graphite-based anodes, active lithium from the lithium-containing oxide or phosphate cathode is consumed due to the side reactions during the formation of solid electrolyte interface (SEI) on the anode surface, accompanied by the decomposition of liquid electrolyte. This leads to Coulombic efficiency values lower than 100% in the very initial charge/discharge cycles (e.g., 90%-95% for the first cycle), which appreciably reduces the energy density of LIBs. [10][11][12][13] For the next-generation highenergy-density LIBs, high-capacity anodes (e.g., Si, Sn, and P with alloy reaction mechanism) undergo much more serious side reactions and show much more initial lithium loss (e.g., >15%) than the graphitebased anodes. Moreover, the side reactions of these high-capacity anodes continue to take place for several cycles, sometimes even tens of cycles, before the stabilization of Coulombic efficiency to over 99.9%, due to the large volume change of these materials (e.g., ≈420% for Si, ≈260% for Sn, and ≈300% for P) from lithium-free state to full lithiation state, which leads to large amount of accumulated lithium loss. [14,15] Consequently, the usable lithium-ion capacity and overall energy density of LIBs using these high-capacity anode materials would be significantly decreased.Prelithiation has been widely investigated as a promising strategy to resolve this lithium loss issue and increase the energy density of LIBs. With the specific purpose of compensating for the initial lithium loss in LIBs, prelithiation is conceptually independent from the pretreatment of battery materials or electrodes, and it can be simply regarded as providing additional active lithium using specific prelithiation reagents/ materials or processing to LIBs prior to battery cell cycling. To increase active lithium inside the entire LIBs, prelithiation can be performed on different battery components, cathodes, or anodes, and also at different levels, materials, or electrodes, depending on the prelithiation approaches. Till now, various prelithiation methods have been developed, including electrochemical prelithiation at the electrode level, [16][17][18][19] chemical prelithiation at the materials or electrode level, [20][21][22] prelithiation additives for cathodes and anodes, [8,[23][24][25][26][27] and direct contact/short circuit between a negative electrode and a lithium metal foil. [28][29][30][31] These prelithiation methods with various mechanisms show different prelithiation efficiency or capability in increasing the energy density of LIBs and other effects, and Lithium-ion batteries (LIBs) have changed lives since their invention in the early 1990s. Further improvement of their energy density is highly desirable to meet the increasing demands of energy storage applications. Active lithium loss in the initial charge process appreciably reduces the capacity and energy density of LIBs due to the formation of a solid electrolyte interface (SEI) on the anode surface, especially for Si based anodes in high-energy-density batteries. To solve...

Metallic Zn is a preferred anode material for rechargeable aqueous batteries towards a smart grid and renewable energy storage. Understanding how the metal nucleates and grows at the aqueous Zn anode is a critical and challenging step to achieve full reversibility of Zn battery chemistry, especially under fast-charging conditions. Here, by combining in situ optical imaging and theoretical modeling, we uncover the critical parameters governing the electrodeposition stability of the metallic Zn electrode, that is, the competition among crystallographic thermodynamics, kinetics, and Zn 2 + -ion diffusion. Moreover, steady-state Zn metal plating/ stripping with Coulombic efficiency above 99 % is achieved at 10-100 mA cm À 2 in a reasonably high concentration (3 M) ZnSO 4 electrolyte. Significantly, a long-term cycling-stable Zn metal electrode is realized with a depth of discharge of 66.7 % under 50 mA cm À 2 in both Zn j j Zn symmetrical cells and MnO 2 j j Zn full cells.

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Metallic lithium (Li) is the ultimate anode candidate for high-energy-density rechargeable batteries. However, its practical application is hindered by serious problems, including uncontrolled dendritic Li growth and undesired side reactions. In this study a concept of "salt-in-metal" is proposed, and a Li/LiNO 3 composite foil is constructed such that a classic electrolyte additive, LiNO 3 , is embedded successfully into the bulk structure of metallic Li by a facile mechanical kneading approach. The LiNO 3 reacts with metallic Li to generate Li + conductive species (e.g., Li 3 N and LiN x O y ) over the entire electrode. These derivatives afford a stable solid electrolyte interphase (SEI) and effectively regulate the uniformity of the nucleation/growth of Li on initial plating, featuring a low nucleation energy barrier and large crystalline size without mossy morphology. Importantly, these derivatives combined with LiNO 3 can in-situ repair the damaged SEI from the large volume change during Li plating/stripping, enabling a stable electrode-electrolyte interface and suppressing side reactions between metallic Li and electrolyte. Stable cycling with a high capacity retention of 93.1% after 100 cycles is obtained for full cells consisting of high-loading LiCoO 2 cathode (≈20 mg cm −2 ) and composite metallic Li anode with 25 wt% LiNO 3 under a lean electrolyte condition (≈12 µL) at 0.5 C.

Lithium‐Ion Batteries Prelithiation provides additional active lithium to batteries through using specific reagents/materials or processing, and is a promising strategy to resolve the lithium loss issue and increase the energy density of lithium‐ion batteries. In article number 2101565 Yongming Sun and co‐workers assess the common parameters of various prelithaition approaches that must be achieved and common challenges/issues that must be solved to enable the practical application of this strategy.

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A 3D railway-like electrode design to tackle the poor conductivity and severe volume expansion in a room temperature Na–S battery.