High-Performance Quasi-Solid-State Lithium Metal Batteries: Interface Engineering Using Solid–Liquid Dual Therapy by Solvated Ionic Liquid and NiO Kuntal Ghosh, Mononita Das, Alok Kumar Chaudhary, Mir Wasim Raja ACS Applied Materials and Interfaces, 2025 High Resolution Image Download MS PowerPoint Slide Developing efficient solid-state lithium metal batteries (SSLMBs) remains challenging due to interfacial incompatibility and dendrite growth at the metal–electrolyte boundary. To address these issues, a dual-therapy approach was introduced, combining solid therapy of LLZO via a NiO sintering aid and liquid therapy using a solvated ionic liquid (SIL) for SSLMBs. The solid therapy treatment enhanced the grain boundary conductivity by ∼7 times and improved densification by forming a new K 2 NiF 4 -type lithiated phase upon introducing 0.5 wt % of NiO into the Ga-doped LLZO matrix (GN050). Meanwhile, SIL infusion in GN050 (GN050-SIL) achieves high ionic conductivity at RT (0.252 mS·cm –1 ), low Li/LLZO interfacial resistance (87.4 Ω), and broader potential window (>5.5 V). This combined approach also minimized the SIL dependency for ionic conduction- a critical step toward scalable, almost solid-state batteries. GN050-SIL shows stable plating/stripping behavior for over 1000 h without any short circuit, with a critical current density (CCD) of 0.55 mA·cm –2 . In the full-cell test with a Li-metal anode and LiMn 2 O 4 cathodes, GN050-SIL exhibited superior charge/discharge performance at different current densities (0.1–1.4 mA·cm –2 ) compared to SIL-infused Ga-doped LLZO electrolyte (GN000-SIL). The Li/GN050-SIL/NMC111 full cell also demonstrates excellent rate capability and long-term cycling stability at higher C-rates. XPS, FESEM/EDX, and distribution of relaxation time (DRT) analyses reveal a uniformly confined SIL within the LLZO framework as well as the formation of a stable LiF/CF x interphase without any structural degradation after cycling. This study thus highlights the potential of dual-therapy engineering for next-generation SSLMBs.
Engineered Li7La3Zr2O12 (LLZO) for Pseudo-Solid-State Lithium Metal Batteries (SSLMBs): Tailor-Made Synthesis, Evolution of the Microstructure, Suppression of Dendritic Growth, and Enhanced Electrochemical Performance Kuntal Ghosh, Mir Wasim Raja ACS Applied Energy Materials, 2023 Morphologically engineered Li 7 La 3 Zr 2 O 12 (LLZO) impregnated with a common solvated ionic liquid (SIL) can greatly influence the cycling performance (360 cycles), coulombic efficiency (>99%), and high rate capability (0.05–1.2 mA·cm –2 ) of pseudo-solid-state lithium metal batteries (SSLMBs). In this report, to obtain a unique microstructure of cubic-LLZO, a fine-tuned combustion synthesis process was first designed; synthetic parameters were duly optimized, and powders were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Fourier transform infrared spectroscopy (FTIR), 1 H NMR, and Raman spectroscopy. An in-depth analysis of powder properties and electrochemical behavior of the fabricated SSLM cells revealed that impurities present in LLZO significantly facilitated electrochemical cell performances. Such a combination of the engineered LLZO impregnated with the SIL enabled the plating and stripping cycles in Li symmetric cells with up to 200 h of operation at a constant current density of 0.05 mA·cm –2 avoiding short circuit. The critical current density (CCD) was found to be 450 μA cm –2, which is significantly higher than the other reported CCD values for pristine LLZO. The post-electrochemical study revealed that transgranular lithium dendritic growth, a genuine problem in SSLMBs, was impeded to a significant extent by the engineered LLZO and an in situ formed phase, Li 0.5 Al 0.5 La 2 O 4, at grain boundaries during cycling. The multicathode compatibility tests as performed (Li/LLZO-SIL/LMO, Li/LLZO-SIL/LFP, and Li/LLZO-SIL/NMC111) exhibited that morphologically altered LLZO with the SIL interface is compatible with most of the commercial cathodes. The study thus envisaged that the engineered LLZO solid electrolyte impregnated with the SIL can exert a synergistic effect to enhance faster Li-ion conduction as well as resistance to Li dendritic growth, providing a path for developing high-performance SSLMBs.
Ga-Doped LLZO Solid-State Electrolyte with Unique "plate-like" Morphology Derived from Water Hyacinth (Eichhornia crassipes) Aquatic Weed: Waste to Wealth Conversion Kuntal Ghosh, Mir Wasim Raja ACS Omega, 2022 An attempt has been made for the first time to convert waste biomass such as water hyacinth (WH) to a functional energy material in a cost-effective way. The present research describes a novel exo-templating methodology to develop engineered microstructure of Ga-doped Li7La3Zr2O12 (Li6.25La3Ga0.25Zr2O12, referred as WH-Ga-LLZO) solid-state electrolyte for its use in all solid-state lithium batteries (ASSLBs) by mimicking the intercellular structure of water hyacinth (Eichhornia crassipes), an invasive and noxious aquatic plant. The developed exo-templated methodology offers a low calcination temperature of 1000 °C in air where all the major peaks could be indexed as cubic garnet, as confirmed by XRD. The FESEM micrographs revealed a unique “plate-like” morphology that mimicked the intercellular structure of water hyacinth fiber. The bulk lithium-ion conductivity in the WH-Ga-LLZO electrolyte was found to be 3.94 × 10–5 S/cm. Li/WH-Ga-LLZO/Li cells were galvanostatically cycled for a continuous 295 h with increasing step current densities from 28 μA/cm2 without a short circuit. The highest current density as measured for maximum polarization in a symmetric cell was found to be 452 μA/cm2. The WH exo-templated methodology was thus developed and optimized and can be extended for synthesizing any application-specific multifunctional materials.
RECENT SCHOLAR PUBLICATIONS
LLZO incorporated dual polymer-based composite electrolyte for enhanced conductivity and long‑term stability for solid‑state lithium‑metal batteries K Ghosh, M Das, MW Raja Journal of Solid State Electrochemistry 30 (1), 121-139 , 2026 2026 Citations: 5
High-Performance Quasi-Solid-State Lithium Metal Batteries: Interface Engineering Using Solid–Liquid Dual Therapy by Solvated Ionic Liquid and NiO K Ghosh, M Das, AK Chaudhary, M Wasim Raja ACS Applied Materials & Interfaces 17 (50), 68052-68073 , 2025 2025
The critical role of Al2O3, BaTiO3 and ZrO2 nanoceramic fillers in PVDF-HFP based composite polymer electrolytes for high performance lithium-metal batteries M Das, K Ghosh, Vijaya, MW Raja Solid State Ionics 430, 117008 , 2025 2025 Citations: 7
Role of LLZO active filler in PVDF-modified cellulosic paper matrix: A sustainable, thermally durable and high-performance separator for next generation lithium batteries K Ghosh, M Das, MW Raja Journal of Power Sources 654, 237838 , 2025 2025 Citations: 6
Mg and F Co-Doped Nasicon Solid Electrolyte with Interfacial Liquid Therapy: A Synergistic Approach for High-Performance Sodium Metal Batteries K Ghosh, M Das, M Wasim Raja 247th ECS Meeting (May 18-22, 2025) , 2025 2025
Studies on Advanced Solid Electrolytes for Solid-State Metal Batteries K Ghosh PhD Thesis, Jadavpur University , 2025 2025
Flexible ceramic based ‘paper separator’with enhanced safety for high performance lithium-ion batteries: probing the effect of ceramics impregnation on electrochemical performances M Das, K Ghosh, MW Raja Journal of Power Sources 606, 234573 , 2024 2024 Citations: 22
Facile Li-ion transport in microstructurally engineered hybrid LLZO electrolyte for application in pseudo-solid state lithium metal batteries K Ghosh, MW Raja Chemical Engineering Journal 480, 148200 , 2024 2024 Citations: 19
Engineered Li 7 La 3 Zr 2 O 12 (LLZO) for Pseudo-Solid-State Lithium Metal Batteries (SSLMBs): Tailor-Made Synthesis, Evolution of the Microstructure, Suppression … K Ghosh, M Wasim Raja ACS Applied Energy Materials 6 (7), 4035-4052 , 2023 2023 Citations: 20
Ga-Doped LLZO Solid-State Electrolyte with Unique “Plate-like” Morphology Derived from Water Hyacinth ( Eichhornia crassipes ) Aquatic Weed: Waste to Wealth … K Ghosh, M Wasim Raja ACS omega 7 (37), 33385-33396 , 2022 2022 Citations: 21
MOST CITED SCHOLAR PUBLICATIONS
Flexible ceramic based ‘paper separator’with enhanced safety for high performance lithium-ion batteries: probing the effect of ceramics impregnation on electrochemical performances M Das, K Ghosh, MW Raja Journal of Power Sources 606, 234573 , 2024 2024 Citations: 22
Ga-Doped LLZO Solid-State Electrolyte with Unique “Plate-like” Morphology Derived from Water Hyacinth ( Eichhornia crassipes ) Aquatic Weed: Waste to Wealth … K Ghosh, M Wasim Raja ACS omega 7 (37), 33385-33396 , 2022 2022 Citations: 21
Engineered Li 7 La 3 Zr 2 O 12 (LLZO) for Pseudo-Solid-State Lithium Metal Batteries (SSLMBs): Tailor-Made Synthesis, Evolution of the Microstructure, Suppression … K Ghosh, M Wasim Raja ACS Applied Energy Materials 6 (7), 4035-4052 , 2023 2023 Citations: 20
Facile Li-ion transport in microstructurally engineered hybrid LLZO electrolyte for application in pseudo-solid state lithium metal batteries K Ghosh, MW Raja Chemical Engineering Journal 480, 148200 , 2024 2024 Citations: 19
The critical role of Al2O3, BaTiO3 and ZrO2 nanoceramic fillers in PVDF-HFP based composite polymer electrolytes for high performance lithium-metal batteries M Das, K Ghosh, Vijaya, MW Raja Solid State Ionics 430, 117008 , 2025 2025 Citations: 7
Role of LLZO active filler in PVDF-modified cellulosic paper matrix: A sustainable, thermally durable and high-performance separator for next generation lithium batteries K Ghosh, M Das, MW Raja Journal of Power Sources 654, 237838 , 2025 2025 Citations: 6
LLZO incorporated dual polymer-based composite electrolyte for enhanced conductivity and long‑term stability for solid‑state lithium‑metal batteries K Ghosh, M Das, MW Raja Journal of Solid State Electrochemistry 30 (1), 121-139 , 2026 2026 Citations: 5
High-Performance Quasi-Solid-State Lithium Metal Batteries: Interface Engineering Using Solid–Liquid Dual Therapy by Solvated Ionic Liquid and NiO K Ghosh, M Das, AK Chaudhary, M Wasim Raja ACS Applied Materials & Interfaces 17 (50), 68052-68073 , 2025 2025
Mg and F Co-Doped Nasicon Solid Electrolyte with Interfacial Liquid Therapy: A Synergistic Approach for High-Performance Sodium Metal Batteries K Ghosh, M Das, M Wasim Raja 247th ECS Meeting (May 18-22, 2025) , 2025 2025
Studies on Advanced Solid Electrolytes for Solid-State Metal Batteries K Ghosh PhD Thesis, Jadavpur University , 2025 2025