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1. Regulating Li‐Ion Transport through Ultrathin Molecular Membrane to Enable High‐Performance All‐Solid‐State–Battery

   https://doi.org/10.1002/smll.202303625  

   Rajendran, Sathish; George, Antony; Tang, Zian; Neumann, Christof; Turchanin, Andrey; Arava, Leela_Mohana_Reddy (June 2023, Small)

   Abstract Solid‐state lithium metal batteries with garnet‐type electrolyte provide several advantages over conventional lithium‐ion batteries, especially for safety and energy density. However, a few grand challenges such as the propagation of Li dendrites, poor interfacial contact between the solid electrolyte and the electrodes, and formation of lithium carbonate during ambient exposure over the solid‐state electrolyte prevent the viability of such batteries. Herein, an ultrathin sub‐nanometer porous carbon nanomembrane (CNM) is employed on the surface of solid‐state electrolyte (SSE) that increases the adhesion of SSE with electrodes, prevents lithium carbonate formation over the surface, regulates the flow of Li‐ions, and blocks any electronic leakage. The sub‐nanometer scale pores in CNM allow rapid permeation of Li‐ions across the electrode–electrolyte interface without the presence of any liquid medium. Additionally, CNM suppresses the propagation of Li dendrites by over sevenfold up to a current density of 0.7 mA cm⁻²and enables the cycling of all‐solid‐state batteries at low stack pressure of 2 MPa using LiFePO₄cathode and Li metal anode. The CNM provides chemical stability to the solid electrolyte for over 4 weeks of ambient exposure with less than a 4% increase in surface impurities. 

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2. Highly‐Cyclable Room‐Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries

   https://doi.org/10.1002/adfm.201910749  

   Rojaee, Ramin; Cavallo, Salvatore; Mogurampelly, Santosh; Wheatle, Bill_K; Yurkiv, Vitaliy; Deivanayagam, Ramasubramonian; Foroozan, Tara; Rasul, Md_Golam; Sharifi‐Asl, Soroosh; Phakatkar, Abhijit_H; et al (June 2020, Advanced Functional Materials)

   Abstract Despite significant interest toward solid‐state electrolytes owing to their superior safety in comparison to liquid‐based electrolytes, sluggish ion diffusion and high interfacial resistance limit their application in durable and high‐power density batteries. Here, a novel quasi‐solid Li⁺ion conductive nanocomposite polymer electrolyte containing black phosphorous (BP) nanosheets is reported. The developed electrolyte is successfully cycled against Li metal (over 550 h cycling) at 1 mA cm⁻²at room temperature. The cycling overpotential is dropped by 75% in comparison to BP‐free polymer composite electrolyte indicating lower interfacial resistance at the electrode/electrolyte interfaces. Molecular dynamics simulations reveal that the coordination number of Li⁺ions around (trifluoromethanesulfonyl)imide (TFSI⁻) pairs and ethylene‐oxide chains decreases at the Li metal/electrolyte interface, which facilitates the Li⁺transport through the polymer host. Density functional theory calculations confirm that the adsorption of the LiTFSI molecules at the BP surface leads to the weakening of N and Li atomic bonding and enhances the dissociation of Li⁺ions. This work offers a new potential mechanism to tune the bulk and interfacial ionic conductivity of solid‐state electrolytes that may lead to a new generation of lithium polymer batteries with high ionic conduction kinetics and stable long‐life cycling. 

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3. Lithium crystallization at solid interfaces

   https://doi.org/10.1038/s41467-023-38757-2  

   Yang, Menghao; Liu, Yunsheng; Mo, Yifei (May 2023, Nature Communications)

   Abstract Understanding the electrochemical deposition of metal anodes is critical for high-energy rechargeable batteries, among which solid-state lithium metal batteries have attracted extensive interest. A long-standing open question is how electrochemically deposited lithium-ions at the interfaces with the solid-electrolytes crystalize into lithium metal. Here, using large-scale molecular dynamics simulations, we study and reveal the atomistic pathways and energy barriers of lithium crystallization at the solid interfaces. In contrast to the conventional understanding, lithium crystallization takes multi-step pathways mediated by interfacial lithium atoms with disordered and random-closed-packed configurations as intermediate steps, which give rise to the energy barrier of crystallization. This understanding of multi-step crystallization pathways extends the applicability of Ostwald’s step rule to interfacial atom states, and enables a rational strategy for lower-barrier crystallization by promoting favorable interfacial atom states as intermediate steps through interfacial engineering. Our findings open rationally guided avenues of interfacial engineering for facilitating the crystallization in metal electrodes for solid-state batteries and can be generally applicable for fast crystal growth. 

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4. Prelithiation of Alloy Anodes via Roll Pressing for Solid‐State Batteries

   https://doi.org/10.1002/adma.202508973  

   Wang, Congcheng; Jeong, Won_Joon; Nelson, Douglas_Lars; Sridhara, Hari; Anderson, Sophia_Nicolette; McDowell, Matthew_T (August 2025, Advanced Materials)

   Abstract Solid‐state batteries with alloy‐type negative electrodes can feature enhanced energy density and safety compared to conventional Li‐ion batteries. However, diffusional Li trapping within Li alloys often causes low initial Coulombic efficiency and leads to capacity loss with cycling. Here, a general roll‐pressing prelithiation method compatible with a variety of alloy‐type negative electrodes (silicon, aluminum, tin, and multi‐phase alloys) is introduced, which is shown to improve performance in solid‐state batteries. By warm‐rolling lithium foil of controlled thickness with various alloy‐type electrodes, both slurry‐cast and foil‐type electrodes can be uniformly prelithiated via direct chemical reaction. The prelithiated electrodes exhibit enhanced specific capacity and extended cycle life in batteries with Li₆PS₅Cl solid‐state electrolyte. Prelithiated multi‐phase foil electrodes with a tailored interface are shown to exhibit superior cycling stability down to 2 MPa stack pressure. This prelithiation technique offers a pathway to overcome intrinsic challenges in alloy anodes for solid‐state batteries. 

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5. NASICON Li _1.2 Mg _0.1 Zr _1.9 (PO ₄ ) ₃ Solid Electrolyte for an All‐Solid‐State Li‐Metal Battery

   https://doi.org/10.1002/smtd.202000764  

   Zhou, Qiongyu; Xu, Biyi; Chien, Po‐Hsiu; Li, Yutao; Huang, Bing; Wu, Nan; Xu, Henghui; Grundish, Nicholas S.; Hu, Yan‐Yan; Goodenough, John B. (September 2020, Small Methods)

   Abstract A thin solid electrolyte with a high Li⁺conductivity is used to separate the metallic lithium anode and the cathode in an all‐solid‐state Li‐metal battery. However, most solid Li‐ion electrolytes have a small electrochemical stability window, large interfacial resistance, and cannot block lithium‐dendrite growth when lithium is plated on charging of the cell. Mg²⁺stabilizes a rhombohedral NASICON‐structured solid electrolyte of the formula Li_1.2Mg_0.1Zr_1.9(PO₄)₃(LMZP). This solid electrolyte has Li‐ion conductivity two orders of magnitude higher at 25 °C than that of the triclinic LiZr₂(PO₄)₃.⁷Li and⁶Li NMR confirm the Li‐ions in two different crystallographic sites of the NASICON framework with 85% of the Li‐ions having a relatively higher mobility than the other 15%. The anode–electrolyte interface is further investigated with symmetric Li/LMZP/Li cell testing, while the cathode–electrolyte interface is explored with an all‐solid‐state Li/LMZP/LiFePO₄cell. The enhanced performance of these cells enabled by the Li_1.2Mg_0.1Zr_1.9(PO₄)₃solid electrolyte is stable upon repeated charge/discharge cycling. 

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