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The utilization of Li metal anodes (LMAs) can satisfy the requirements of high-energy-density rechargeable batteries. However, LMAs are plagued by dendrite formation, low coulombic efficiency (CE), and interfacial side reactions. Here, a metal–organic framework (MOF) with high specific area and 1D aligned molecular channels is designed and prepared as an artificial solid electrolyte interphase (SEI) to regulate the interfacial stability of LMAs. The porous structure enables the accommodation of the liquid electrolyte, while the Li+ transport channel promotes uniform lithium deposition and mitigates dendrite growth. The open metal sites in the MOF facilitate the entrapment of anions, thereby impeding anion migration and improving Li+ transport kinetics. Owing to these advantages, cells based on MOF modified copper current collectors exhibit a high CE of 98.6% for 200 cycles at 1 mA cm−2 and 1 mA h cm−2. The symmetric cell shows an improved lifespan of 2000 h with a small voltage hysteresis of 25 mV at 0.5 mA cm−2 and 1 mA h cm−2. [ABSTRACT FROM AUTHOR]

LiNO3 is an effective additive for improving the performance of Li metal anodes. However, the practical application of LiNO3 is limited due to its poor solubility. Here, a novel electrolyte additive of MgAl layered double hydroxides (LDHs) with open interlayered anionic vacancies is proposed. The electropositive MgAl LDHs promote the spontaneous coordination of NO3− into anionic vacancies of LDH interlayers via memory effect, rehydrating to original NO3−‐MgAl LDHs structure and accelerating LiNO3 dissolution. The reconstructed NO3−‐MgAl LDHs play a crucial role as sustainable nitrate resources, preventing partial NO3− from participating in the Li+ solvent sheath to reduce the solvation binding energy. Moreover, MgAl LDHs absorb the anions due to electrostatic attraction, accounting for more dissociated Li+ and active Li+ migration in carbonate electrolytes. NO3− stored in MgAl LDHs is also preferentially reduced to form Li3N‐rich solid electrolyte interphase (SEI), decreasing the activation energy barrier for Li+ transport and striving to form a uniform Li deposition. The cells assembled with MgAl LDHs and LiNO3 additives deliver high Coulombic efficiency, excellent rate capability, and high capacity retention. This strategy provides new insights into LiNO3‐promotor design and excavates the potential of LDHs materials for Li metal batteries. [ABSTRACT FROM AUTHOR]

With the ever-growing market of electric vehicles, spent lithium-ion batteries (LIBs) eventually turn into a very challenging issue to both the environment and resource sustainability. Recycling the valuable components in spent LIBs becomes a key link in the closed-loop LIB industry. Pretreatment is the primary procedure for recycling LIBs in view of component classification. Traditional separation methods usually destroy the active materials or current collectors. Herein, we report a facile one-step solvothermal pretreatment using ethanol as the solvent. The separation mechanism of cathode materials and Al foil via digestion of polyvinylidene fluoride has been discussed. The pretreatment causes minimum damage to both the LiNi0.5Co0.2Mn0.3O2 (NCM523) cathode material and Al foil. Subsequently, the degraded NCM523 powders are regenerated by repairing the layered crystal structure and restoring the lost Li. The regenerated NCM523 cathode delivers excellent electrochemical performance. This work provides a feasible and cost-effective strategy to recycle the Al current collector and regenerate spent cathode materials. [ABSTRACT FROM AUTHOR]

Solid‐state electrolytes hold great promise for lithium‐based batteries with high energy density and safety. Here, novel metal‐organic frameworks (MOFs) based composite membranes were fabricated by a rolling process and subsequently employed as quasi solid‐state electrolytes, exhibiting improved ionic conductivity and Li+ transference number as well as stable electrochemical window. Furthermore, the MOF‐based membranes presented a significant effect in modulating the stripping/plating process of Li and resulted in a dendrite‐free Li deposition. The corresponding LiFePO4|Li batteries were assembled and presented improved rate capability and high Coulombic efficiency, offering a new option for MOF‐based electrolytes. [ABSTRACT FROM AUTHOR]

The carbonate electrolyte chemistry is a primary determinant for the development of high-voltage lithium metal batteries (LMBs). Unfortunately, their implementation is greatly plagued by sluggish electrode interfacial dynamics and insufficient electrolyte thermodynamic stability. Herein, lithium trifluoroacetate-lithium nitrate (LiTFA-LiNO 3 ) dual-salt additive-reinforced carbonate electrolyte (LTFAN) is proposed for stabilizing high-voltage LMBs. We reveal that 1) the in situ generated inorganic-rich electrode-electrolyte interphase (EEI) enables rapid interfacial dynamics, 2) TFA - preferentially interacts with moisture over PF 6 - to strengthen the moisture tolerance of designed electrolyte, and 3) NO 3 - is found to be noticeably enriched at the cathode interface on charging, thus constructing Li + -enriched, solvent-coordinated, thermodynamically favorable electric double layer (EDL). The superior moisture tolerance of LTFAN and the thermodynamically stable EDL constructed at cathode interface play a decisive role in upgrading the compatibility of carbonate electrolyte with high-voltage cathode. The LMBs with LTFAN realize 4.3 V-NCM523/4.4 V-NCM622 superior cycling reversibility and excellent rate capability, which is the leading level of documented records for carbonate electrode., (© 2024 Wiley-VCH GmbH.)