Faculty Publications
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Item Advanced Electrolyte Additives for Lithium-Ion Batteries: Classification, Function, and Future Directions(American Chemical Society, 2025) Brijesh, K.; Jareer, M.; Lakshmi Sagar, G.; Mukesh, P.; Alagarsamy, A.; Mandal, D.; Nagaraja, H.S.; Shahgaldi, S.Lithium-ion batteries (LIBs) are widely employed as energy storage devices, particularly in portable electronics and electric vehicles, owing to their high energy density and efficiency. Among the key components of LIBs, the electrolyte plays a crucial role in determining capacity, cycling stability, rate performance, the electrode/electrolyte interface, and overall battery efficiency. However, traditional electrolytes face significant challenges, including severe structural degradation and interfacial side reactions under high-voltage and high-temperature conditions. Protective layers, such as the cathode-electrolyte interphase (CEI) and solid-electrolyte interphase (SEI), are essential for addressing these issues. These layers inhibit electron transfer while allowing lithium-ion (Li+) transport, preserving the structural and electrochemical integrity of the battery. A cost-effective strategy to further enhance the electrode-electrolyte interface and boost LIB performance is the incorporation of carefully designed electrolyte additives. While some articles discuss the use of electrolyte additives in LIBs, there is a lack of detailed studies classifying these additives based on their chemical composition-based grouping. Such a classification enables a more focused examination of the roles and mechanisms by which these additives improve LIB performance. This review paper bridges this gap by examining various electrolyte additives and their contributions to enhancing the safety and performance of next-generation LIBs. It provides valuable insights into the current progress and challenges associated with additives in liquid electrolytes. The article is organized into seven sections, addressing boron-based electrolyte additives (Section 2), sulfur-based electrolyte additives (Section 3), phosphorus-based electrolyte additives (Section 4), fluorine-based electrolyte additives (Section 5), and nitrogen-based electrolyte additives (Section 6). Each section discusses specific examples, the formation of SEI and CEI layers, and the electrochemical properties of these additives. Furthermore, the article concludes with a summary and outlook, advocating for continued advancements in electrolyte engineering for LIBs. © 2025 American Chemical Society.Item Enhanced Electrochemical Performance of Low-Content Graphene Oxide in Porous Co3O4 Microsheets for Dual Applications of Lithium-Ion Battery Anode and Lithium-Ion Capacitor(Springer, 2024) Lakshmi Sagar, G.; Brijesh, K.; Mukesh, P.; Amudha, A.; Bhat, K.S.; Nagaraja, H.S.The enhancement of electrochemical performance in lithium-ion battery (LIB) anode materials through nanostructures is of paramount importance, facilitated by the synergistic integration of these unique architectures with active materials, which increases the availability of active sites and decreases the diffusion path for lithium ions. In this investigation, we successfully synthesized cobalt oxide (Co3O4) microsheets composed of small nanoparticles (measuring 28–33 nm), employing a straightforward hydrothermal process followed by annealing. Furthermore, to enhance the composite’s ability to endure volume changes and increase its electrical conductivity, we created a Co3O4/reduced graphene oxide (rGO) composite embedding a judicious amount of graphene oxide (GO). This engineered composite exhibited remarkable specific discharge capacity of 1081 mAh g−1 at 100 mA g−1, a substantial improvement over the pristine material’s capacity of 718 mAh g−1. The composite demonstrated reduced irreversible capacity loss relative to the pristine counterpart and approached a reversible capacity of nearly 99%. Even after 400 cycles under the demanding conditions of high current density of 500 mA g−1, the composite managed to retain 81% of its initial capacity, underscoring its exceptional cycling stability. Moreover, the application of the Co3O4/rGO//carbon black (CB) assembly in lithium-ion capacitors (LIC) yielded notable energy density of 15.6 Wh kg−1 at elevated power density of 1007 W kg−1. These LIC devices demonstrated robust cyclic stability across extended cycles, sustaining 56% of their initial capacity after 2000 cycles while operating at a current density of 2 A g−1. Graphical Abstract: [Figure not available: see fulltext.]. © 2024, The Minerals, Metals & Materials Society.Item Impact of copper doping on the electrochemical response of MnSe2 as anode for lithium-ion battery(Springer, 2024) Mukesh, P.; Lakshmi Sagar, G.; Brijesh, K.; Kumawat, S.; Hegde, A.; Kumar, A.; Nagaraja, H.S.Transition Metal Chalcogenides (TMC), due to their unique physicochemical properties, are studied in various fields and have potent applications in energy storage applications. This work is based on the synthesis and characterization of copper-doped manganese di-selenide and the effect of its doping on electrochemical performance as anode material for lithium-ion battery applications using the solvothermal method. The characterization techniques used are X-ray diffraction, Raman spectroscopy, field-emission scanning electron microscopy, XPS, UV–visible absorption spectroscopy, and electrochemical analysis. The XRD data confirms the formation of MnSe2 exhibiting Cubic crystal geometry. The FESEM images show the micro-cube-like structure with agglomerated nanocluster nanostructures on the surface with a dimension of 100–200 nm. The doping of the copper has decreased the band gap of the MnSe2, as studied by the UV–visible absorption spectrum. The electrochemical performance is analyzed as anode material for lithium-ion batteries. The charge/discharge measurements show a specific capacity of 706 mAh g−1 as the initial discharge capacity and 336 mAh g−1 as the initial charge capacity at 0.1 A g−1 current density. Meanwhile, 3% Copper-doped MnSe2 showed a better specific capacity of 878 mAh g−1 as the initial discharge capacity and 461 mAh g−1 as the initial charge capacity at 0.1 A g−1 current density. Cyclic stability, rate capability, and electrochemical impedance spectroscopy were performed, and it shows that 3% copper-doped MnSe2 has good stability and better conductivity and charge kinetics, indicating copper doping has enhanced the electrochemical performance of pristine MnSe2. © The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature 2024.Item Nano-composites of NiFe-LDH/V Se2 heterostructures for effective water splitting electrocatalyst(Elsevier Ltd, 2024) Hegde, A.; Mukesh, P.; G, L.S.; Kumar, A.; Nagaraja, H.S.In the realm of sustainable and environmentally friendly “green-hydrogen” fuel demand, water electrolysis stands as a pathway of hope for the extraction of renewable hydrogen. However, the durability and efficiency of electrocatalysts have been a major challenge in this process, owing to factors like the high costs of noble catalysts (Pt, Ir, Ru, etc.) and their limited stability. Layered Nickel-iron double hydroxides (NiFe-LDH) have shown potential as low-cost and efficient electrocatalysts because of their suitable electronic configuration and distinguished orbital confinement. However, their durability In the realm of sustainable and environmentally friendly “green-hydrogen” fuel demand, water electrolysis stands as a pathway of hope for the extraction of renewable hydrogen. However, the durability and efficiency of electrocatalysts have been a major challenge in this process, owing to factors like the high costs of noble catalysts (Pt, Ir, Ru, etc.) and their limited stability. Layered Nickel-iron double hydroxides (NiFe-LDH) have shown potential as low-cost and efficient electrocatalysts because of their suitable electronic configuration and distinguished orbital confinement. However, their performance and durability in corrosive alkaline water at high current density remain limited. In this regard, one can make the nano-composites of this NiFe-LDH with high electronic conductivity materials and layered structures like VSe2. With this motivation, this work presents a novel electrocatalyst, NiFe-LDH, supported with VSe2 nanosheets (V Se2/NiFe−LDH), designed to address these challenges and enhance water splitting efficiency. Experimental results demonstrate that the heterostructure synergistically reduces charge transfer resistance, increases exposure of active sites, and enhances oxygen gas evolution ability. Consequently, the V Se2/NiFe−LDH electrocatalyst demonstrated superior sustainability, maintaining an elevated current density (500mAcm−2) for over 50 h of continuous electrolysis without noticeable degradation. This research opens up new possibilities and shows that nano-compositing can be a good option for achieving efficient and durable electrocatalysts in alkaline water splitting, thereby contributing to sustainable hydrogen production. © 2024 Hydrogen Energy Publications LLCItem Synergistic boost in Fe3O4 anode performance for li-ion batteries via Zn and Cu double doping and multi-walled carbon nanotube composite integration(Elsevier B.V., 2024) Kumar, A.; Mukesh, P.; Lakshmi Sagar, G.; Hegde, A.; Nagaraja, H.S.In this study, a novel nanocomposite material comprising pure Fe3O4 (FO), doped Zn0.5Cu0.5Fe2O4-3 (ZCFO-3), and Zn0.5Cu0.5Fe2O4-3@ Multi-walled carbon nanotube (ZCFO-3@MWCNT) nanocomposite material is carefully prepared using a simple one-step hydrothermal process. Comprehensive surface and morphological analysis are conducted using X-ray diffraction (XRD), Field emission scanning electron microscopy (FESEM), and High-resolution transmission electron microscopy (HRTEM), while compositional studies are investigated through Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). The electrochemical performance is fully analyzed through Cyclic voltammetry (CV), Electrochemical impedance spectroscopy (EIS), rate capability tests, discharge/charge capacity, and cyclic stability evaluations. Among these three nanomaterials, ZCFO-3@MWCNT nanocomposite at 100 mA g−1 current density reveals the best performance, with a discharge capacity of 1974 mAh g–1, ZCFO-3 and FO reveal 1340 mAh g–1 and 1317 mAh g–1 respectively. After 800 cycles at 500 mA g−1 current density, ZCFO-3@MWCNT stays strong with a discharge capacity of 646 mAh g–1, while ZCFO-3 manages only 362 mAh g–1 and FO only 111 mAh g–1. After 1200 cycles at 500 mA g−1, the nanocomposite still delivers 518 mAh g–1. This study suggests that ZCFO-3@MWCNT could be a promising anode material for lithium-ion batteries. © 2024 Elsevier B.V.Item Dual storage mechanism of Bi2O3/Co3O4/MWCNT composite as an anode for lithium-ion battery and lithium-ion capacitor(Elsevier B.V., 2024) Lakshmi Sagar, G.; Brijesh, K.; Mukesh, P.; Hegde, A.P.; Kumar, A.; Kumar, A.; Bhat, K.S.; Nagaraja, H.S.Bismuth oxide(Bi2O3) and cobalt oxide(Co3O4) are promising owing to their unique properties, high storage capacity, low cost, and eco-friendliness, making them ideal for lithium-ion batteries(LIBs) and lithium-ion capacitors(LICs) anodes. This study presents the synthesis and thorough characterization of Bi2O3/Co3O4 and Bi2O3/Co3O4/MWCNT composites as potential LIB and LIC anode materials. The materials are synthesized using a hydrothermal process succeeded by annealing. Structural, morphological, and compositional studies were analyzed. Various tests evaluated electrochemical performance, including cyclic voltammetry(CV), confirming a dual storage mechanism like alloying and conversion reaction involved for better energy storage. Specific discharge capacities of 834 mAh/g and 1184 mAh/g were recorded for Bi2O3/Co3O4 and Bi2O3/Co3O4/MWCNT composite electrodes at a current density of 100 mA/g, respectively. The composite material exhibited notably enhanced rate capability, with 31 % and 51 % discharge capacities for Bi2O3/Co3O4 and Bi2O3/Co3O4/MWCNT, respectively. The cyclic stability assessment revealed that Bi2O3/Co3O4 and Bi2O3/Co3O4/MWCNT maintained a high coulombic efficiency of around 99 % over 250 charge–discharge cycles at a high current density of 1 A/g. The capacity retention was approximately 253 mAh/g for Bi2O3/Co3O4 and 439 mAh/g for the Bi2O3/Co3O4/MWCNT composite, indicating excellent cyclic stability and minimal energy loss during cycling. Moreover, the LICs assembly of Bi2O3/Co3O4/MWCNT//CB was investigated, revealing a power density of 200 W kg?1 alongside an energy density of 8.64 Wh kg?1. The cyclic stability assessment over 10,000 cycles exhibits a capacity retention of approximately 45 % under a high current density of 2 A/g. © 2024 Elsevier B.V.Item Cerium doping of FeS2 for the effective hydrogen evolution reaction (HER) electrocatalysis(Taylor and Francis Ltd., 2025) Hegde, A.P.; Gonde, A.; Kumawat, A.; Mukesh, P.; Lakshmisagar, G.; Kumar, A.; Nagaraja, H.S.Crafting and developing nanostructured electrocatalyst materials that are both active and stable plays a pivotal role in the shift toward economically viable hydrogen production through electrochemical water splitting, paving the way for the future replacement of fossil fuels. Such materials need to be cost-effective, simple to produce, and durable. In this context, the current research delves into improving the hydrogen evolution reaction (HER) electrocatalytic performance by incorporating cerium (Ce) into iron disulfide (FeS2) catalysts, using an uncomplicated hydrothermal fabrication approach. The study systematically examines the effects of various Ce doping levels on electrocatalytic activity. Notably, the catalyst with 15% Ce doping demonstrated exceptional efficiency, reducing the overpotential to 369 mV at 100 mA cm?2 current density. This enhanced performance can be attributed to the reduction in total charge-transfer resistance and a significant increase in the electrochemical active surface area (ECSA). Furthermore, the durability assessment of the 15% Ce-doped sample revealed its ability to sustain its catalytic activity for over 100 h under a continuous HER operation at 300 mA cm-2, with low performance-falloff. These results highlight the potential of Ce-dopping of FeS2 catalysts as a formidable choice for achieving efficient and long lasting HER electrocatalysis. © 2025 Taylor & Francis Group, LLC.Item Enhancing conductivity of Bi2O3 through ‘Fe3+’ doping for pseudocapacitor application(Springer Science and Business Media Deutschland GmbH, 2025) G, L.S.; Bhat, K.S.; Mukesh, P.; Hegde, A.P.; Kumar, A.; Brijesh, K.; Nagaraja, H.S.Binary metal oxides have emerged as pSromising materials for advanced electrochemical energy storage systems due to their superior performance characteristics. In this study, we focus on bismuth oxide (Bi?O?), a material renowned for its high theoretical capacity, wide potential range, and exceptional power density, as a potential candidate for supercapacitors. Iron doping was employed as a strategy to enhance its electrochemical performance and modulate the band gap, thereby improving conductivity and charge storage efficiency. Fe-doped bismuth oxide (Fe-Bi?O?) was synthesized via a solvothermal method with varying iron concentrations (2%, 4%, and 6%), followed by annealing. The pure and iron-doped bismuth oxide samples revealed a combination of monoclinic and cubic phases and a prominent micro-sheet architecture. The introduction of iron doping led to a noticeable reduction in the band gap, highlighting its role in fine-tuning the electronic properties for enhanced energy storage capabilities. The electrochemical evaluation highlighted the 4% Fe-Bi?O? sample as the optimal composition, achieving a remarkable specific capacity of 904 F g?1, a substantial improvement over 101 F g?1 for pristine Bi?O?, at 1 A g?1 in a 2 M KOH electrolyte. Moreover, this sample exhibited outstanding cyclic stability, retaining 104 F g?1 after 2000 cycles at 10 A g?1. © The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2025.Item Reinforcing NiO microsphere structural stability via amorphous carbon sheets obtained from waste milk for lithium-ion capacitor application(Springer Science and Business Media B.V., 2025) Lakshmi Sagar, G.; Brijesh, K.; Mukesh, P.; Hegde, A.P.; Kumar, A.; Paliwal, A.; Bhat, K.S.; Nagaraja, H.S.In the pursuit of sustainable chemistry and environmentally friendly energy storage, the study addressed the limitations of nickel oxide utilized as the active material for the anode in lithium-ion capacitors. Despite its abundance and favorable environmental properties, NiO suffered from significant volumetric expansion and slow electrochemical kinetics compared to carbon materials. To overcome these issues, amorphous carbon was extracted from spoiled waste milk through a simple combustion process, effectively converting biomass waste into renewable resources. The engineered NiO/amorphous carbon composite, synthesized through hydrothermal and annealing processes, mitigated the limitations of NiO. Field Emission Scanning Electron Microscopy confirmed the deposition of amorphous carbon sheets encasing NiO microspheres, which preserved structural integrity during electrochemical cycling. The amorphous carbon acted as a stabilizing matrix, encapsulating NiO microspheres to mitigate volumetric expansion and enhance lithium-ion transport kinetics. Electrochemical tests demonstrated a specific discharge capacity of 1230 mAh g?1 at a current density of 100 mA g?1, retaining 401 mAh g?1 after 1000 cycles at 1 A g?1, nearly doubling the retention performance of pristine NiO. Furthermore, the NiO/AC//AC lithium-ion capacitor achieved an energy density of 25.4 Wh kg?1 at a power density of 1991 W kg?1, maintaining 96% capacity after 3500 cycles. This study highlighted the potential of waste-derived carbon in developing high-performance, sustainable energy storage systems. © The Author(s), under exclusive licence to Springer Nature B.V. 2025.