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The sufficient and reversible active lithium is the cornerstone for the operation of high‐energy lithium‐ion batteries. However, active lithium is inevitably depleted due to the formation of a solid electrolyte and the presence of irreversible side reactions. The shortage of lithium in optimally designed batteries not only leads to a depreciation of energy density but also deteriorates the electrode structure resulting in degradation of cycle life. Inspiringly, prelithiation technology that additionally compensates for lithium has been proposed and is playing an increasingly significant role in enhancing battery energy density and prolonging cycle life. Herein, guided by the factors that initiate lithium loss, the action mechanism and the effectiveness of prelithiation are scrutinized. Moreover, the emerging advanced prelithiation technologies based on anode/cathode materials, the key barriers, and the applicability at scale are systematically summarized and compared. Integrating the challenges and development trends aspires to provide a comprehensive prelithiated hybrid lithium replenishment and storage technology as a reference in the scale‐up of prelithiation technologies. [ABSTRACT FROM AUTHOR]

Solid/solid interface is the major challenge for high‐performance solid‐state batteries. Solid electrolytes (SEs) play a crucial role in the fabrication of effective interfaces in solid‐state batteries. Herein, the electrolyte distribution with varied particle sizes is tuned to construct solid‐state batteries with excellent performance at different operating temperatures. Solid‐state batteries with the configuration S/L (small‐sized SE in composite cathode and large‐sized SE in electrolyte layer) show the best performance at room temperature (168 mA h g−1 at 0.2 C, retention of 99%, 100 cycles) and −20 °C (89 mA h g−1 at 0.05 C), while the configuration S/S displays better performance at elevated temperature. The superior performance of S/L battery is associated with faster lithium‐ion dynamics due to the better solid/solid interface between active materials and electrolytes. Moreover, the inferior performance at 60 °C is caused by the formation of voids and cracks in the electrolyte layer during cycling. In contrast, the S/S battery delivers superior performance at elevated operating temperature because of the integrated structure. This work confirms that tailoring electrolyte size has significant effect on fabricating all‐climate solid‐state batteries. [ABSTRACT FROM AUTHOR]

The advancements of lithium‐ion batteries indubitably call for advanced electrolytes with superior environmental adaptability and long‐term stability. Propylene carbonate (PC) proves to be a competitive solvent with the high permittivity and wide‐liquid range, while the application is intrinsically hindered by the poor graphite compatibility and high viscosity. Here, a PC‐based electrolyte with wide‐temperature range is developed by tuning the strength and topology of the Li+‐PC interactions via non‐solvating interactions without altering the solvation structure. Thus, the problem of graphite exfoliation caused by Li+‐PC co‐intercalation can be successfully mitigated. Consequently, such electrolyte shows compatibility with both graphite and high‐nickel cathode, exhibiting an expanded liquid range from −90 to 90 °C. This work, breaking from the traditional EC‐based formula, provides a new strategy for designing PC‐enabled electrolyte featuring high performance, wide‐temperature compatibility, and sustainability [ABSTRACT FROM AUTHOR]

Sodium storage in both solid-liquid and solid-solid interfaces is expected to extend the horizon of sodium-ion batteries, leading to a new strategy for developing high-performance energy-storage materials. Here, a novel composite aerogel with porous Li4Ti5O12 (PLTO) nanofibers confined in a highly conductive 3D-interconnected graphene framework (G-PLTO) is designed and fabricated for Na storage. A high capacity of 195 mA h g-1 at 0.2 C and super-long cycle life up to 12 000 cycles are attained. Electrochemical analysis shows that the intercalation-based and interfacial Na storage behaviors take effect simultaneously in the G-PLTO composite aerogel. An integrated Na storage mechanism is proposed. This study ascribes the excellent performance to the unique structure, which not only offers short pathways for Na+ diffusion and conductive networks for electron transport, but also guarantees plenty of PLTO-electrolyte and PLTO-graphene interfacial sites for Na+ adsorption. [ABSTRACT FROM AUTHOR]

Chlorine-rich argyrodite Li 5.5 PS 4.5 Cl 1.5 with low-cost and high ionic conductivity displays great potential as a solid electrolyte for solid-state battery. However, poor compatibility with bare high-voltage cathode limits its applications. Here, the Li 2 ZrO 3 coating and Li 3 InCl 6 isolating layer strategy are employed to mitigate the interfacial instability between Li 5.5 PS 4.5 Cl 1.5 electrolytes and LiNi 0.7 Co 0.1 Mn 0.2 O 2 materials, respectively. A diversified combination of two strategies is applied to construct all-solid-state batteries with a long lifespan and high energy density. Electrochemical performance results indicate that introducing Li 3 InCl 6 electrolyte in the cathode mixture yields high discharge capacities at beginning and then suffers rapid capacity degradation during extended cycling. In contrast, the assembled Li 2 ZrO 3 @LiNi 0.7 Co 0.1 Mn 0.2 O 2 /Li 5.5 PS 4.5 Cl 1.5 /Li–In battery delivers slightly lower capacities and superior capacity retention. Multiple characterization methods are employed to unravel the mechanism behind battery performance differences. The poor cycle performance of Li 3 InCl 6 -involved solid-state battery configurations is partially associated with the decomposition of Li 3 InCl 6 in the cathode mixture. The Li 2 ZrO 3 coating layer mitigates the side reaction between LiNi 0.7 Co 0.1 Mn 0.2 O 2 and Li 3 InCl 6 , resulting in enhanced capacities and improved cyclability. Furthermore, the interfacial instability between Li 3 InCl 6 and Li 5.5 PS 4.5 Cl 1.5 electrolytes leads to the poor cycling performance of batteries containing the Li 3 InCl 6 /Li 5.5 PS 4.5 Cl 1.5 bilayer structure. This work offers a comprehensive guide for designing high-performances all-solid-state lithium batteries. • Li 2 ZrO 3 coating layer is introduced to alleviate instability of cathode interface. • Li 3 InCl 6 separator layer is utilized to isolate cathode and Li 5.5 PS 4.5 Cl 1.5. • The advantages of Li 2 ZrO 3 and Li 3 InCl 6 protecting strategies have been studied. • Two protection strategies are combined to improve battery performance. • The instability between Li 3 InCl 6 and Li 5.5 PS 4.5 Cl 1.5 affects battery performance. [ABSTRACT FROM AUTHOR]

The characteristics of thermal runaway in batteries exhibit significant differences depending on their states of charge (SOCs), posing considerable challenges in accurate and timely warning for thermal runaway accidents. This paper conducts an experimental investigation into the external expansion force, voltage, and temperature behaviours of batteries under different SOCs under thermal abuse scenarios. The expansion force signal was found first to exhibit abnormal characteristics (with an indicator value of 5 N/s), offering an earlier warning signal >642 s prior to thermal runaway, when the battery back temperature is merely approximately 318.15 K. To analyse the main causes of abnormal expansion, ultrasonic nondestructive tests were performed and suggested that a higher SOC intensify the side reactions and cause gas generation inside batteries. Notably, compared to normal-charged batteries (0% ≤ SOC ≤ 100%), over-charged batteries (SOC > 100%) are more sensitive to expansion force than normal-charged batteries. Furthermore, compared with voltage and temperature signals, the early warning time of the expansion force rises with the increase in the SOC of an overcharged battery, in contrast to normal-charged batteries. Finally, a novel hazard classification safety warning strategy for battery failure is effectively proposed. These novel findings hold substantial practical implications for creating more accurate early warning systems for battery thermal runaway, enhancing the safe and reliable operation of battery systems. • Effect of SOC on multidimensional signal evolution is comprehensively revealed. • Expansion force can serve as an early warning signal of battery failure. • Expansion force evolution of batteries with different states of charge is revealed. • Nondestructive tests are conducted to analyse the main causes of abnormal expansion. • A novel warning strategy with hazard classification for battery failure is proposed. [ABSTRACT FROM AUTHOR]

A type of sulfur-doped carbon (SC) was synthetized by pyrolyzing the freeze-dried gel of agarose and sulfur powder as anode material for sodium ion batteries (SIBs), and its sodium-storage mechanism was assayed by structure and electrochemical characterizations. The most sulfur atoms were doped between (002) interlayers of carbon matrix probably because of the perfect structure of agarose sourced carbon, as the (002) interplanar spacing has increased from 0.323 nm to 0.393 nm, which benefits the faster diffusion of Na+-ions inside carbon lattice. The optimized SC material exhibited an initial discharge capacity more than 420 mAh g−1 at 100 mA g−1. When cycled at various current densities from 0.1, 0.2, 0.3, 0.5, 1.0, 2.0–3.0 A g−1, the reversible specific capacity changed from 331, 293, 273, 245, 207, 152 to 110 mAh g−1 respectively, which displayed high rate performance. When cycled to the 1000th time at 500 mA g−1 and 1000 mA g−1, the capacity retention was still kept at 91.6% and 91.8% based on the stable reversible capacity during the charge/discharge processes, respectively. The advantage of stable cycling performance makes the low cost S-doped carbon derived from natural seaweed be a promising candidate as anode material for rechargeable SIB. A type of sulfur-doped carbon (SC) has been synthesized by pyrolyzing the freeze-dried gel of agarose and sulfur powder. After doped with S, the SC is endowed with large BET surface area, small pore size, large pore volumes and enlarged (002) interplanar spacing, which make the SC with excellent rate capability and cyclability. The study of sodium-storage mechanism shows that the released capacity is mainly contributed by the Na+-insertion/extraction process and is largely dependent on the low operation voltage. Image 1 • Sulfur-doped agarose-sourced carbon has been prepared as anode material for SIBs. • The sulfur atoms are mainly doped within the (002) interlayers of carbon matrix. • Sulfur-doped carbon exhibits excellent capacity and long-term cyclic stability. • The sodium-storage mechanism has been studied by various characterizations. [ABSTRACT FROM AUTHOR]

A novel bottom-up synthesis route based on hydrogen bonds has been developed to prepare NaVPO 4 F/C (NVPF/C) composite as the cathode material for sodium ion batteries (SIBs). NVPF grains are anchored through effective hydrogen bonds between the fluorine ions and hydrogen atoms inside the sol-gel template, which endows the final product an interconnected and porous three-dimensional (3D) coral-like structure composed by oriented packing of uniform nanoparticles (15–20 nm). The as-prepared NVPF/C exhibits excellent rate capability and extraordinary cyclic stability. The corresponding discharge capacities at 1, 2, 5, 10, 20, 30 and 50 C range from 106, 102, 99, 98, 93, 90 to 88 mAh g −1 respectively. At 5 C, it releases an initial capacity of 100 mAh g −1 , and still maintains 70 mAh g −1 after 2500 cycles, corresponding to a very low capacity fading of 0.012% per cycle. The uniform nanometers sized (15–20 nm) fundamental particles and nanopores (3–8 nm) of as-prepared NVPF/C endow the efficient transfer of both electrons and sodium ions. This work implies that the novel 3D coral-like structured NVPF/C is a very promising high-performance cathode for SIBs, and the new synthetic method can also be applied to prepare other fluorine contained polyanion-type materials. [ABSTRACT FROM AUTHOR]

Liquid metal battery (LMB), with three-liquid-layer structure and high operating temperature (300–700 °C), is a newly emerging technology for large scale energy storage applications. A thermal management system is critical to achieve satisfied LMB performance and extend the life of batteries. In this work, an improved coupling model composing of a 3D heat-transfer model and a 1D electrochemical model is developed for the thermal analysis of a Li||Sb–Sn LMBs module (5.5 kWh). Key results including transient values, the contribution ratio of heat sources, temperature homogeneity and distribution, as well as the energy efficiency of the battery module, are presented. Based on the coupling model, the changeable-power-heating mode, sand filling material and vacuum insulation are further proposed to achieve the high energy efficiency and optimal performance of the LMBs module. Moreover, the LMBs module can achieve “self-heating” when operated at 0.2 C charge/discharge, under the vacuum insulation (0.01 W m −1 K −1 thermal conductivity, 100 mm thickness), requiring no external heating to keep the batteries at operating temperature. [ABSTRACT FROM AUTHOR]

Lithium argyrodites electrolyte with high ionic conductivity and relatively lower cost show great potential as candidates for solid-state batteries. Further improvement of their conductivities can accelerate their applications. One of the means to significantly promote the conductivity of Li-ion is dual doping. Herein, Ag/Br dual-doping strategy is applied on Li 6 PS 5 Br (2.76 mS cm−1) to boast its conductivity to 6.15 mS cm−1 for Li 5.55 Ag 0.05 PS 4.6 Br 1.4. The structural variations and chemical/electrochemical stability of the obtained electrolyte are carefully investigated. Li 3 InCl 6 electrolyte is introduced in the new battery configuration to mitigate the interfacial instability with LiNi 0.6 Mn 0.2 Co 0.2 O 2 active material enabling good electrochemical performances. The assembled battery delivers a discharge capacity of 160.8 mAh g−1 for the 1st cycle and maintains 85.9% of the initial value after 50 cycles at 0.5C. This modification strategy was proved effective for increasing the conductivity of sulfide electrolytes in this work. AgBr dual-doping on Li6PS5Br (2.76 mS cm−1) yields boasting Li-ion conductivity of up to 6.15 mS cm−1 for Li5.55Ag0.05PS4.6Br1.4 due to the enlargement of diffusion channels for ions and the increase of anion disorders, resulting in excellent electrochemical performances for the corresponding solid-state batteries. [Display omitted] [ABSTRACT FROM AUTHOR]

Carbon-coated Sb 2 Se 3 composite (Sb 2 Se 3 @C) is prepared via high energy mechanical milling accompanied with planetary milling method and investigated as a novel anode for Na-ion batteries for the first time. It exhibits a high Na-storage capacity of 650 mAh g − 1 at 0.1 A g − 1 , and maintains a reversible capacity of 624 mAh g − 1 with negligible capacity fading at 0.2 A g − 1 after 100 cycles, demonstrating a stable cycling performance. In addition, the ex situ XRD analysis reveals that the Na-storage mechanism of the Sb 2 Se 3 @C anode includes conversion reaction and alloying reaction. [ABSTRACT FROM AUTHOR]

• A facile process is developed to prepare argyrodite electrolytes in large quantities. • The electrolyte Li 5.5 PS 4.5 Cl 1.5 achieves a high ionic conductivity of 9.03 mS/cm. • The SSBs deliver superior rate capability and cycling performance at RT and −20 ℃. Solid-state batteries (SSBs) employing sulfide electrolytes (SEs) are considered with poor rate capability and short cycling span life, especially towards the pristine nickel-rich cathode. The high cost, low conductivity, and compatibility are regarded as the major obstacles. In this work, chlorine-rich Li 5.5 PS 4.5 Cl 1.5 electrolyte with high conductivity (9.03 mS/cm) is synthesized via an easy scale-up route. The role of carbon in the cathode mixture is unraveled at room temperature (RT) and low temperature. SSBs using designed cathode without carbon deliver capacity retention of 82.4% after 10,000 cycles under 10C at room temperature and 97.0% after 200 cycles under 0.2C at −20 ℃. This research shows the potential of utilizing SEs to manufacture SSBs with high rates and long cyclability under different temperatures. [ABSTRACT FROM AUTHOR]