crucial to tailor electrodes based on a comprehensive understanding of the complex reaction kinetics to realize fast‐charging LIBs. A multi‐interface strategy is proposed for electrode tailoring using Al2O3 nanoparticles to enhance fast‐charging capability while suppressing Li metal plating. Molecular dynamics simulations suggest that the incorporated Al2O3 nanoparticles perturb the charge and molecule distributions in the boundary layer, forming an "interfacial highway" for facile Li+ transport at the Al2O3/electrolyte interface. This pushes Li+ deeper into the electrode and homogenizes the Li+ flux across the electrode's top surface. A full cell assembled with the Al2O3‐decorated graphite electrode (areal capacity of 4.4 mAh cm−2) exhibits excellent cyclability with a capacity retention of 83.4% over 500 cycles even at a 2C rate without any noticeable signal for undesirable Li plating. The role of interfacial highways predicted by theoretical computations is further validated using a pouch‐type full cell (500 mAh). These findings provide insights into the interfacial and microstructural design of high‐capacity graphite electrodes for fast‐charging, long‐cycling LIBs. [ABSTRACT FROM AUTHOR]

Inorganic solid electrolytes offer inherently unique transport, thermal, and mechanical attributes that can potentially address the fast‐charging barriers of safety, performance, and degradation exhibited by their liquid counterparts; however, to achieve reliable fast charging while retaining long cycle life remains a challenge for all‐solid‐state lithium batteries (ASSLBs), which is hindered by the electro‐chemo‐mechanical and transport issues at solid–solid interface. Herein, a high‐entropy strategy is reported to design ideal argyrodite electrolytes for fast‐charging ASSLBs with boosted transport kinetics and mitigated electrolyte‐electrode reactions via anionic site disordering. As proof of concept, multiple aliovalent cations (Si4+/Ge4+/Sn4+) and anions (Cl−) are introduced to Li6PS5Br (LPSBr) to prepare its high‐entropy counterpart, HE‐LPSBrCl. As the configuration entropy increases from 1.35 to 2.29 R, the disordering increases by 6.83‐fold and ionic conductivity increases by nearly one order of magnitude (7.96 mS cm−1 at 30 °C for HE‐LPSBrCl). The HE‐LPSBrCl full cells deliver a high capacity of 67.7 mA h g−1 at 10 C, 61.5 times higher than that of LPSBr counterparts, and retain 85.6% of the capacity (96.2 mA h g−1 at 5 C) after 1400 cycles. Unwanted mechanical penetration of Li and interfacial delamination and particle cracking of composite cathode at high rates are successfully suppressed. [ABSTRACT FROM AUTHOR]

The practical application of lithium (Li) metal anode (LMA) is still hindered by non‐uniformity of solid electrolyte interphase (SEI), formation of "dead" Li, and continuous consumption of electrolyte although LMA has an ultrahigh theoretical specific capacity and a very low electrochemical redox potential. Herein, a facile protection strategy is reported for LMA using a double layer (DL) coating that consists of a polyethylene oxide (PEO)‐based bottom layer that is highly stable with LMA and promotes uniform ion flux, and a cross‐linked polymer‐based top layer that prevents solvation of PEO layer in electrolytes. Li deposited on DL‐coated Li (DL@Li) exhibits a smoother surface and much larger size than that deposited on bare Li. The LiF/Li2O enriched SEI layer generated by the salt decomposition on top of DL@Li further suppresses the side reactions between Li and electrolyte. Driven by the abovementioned advantageous features, the DL@Li||LiNi0.6Mn0.2Co0.2O2 cells demonstrate capacity retention of 92.4% after 220 cycles at a current density of 2.1 mA cm–2 (C/2 rate) and stability at a high charging current density of 6.9 mA cm–2 (1.5 C rate). These results indicate that the DL protection is promising to overcome the rate limitation of LMAs and high energy‐density Li metal batteries. [ABSTRACT FROM AUTHOR]

Metastable orthorhombic niobium pentoxide (T‐Nb2O5) is a promising anode to fulfill the requirements for high‐rate Li‐ion batteries (LIBs). Stoichiometric T‐Nb2O5 is plagued by low electric conductivity and particle pulverization after repeated charge/discharge processes. In this work, oxygen vacancies are implanted into T‐Nb2O5 particles via acid immersion of Nb2O5·nH2O with the formation of Lewis acid sites. The multiple characterizations and simulations reveal the lengthening of NbO bonds, and the transformation from NbO7 pentagonal bipyramids and NbO6 tetragonal bipyramids in T‐Nb2O5−x. The enrichment of oxygen vacancies endows T‐Nb2O5−x with higher electric conductivity, better electrochemical kinetics, larger pseudocapacitive contribution. O‐doped graphitic C3N4 is creatively proposed as a trace oxygen pump to repair excessive oxygen vacancies, and it also serves as a sacrifice template for Nb2O5−x growth to construct a porous and monolithic electrode network. Defect‐modulated Nb2O5−x displays extraordinary cycling stability (164 mAh g−1 at 5 C after 1100 cycles), high capacity retention (104 mAh g−1) at an ultrahigh rate (25 C), and large areal capacity (0.74 mAh cm−2) under high mass loading (4 mg cm−2). The practical prospect is proved by Nb2O5−x/LiNi0.8Co0.1Mn0.1O2 full cells with high average platform (2.12 V) and high specific capacity (229 mAh g−1). The oxygen‐defect modulation strategy on oxide anodes provides an alternative solution to fast‐charging and durable LIBs. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (ZIBs) are a promising candidate for fast‐charging energy‐storage systems due to its attractive ionic conductivity of water‐based electrolyte, high theoretical energy density, and low cost. Current strategies toward high‐rate ZIBs mainly focus on the improvement of ionic or electron conductivity within cathodes. However, enhancing intrinsic electrochemical reaction kinetics of active materials to achieve fast Zn2+ storage has been greatly omitted. Herein, for the first time, stable radical intermediate generation is demonstrated in a typical organic electrode material (methylene blue [MB]), which effectively decreases the reaction energy barrier and enhances the intrinsic kinetics of MB cathode, enabling ultrafast Zn2+ storage. Meanwhile, anionic co‐intercalation essentially avoids MB molecules rearranging their configuration and sharing Zn2+ with adjacent functional groups, thus keeps the structure stable. As a result, Zn–MB batteries exhibit an excellent rate capability up to 500C and ultralong life of 20 000 cycles with a negligible 0.07% capacity decay per cycle at 100C, which is superior to that of most reported aqueous ZIBs batteries. This work provides a novel strategy of stable radical chemistry for ultrafast‐charging aqueous ZIBs, which can be introduced to other appropriate organic materials and multivalent ion battery systems. [ABSTRACT FROM AUTHOR]

A novel flexible hybrid battery–supercapacitor device is proposed consisting of high specific surface area electrodes paired with an electrolyte, which contains a redox species that can exist in more than two oxidation states. The two initially equal half‐cells of the device consist of a reduced graphene oxide hydrogel which encapsulates vanadium ions, synthesized with a single‐step method. During charge, the oxidation state of the vanadium ions changes, resulting in two half‐cells with different potentials which considerably increases the energy density. The achieved maximum capacity of more than 225 mAh g−1 is roughly eight times higher than that of comparable graphene hydrogel supercapacitors without vanadium content, but the potentiostatic charging time is only double. Operated as a supercapacitor, it retains 95% of the initial capacitance over 1000 cycles. As battery, the losses are more significant, retaining around 50% of the initial capacity. However, these losses during battery operation can be almost entirely restored by electric measures. The vanadium ion addition also improves the self‐discharge characteristics of the device. Moreover, the self‐discharge does not permanently damage the hybrid device since both half‐cells initially consist of the same vanadium graphene hydrogel and discharging resets it to initial conditions. [ABSTRACT FROM AUTHOR]

Rechargeable batteries with a Li metal anode and Ni‐rich Li[NixCoyMn1−x−y]O2 cathode (Li/Ni‐rich NCM battery) have been emerging as promising energy storage devices because of their high‐energy density. However, Li/Ni‐rich NCM batteries have been plagued by the issue of the thermodynamic instability of the Li metal anode and aggressive surface chemistry of the Ni‐rich cathode against electrolyte solution. In this study, a bi‐functional additive, adiponitrile (C6H8N2), is proposed which can effectively stabilize both the Li metal anode and Ni‐rich NCM cathode interfaces. In the Li/Ni‐rich NCM battery, the addition of 1 wt% adiponitrile in 0.8 m LiTFSI + 0.2 M LiDFOB + 0.05 M LiPF6 dissolved in EMC/FEC = 3:1 electrolyte helps to produce a conductive and robust Li anode/electrolyte interface, while strong coordination between Ni4+ on the delithiated Ni‐rich cathode and nitrile group in adiponitrile reduces parasitic reactions between the electrolyte and Ni‐rich cathode surface. Therefore, upon using 1 wt% adiponitrile, the Li/full concentration gradient Li[Ni0.73Co0.10Mn0.15Al0.02]O2 battery achieves an unprecedented cycle retention of 75% over 830 cycles under high‐capacity loading of 1.8 mAh cm−2 and fast charge–discharge time of 2 h. This work marks an important step in the development of high‐performance Li/Ni‐rich NCM batteries with efficient electrolyte additives. [ABSTRACT FROM AUTHOR]

Rechargeable lithium ion battery (LIB) has dominated the energy market from portable electronics to electric vehicles, but the fast‐charging remains challenging. The safety concerns of lithium deposition on graphite anode or the decreased energy density using Li4Ti5O12 (LTO) anode are incapable to satisfy applications. Herein, the sulfurized polyacrylonitrile (SPAN) is explored for the first time as a high capacity and safer anode in LIBs, in which the high voltage cathode of LiNi1/3Co1/3Mn1/3O2 (NCM‐H) is further introduced to configure a new SPAN|NCM‐H battery with great fast‐charging features. The LIB demonstrates a good stability with a high capacity retention of 89.7% after 100 cycles at a high voltage of 3.5 V (i.e., 4.6 V vs Li+/Li). Particularly, the excellent rate capability is confirmed and 78.7% of initial capacity can still be delivered at 4.0C. In addition, 97.6% of the battery capacity can be charged within 2.0C, which is much higher than 80% in current fast‐charging application standards. The feature of lithiation potential (>1.0 V vs Li+/Li) of SPAN avoids the lithium deposition and improves the safety, while the high capacity over 640 mAh g−1 promises 43.5% higher energy density than that of LTO‐based battery, enabling its great competitiveness to conventional LIBs. Sulfurized polyacrylonitrile (SPAN) is explored for the first time as a high capacity and safer anode in a lithium ion battery, in which the high voltage cathode of LiNi1/3Co1/3Mn1/3O2 (NCM‐H) is further introduced to configure a new SPAN|NCM‐H battery with great fast‐charging features. Excellent rate capability is confirmed and 97.6% of the battery capacity can be charged within 2.0C. [ABSTRACT FROM AUTHOR]