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.
Advanced Sustainable Trilayer Cellulosic “Paper Separator” Functionalized with Nano-BaTiO3 for Applications in Li-Ion Batteries and Supercapacitors Mononita Das, Pradip Sekhar Das, Nimai Chand Pramanik, Rajendra Nath Basu, Mir Wasim Raja ACS Omega, 2023 In the quest of developing a sustainable, low-cost and improved separator membrane for application in energy storage devices like lithium-ion batteries (LIBs) and supercapacitors (SCs), here we fabricated a trilayer cellulose-based paper separator engineered with nano-BaTiO3 powder. A scalable fabrication process of the paper separator was designed step-by-step by sizing with poly(vinylidene fluoride) (PVDF), thereafter impregnating nano-BaTiO3 in the interlayer using water-soluble styrene butadiene rubber (SBR) as the binder and finally laminating the ceramic layer with a low-concentration SBR solution. The fabricated separators showed excellent electrolyte wettability (216–270%), quicker electrolyte saturation, increased mechanical strength (43.96–50.15 MPa), and zero-dimensional shrinkage up to 200 °C. The electrochemical cell comprising graphite|paper separator|LiFePO4 showed comparable electrochemical performances in terms of capacity retention at different current densities (0.05–0.8 mA/cm2) and long-term cycleability (300 cycles) with coulombic efficiency >96%. The in-cell chemical stability as tested for 8 weeks revealed a nominal change in bulk resistivity with no significant morphological changes. The vertical burning test as performed on a paper separator showed excellent flame-retardant property, a required safety feature for separator materials. To examine the multidevice compatibility, the paper separator was tested in supercapacitors, delivering a comparable performance to that of a commercial separator. The developed paper separator was also found to be compatible with most of the commercial cathode materials such as LiFePO4, LiMn2O4, and NCM111.
Paperator: The Paper-Based Ceramic Separator for Lithium-Ion Batteries and the Process Scale-Up Strategy Mir Wasim Raja, Rajendra Nath Basu, Nimai Chand Pramanik, Pradip Sekhar Das, Mononita Das ACS Applied Energy Materials, 2022 Due to its flexibility, cost-effectiveness, and natural abundance, paper has become a material of choice for its targeted applications in electronic and optoelectronic devices. With an aim to develop a paper-based ceramic separator (henceforth will be referred to as paperator), a low-cost paper substrate sourced from the local market has been functionalized by the wet-coating method using duo-polymer (chitosan and polyvinyl alcohol) and ceramic (BaTiO3) nanopowder. The developed paperator shows excellent air permeability, improved thermal stability of up to 200 °C without dimensional shrinkage, quicker wettability to an electrolyte, and comparable electrochemical performance to that of polypropylene-based commercial separator. The modification of the paper substrate using polymer and ceramic particles has also improved the tensile strength of the paperator to a maximum value of 45.23 MPa w.r.t. 28.20 MPa for pristine paper. The electrochemical performance of the developed paperators shows satisfactory cell performance at different current densities with excellent coulombic efficiency and comparable discharge capacities with that of a commercial separator. Compared to the commercial PP-based membrane, slightly lowered discharge capacities are obtained from the cells fabricated with developed paperators, which may primarily be due to the higher thickness (60/70 μm) and cellulosic tortuosity. Electrochemical performances of the developed “paperators” were also evaluated for use in supercapacitors (SCs) by fabricating SC cells and their testing as per IEC 62391-1, which showed the cell capacitance and ESR values of 17.2 ± 0.8 F and 76 ± 3 mΩ, respectively, and the results were also compared with those of commercial cellulose-based paper separators. Based on the R&D achievements, the present study has also been extended for a scale-up strategy to produce a paper-based separator in roll form, where a “paperator” of 60 mm in width in a continuous manner has been fabricated by using in-house-designed semi-automated double-decker separator fabricator machine.
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, 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, MW Raja 247th ECS Meeting (May 18-22, 2025) , 2025 2025
Development of cellulose-based composite separator membranes for energy storage devices M Das Jadavpur University, Kolkata, West Bengal , 2025 2025
Flexible trilayer cellulosic paper separators engineered with the BaTiO 3 ferroelectric fillers for high energy density sodium-ion batteries SK Sapra, M Das, MW Raja, JK Chang, RS Dhaka Journal of Materials Chemistry A 13 (3), 1996-2009 , 2025 2025 Citations: 13
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
Advanced Sustainable Trilayer Cellulosic “Paper Separator” Functionalized with Nano-BaTiO 3 for Applications in Li-Ion Batteries and Supercapacitors M Das, PS Das, NC Pramanik, RN Basu, M Wasim Raja ACS omega 8 (23), 21315-21331 , 2023 2023 Citations: 21
Cellulose-ceramic composite flexible paper separator with improved wettability and flame retardant properties for lithium-ion batteries M Das, PS Das, RN Basu, MW Raja Cellulose 29 (18), 9899-9917 , 2022 2022 Citations: 15
Paperator: the paper-based ceramic separator for lithium-ion batteries and the process scale-up strategy MW Raja, RN Basu, NC Pramanik, PS Das, M Das ACS Applied Energy Materials 5 (5), 5841-5854 , 2022 2022 Citations: 18
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
Advanced Sustainable Trilayer Cellulosic “Paper Separator” Functionalized with Nano-BaTiO 3 for Applications in Li-Ion Batteries and Supercapacitors M Das, PS Das, NC Pramanik, RN Basu, M Wasim Raja ACS omega 8 (23), 21315-21331 , 2023 2023 Citations: 21
Paperator: the paper-based ceramic separator for lithium-ion batteries and the process scale-up strategy MW Raja, RN Basu, NC Pramanik, PS Das, M Das ACS Applied Energy Materials 5 (5), 5841-5854 , 2022 2022 Citations: 18
Cellulose-ceramic composite flexible paper separator with improved wettability and flame retardant properties for lithium-ion batteries M Das, PS Das, RN Basu, MW Raja Cellulose 29 (18), 9899-9917 , 2022 2022 Citations: 15
Flexible trilayer cellulosic paper separators engineered with the BaTiO 3 ferroelectric fillers for high energy density sodium-ion batteries SK Sapra, M Das, MW Raja, JK Chang, RS Dhaka Journal of Materials Chemistry A 13 (3), 1996-2009 , 2025 2025 Citations: 13
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, 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, MW Raja 247th ECS Meeting (May 18-22, 2025) , 2025 2025
Development of cellulose-based composite separator membranes for energy storage devices M Das Jadavpur University, Kolkata, West Bengal , 2025 2025