High dielectric single-ion conducting interphase enables fast-charging lithium metal batteries.

The poor stability and slow lithium ion (Li+) transfer kinetics of solid electrolyte interphase (SEI) pose significant challenges to lithium (Li) metal batteries. Although various SEI-related strategies have been developed, the Li+ transport properties and uniform Li deposition still require substantial improvement for fast-charging applications. Herein, we introduce a dielectric, single-ion-conductive artificial SEI (DS-SEI) composed of lithiated Nafion and BaTiO3 (BTO) nanoceramics to address these issues. The lithiated Nafion stabilizes the Li anode with its elastic F-rich components and facilitates fast, single Li+ conduction through its anion-anchored structure. The high-dielectric BTO dynamically homogenizes the electric field (E-field) to promote uniform Li deposition, synergistically enhancing intrinsic single Li+ conductivity and Li+ desolvation/diffusion kinetics, thereby enabling fast charging of the Li anode. Consequently, the DS-SEI protected Li anode can cycle over 6800 h in a Li||Li cell at 10 mA cm-2/5 mAh cm-2, over 400 cycles in a 2.75 mAh cm-2 Li||LiFePO4 cell at 1C, with 83.0 % capacity retention at 6C (16.5 mA cm-2), and maintain stable cycling in a 5.62 mAh cm-2 Li||Li6PS5Cl|| LiNi0.8Co0.1Mn0.1O2 all solid-state cell. Our findings provide insights into the interfacial regulation of Li anode, paving the way for fast-charging Li metal batteries.

Ai G ，Lian X ，Hu Z ，Lyu Y ，Mo T ，Zhao X ，Hou X ，Sun M ，Zhao H ，Zhang T ，Mao W ... -  《-》

Superionic conducting vacancy-rich β-Li(3)N electrolyte for stable cycling of all-solid-state lithium metal batteries.

The advancement of all-solid-state lithium metal batteries requires breakthroughs in solid-state electrolytes (SSEs) for the suppression of lithium dendrite growth at high current densities and high capacities (>3 mAh cm-2) and innovation of SSEs in terms of crystal structure, ionic conductivity and rigidness. Here we report a superionic conducting, highly lithium-compatible and air-stable vacancy-rich β-Li3N SSE. This vacancy-rich β-Li3N SSE shows a high ionic conductivity of 2.14 × 10-3 S cm-1 at 25 °C and surpasses almost all the reported nitride-based SSEs. A Li- and N-vacancy-mediated fast lithium-ion migration mechanism is unravelled regarding vacancy-triggered reduced activation energy and increased mobile lithium-ion population. All-solid-state lithium symmetric cells using vacancy-rich β-Li3N achieve breakthroughs in high critical current densities up to 45 mA cm-2 and high capacities up to 7.5 mAh cm-2, and ultra-stable lithium stripping and plating processes over 2,000 cycles. The high lithium compatibility mechanism of vacancy-rich β-Li3N is unveiled as intrinsic stability to lithium metal. In addition, β-Li3N possesses excellent air stability through the formation of protection surfaces. All-solid-state lithium metal batteries using the vacancy-rich β-Li3N as SSE interlayers and lithium cobalt oxide (LCO) and Ni-rich LiNi0.83Co0.11Mn0.06O2 (NCM83) cathodes exhibit excellent battery performance. Extremely stable cycling performance is demonstrated with high capacity retentions of 82.05% with 95.2 mAh g-1 over 5,000 cycles at 1.0 C for LCO and 92.5% with 153.6 mAh g-1 over 3,500 cycles at 1.0 C for NCM83. Utilizing the vacancy-rich β-Li3N SSE and NCM83 cathodes, the all-solid-state lithium metal batteries successfully accomplished mild rapid charge and discharge rates up to 5.0 C, retaining 60.47% of the capacity. Notably, these batteries exhibited a high areal capacity, registering approximately 5.0 mAh cm-2 for the compact pellet-type cells and around 2.2 mAh cm-2 for the all-solid-state lithium metal pouch cells.

Li W ，Li M ，Wang S ，Chien PH ，Luo J ，Fu J ，Lin X ，King G ，Feng R ，Wang J ，Zhou J ，Li R ，Liu J ，Mo Y ，Sham TK ，Sun X ... -  《-》

A Self-Healing, Flowable, Yet Solid Electrolyte Suppresses Li-Metal Morphological Instabilities.

Lithium metal (Li0) solid-state batteries encounter implementation challenges due to dendrite formation, side reactions, and movement of the electrode-electrolyte interface in cycling. Notably, voids and cracks formed during battery fabrication/operation are hot spots for failure. Here, a self-healing, flowable yet solid electrolyte composed of mobile ceramic crystals embedded in a reconfigurable polymer network is reported. This electrolyte can auto-repair voids and cracks through a two-step self-healing process that occurs at a fast rate of 5.6 µm h-1. A dynamical phase diagram is generated, showing the material can switch between liquid and solid forms in response to external strain rates. The flowability of the electrolyte allows it to accommodate the electrode volume change during Li0 stripping. Simultaneously, the electrolyte maintains a solid form with high tensile strength (0.28 MPa), facilitating the regulation of mossy Li0 deposition. The chemistries and kinetics are studied by operando synchrotron X-ray and in situ transmission electron microscopy (TEM). Solid-state NMR reveals a dual-phase ion conduction pathway and rapid Li+ diffusion through the stable polymer-ceramic interphase. This designed electrolyte exhibits extended cycling life in Li0-Li0 cells, reaching 12 000 h at 0.2 mA cm-2 and 5000 h at 0.5 mA cm-2. Furthermore, owing to its high critical current density of 9 mA cm-2, the Li0-LiNi0.8Mn0.1Co0.1O2 (NMC811) full cell demonstrates stable cycling at 5 mA cm-2 for 1100 cycles, retaining 88% of its capacity, even under near-zero stack pressure conditions.

He Y ，Wang C ，Lin R ，Hu E ，Trask SE ，Li J ，Xin HL ... -  《-》

Study on an Interpenetrating Artificial SEI for Lithium Metal Anode Modification and Fast Charging Characterization.

Li A ，Xin W ，Wang Q ，Ai W ，Han W ，Yang C ，Wang Y ，Du N ，Liu C ，Zhang Y ，Li X ，Zhang Y ... -  《-》

Long-Cycling, Fast-Charging Lithium Metal Batteries Enabled by Nickel-Carbon Composite Nanosheet Arrays Modified Lithium Metal Anodes.

Lithium (Li) metal anode, one of the most promising candidates for next-generation rechargeable batteries, has always suffered from uneven Li deposition/stripping. To address this issue, this work designs a novel nickel-carbon composite modified Li metal anode (FNC-NF) by carbonizing fluoride nickel hydroxide nanosheet arrays grown on nickel foam (NF). These electrochemical tests present that the conductive and lithiophilic FNC can effectively restrain the growth of Li dendrites during the cycling of Li deposition/stripping at large capacities up to 10 mAh cm-2. This result is attributed to the featured FNC composition combining a core of nickel hydroxide and a mixed coating of defective carbon and Ni nanoparticles, and the unique hierarchical morphology of the FNC-NF integrating porous NF and vertically aligned FNC nanosheets. Consequently, the FNC-NF presents a stable coulombic efficiency performance after 900 cycles with an average of 99.23% for half cells, a lifespan over 3200 h for symmetric cells at 1 mA cm-2 and 1 mAh cm-2, and a remarkable cycling stability at large current densities of up to 15 mA cm-2 at 1 mAh cm-2. Moreover, the Li||FNC-NF||LiFePO4 full cells show superior capacity retention and cycling stability at 1 C.

Wang X ，Xu L ，Niu S ，Zhang Q ，Lian Q ，Xiang S ，Mao Z ，Han Y ，Huang Y ，Li G ，Zuo Z ，Lan S ，Shi R ，Liao C ，Li H ，Amini A ，Wang N ，Cheng C ... -  《-》