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Li+ de‐solvation at solid‐electrolyte interphase (SEI)‐electrolyte interface stands as a pivotal step that imposes limitations on the fast‐charging capability and low‐temperature performance of lithium‐ion batteries (LIBs). Unraveling the contributions of key constituents in the SEI that facilitate Li+ de‐solvation and deciphering their mechanisms, as a design principle for the interfacial structure of anode materials, is still a challenge. Herein, we conducted a systematic exploration of the influence exerted by various inorganic components (Li2CO3, LiF, Li3PO4) found in the SEI on their role in promoting the Li+ de‐solvation. The findings highlight that Li3PO4‐enriched SEI effectively reduces the de‐solvation energy due to its ability to attenuate the Li+‐solvent interaction, thereby expediting the de‐solvation process. Building on this, we engineer Li3PO4 interphase on graphite (LPO−Gr) anode via a simple solid‐phase coating, facilitating the Li+ de‐solvation and building an inorganic‐rich SEI, resulting in accelerated Li+ transport crossing the electrode interfaces and interphases. Full cells using the LPO−Gr anode can replenish its 80 % capacity in 6.5 minutes, while still retaining 70 % of the room temperature capacity even at −20 °C. Our strategy establishes connection between the de‐solvation characteristics of the SEI components and the interfacial structure design of anode materials for high performance LIBs. [ABSTRACT FROM AUTHOR]

The uncontrollable growth of dendrites, infinite volume changes, low Coulombic efficiencies, and poor charging/discharging rates in lithium metal anodes have seriously hampered the further development of lithium metal batteries. Trapping lithium (Li) into rationally designed three‐dimensional (3D) structured Li metal anodes in order to construct a 3D‐Li framework is an effective approach to suppress the growth of Li dendrites. However, material inconsistencies and high costs still seriously limit practical applications. In this study, we describe the use of commercial low‐cost graphite fiber (GF) as a suitable conformal scaffold for preparing a lithiophilic SnO2@GF material using facile infiltration method. The lithiophilic 3D porous conductive framework allows homogeneous Li deposition on the surface of a structured electrode and accommodates the volume change during Li plating/stripping, leading to a significant boost in both the charging/discharging rates and cycling stability. This study highlights the significance of interface‐related science and engineering in designing high‐performance Li metal anodes, but also highlights the need for greater dedication to the construction of highly stable lithium anodes and high‐energy density Li metal batteries in a low‐cost manner. [ABSTRACT FROM AUTHOR]

Electrocatalysis is generally confined to dynamic liquid-solid and gas-solid interfaces and is rarely applicable in solid-state reactions. Here, we report a paradigm shift strategy to exploit electrocatalysis to accelerate solid-state reactions in the context of lithium-ion batteries (LIBs). We employ heteroatom doping, specifically boron for silicon and sulfur for phosphorus, to catalyze electrochemical Li-alloying reactions in solid-state electrode materials. The preferential cleavage of polar dopant-host chemical bonds upon lithiation triggers chemical bond breaking of the host material. This solid-state catalysis, distinct from liquid and gas phases, requires a critical doping concentration for optimal performance. Beyond a critical concentration of ∼1 atom %, boron and sulfur doping drastically reduces activation energies and accelerates redox kinetics during lithiation/delithiation processes, leading to markedly enhanced rate performance in boron-doped silicon and sulfur-doped black/red phosphorus anode. Notably, a sulfur-doped black phosphorus anode coupled with a lithium cobalt oxide cathode achieves an ultrafast-charging battery, recharging 80% energy of a battery in 302 Wh kg -1 in 9 min, surpassing the thus far reported LIBs.

Li + de-solvation at solid-electrolyte interphase (SEI)-electrolyte interface stands as a pivotal step that imposes limitations on the fast-charging capability and low-temperature performance of lithium-ion batteries (LIBs). Unraveling the contributions of key constituents in the SEI that facilitate Li + de-solvation and deciphering their mechanisms, as a design principle for the interfacial structure of anode materials, is still a challenge. Herein, we conducted a systematic exploration of the influence exerted by various inorganic components (Li 2 CO 3 , LiF, Li 3 PO 4 ) found in the SEI on their role in promoting the Li + de-solvation. The findings highlight that Li 3 PO 4 -enriched SEI effectively reduces the de-solvation energy due to its ability to attenuate the Li + -solvent interaction, thereby expediting the de-solvation process. Building on this, we engineer Li 3 PO 4 interphase on graphite (LPO-Gr) anode via a simple solid-phase coating, facilitating the Li + de-solvation and building an inorganic-rich SEI, resulting in accelerated Li + transport crossing the electrode interfaces and interphases. Full cells using the LPO-Gr anode can replenish its 80 % capacity in 6.5 minutes, while still retaining 70 % of the room temperature capacity even at -20 °C. Our strategy establishes connection between the de-solvation characteristics of the SEI components and the interfacial structure design of anode materials for high performance LIBs., (© 2024 Wiley-VCH GmbH.)

The most successful lithium-ion batteries (LIBs) based on ethylene carbonate electrolytes and graphite anodes still suffer from severe energy and power loss at temperatures below -20 °C, which is because of high viscosity or even solidification of electrolytes, sluggish de-solvation of Li + at the electrode surface, and slow Li + transportation in solid electrolyte interphase (SEI). Here, a coherent lithium phosphide (Li 3 P) coating firmly bonding to the graphite surface to effectively address these challenges is engineered. The dense, continuous, and robust Li 3 P interphase with high ionic conductivity enhances Li + transportation across the SEI. Plus, it promotes Li + de-solvation through an electron transfer mechanism, which simultaneously accelerates the charge transport kinetics and stands against the co-intercalation of low-melting-point solvent molecules, such as propylene carbonate (PC), 1,3-dioxolane, and 1,2-dimethoxyethane. Consequently, an unprecedented combination of high-capacity retention and fast-charging ability for LIBs at low temperatures is achieved. In full-cells encompassing the Li 3 P-coated graphite anode and PC electrolytes, an impressive 70% of their room-temperature capacity is attained at -20 °C with a 4 C charging rate and a 65% capacity retention is achieved at -40 °C with a 0.05 C charging rate. This research pioneers a transformative trajectory in fortifying LIB performance in cryogenic environments., (© 2023 Wiley‐VCH GmbH.)