@article {48214, title = {MXenes: advances in the synthesis and application in supercapacitors and batteries}, journal = {Journal of Materials Research}, volume = {37}, year = {2022}, month = {NOV}, pages = {3865-3889}, type = {Review}, abstract = {

MXenes, the newest family member of the two-dimensional materials have been widely investigated for different applications, particularly in the energy storage realm. With regard to this, MXene precursors have attained widespread attention for the application in electrochemical energy storage devices especially supercapacitors and batteries. This review has comprehensively studied various synthesis strategies adopted for MXenes including the top-down and bottom-up approaches. The shift to renewable energy alternatives have focused on the electrochemical choices such as supercapacitors and batteries, the most common and relevant ones. Thus the application of MXenes and its composite in supercapacitors as electrodes have been analyzed along with its detailed mechanism and electrochemical performance. Several battery chemistries including lithium-ion, sodium-ion and other battery systems utilizing MXenes have also been discussed here. Thus the existing strategies, advancements, and drawbacks regarding the inclusivity of MXenes in the electrochemical energy systems of supercapacitors and batteries are reviewed in this article.

}, issn = {0884-2914}, doi = {10.1557/s43578-022-00770-4}, author = {Wasnik, Kundan and Pawar, Meenakshi D. and Raphael, Leya Rose and Pullanchiyodan, Abhilash and Shelke, V. Manjusha and Raghavan, Prasanth} } @article {48329, title = {Few-layer graphene lithiophilic and sodiophilic diffusion layer on porous stainless steel as lithium and sodium metal anodes}, journal = {Chemistry-An Asian Journal}, volume = {18}, year = {2023}, month = {APR }, type = {Article}, abstract = {

In order to subdue the obvious problem of uneven electric field distribution on regularly used copper/aluminum current collectors for alkali metal batteries, graphene on porous stainless steel (pSS_Gr) was fabricated using the ion etching technique that is employed as an effective host for lithium and sodium metal anodes. The binder-free pSS_Gr demonstrated stable Li plating and stripping at areal current and capacity of 6 mA cm(-2) and 2.54 mAh cm(-2), respectively, for over 1000 cycles with 98\% coulombic efficiency (C.E.). Also, in the case of Na metal anode, the host has shown stable performance at 4 mA cm(-2) and 1 mAh cm(-2) over 1000 cycles with similar to 100\% C.E.. Further, a full cell composed of Li-plated pSS_Gr as an anode and LiFePO4 as a cathode is electrochemically tested at 50 mA g(-1) current density with stable 100 cycles.

}, keywords = {Few layer graphene, Free-standing, Li and Na metal functional host, Na depth profiles, post-cycling XPS}, issn = {1861-4728}, doi = {10.1002/asia.202300068}, author = {Patrike, Apurva and Wasnik, Kundan and Shelke, Manjusha V.} } @article {48829, title = {High rate, high temperature, dendrite free plating/stripping of Li in 3-dimensional honeycomb boron carbon nitride to realize an ultrastable lithium metal anode}, journal = {Journal of Energy Storage}, volume = {68}, year = {2023}, month = {SEP}, pages = {107547}, type = {Article}, abstract = {

Lithium (Li) metal could be the anode of choice for energy dense Li-batteries owing to its high theoretical specific capacity. However, low coulombic efficiency and poor safety on account of the occurrence of the Li-dendrites during charging-discharging pose a bottleneck for practical applications. In this work, we report a high-rate plating and stripping of Li through host engineering to realize ultrastable Li metal anode (LMA). Benchmark plating/stripping efficiency could be achieved via uniquely structured, highly ordered honeycomb boron carbon nitride (HBCN) as a functional scaffold. Boron and nitrogen doping, large surface area and ordered mesoporous structure induce homogeneous solid electrolyte interface (SEI) layer formation and provide numerous nucleation sites with subsequent dendrite-free growth with 99.98 \% coulombic efficiency at 8 mA cm(-2) high current and 10 mAh cm(-2) capacity over 3000 cycles. Via post-cycling advanced characterizations techniques of Ex-situ XPS, 3D X-ray micro-tomography analyses and FESEM, we demonstrate the formation of a stable SEI layer and morphological changes that occurred during Li plating cycles in the HBCN structure. Computational studies validate the high lithium plating-stripping efficacy of HBCN to its highly ordered porous nature, exothermic Li-binding and upshift in the Fermi levels. When tested at elevated temperature (50 degrees C), a stable Li plating-stripping in HBCN is realised at 4 mA cm(-2) current and 10 mAh cm(-2) capacity values with similar to 100 \% C.E. Furthermore, we report the results of testing a Li metal cell comprised of Li deposited HBCN anode and LiFePO4 (LFP) cathode.

}, keywords = {Boron carbon nitride, Dendrite-free Li metal anode, Functional scaffold, High temperature plating/stripping of Li, Molecular planarity parameter, X-ray micro-tomography}, issn = {2352-152X}, doi = {10.1016/j.est.2023.107547}, author = {Patrike, Apurva and Karbhal, Indrapal and Wasnik, Kundan and Torris, Arun and Maibam, Ashakiran and Krishnamurty, Sailaja and Shelke, V, Manjusha} } @article {49333, title = {PANI-grafted boron, nitrogen co-doped carbon fiber: An outstanding, high-performance supercapacitor electrode}, journal = {JOURNAL OF ENERGY STORAGE}, volume = {96}, year = {2024}, month = {AUG }, pages = {112668}, type = {Journal Article}, keywords = {Composite, polyaniline, Solid-state supercapacitor}, issn = {2352-152X}, doi = {10.1016/j.est.2024.112668}, author = {Nayan, Rajiv and Sinha, Shubhra and Dixit, Vaibhav and Satnami, Manmohan L. and Ghosh, Kallol K. and Pervez, Shamsh and Deb, Manas Kanti and Shrivas, Kamlesh and Rai, Manish K. and Yenchalwar, Sandeep G. and Wasnik, Kundan and Jadkar, Sandesh R. and Karbhal, Indrapal} } @article {49286, title = {Unveiling a promising active host material for sodium metal anodes through V2AlC max derivation}, journal = {ACS Applied Energy Materials}, volume = {7}, year = {2024}, month = {JUL }, pages = {6084-6089}, type = {Article}, abstract = {

To address the issue of nonuniform sodium deposition, in this study, V2ZnC (named VZC), which is synthesized by substituting Zn for Al in V2AlC, is used as a host material to facilitate effective Na utilization. The key concept is to utilize Zn and its forms as an active site to trap Na, while the high mechanical strength of VZC can accommodate volume changes in the sodium metal anode during charging and discharging. VZC displayed regulated plating and stripping at a higher current and capacity of 8 mA cm-2 and 2 mAh cm(-2), respectively, with Coulombic efficiency close to 99.99\%.

}, keywords = {electrodes, Nucleation, overpotential, sodium metal, XPS depth profiling}, issn = {2574-0962}, doi = {10.1021/acsaem.4c01059}, author = {Wasnik, Kundan and Patrike, Apurva and Shelke, Manjusha V.} } @article {49112, title = {Wide temperature enhanced sodium storage in tailored, sustainable sodiophilic biphasic N-doped carbon}, journal = {Materials Today Chemistry }, volume = {37}, year = {2024}, month = {APR}, type = {Article}, abstract = {

Alternative to Li-ion batteries(LIB), Na-ion batteries (NIB) and Na metal batteries (NMB) are gaining significant attention due to their low cost, abundance, and safety. By modulating microstructural properties such as graphitization, heteroatom doping, surface-rich functional groups, and interlayer d-spacing, Na-ion storage in NIB and Na plating/striping in NMB can be ameliorated. This study reports sodiophilic N-doped polymer-derived carbon (PDC) as an anode for NIB and host for Na metal in NMB. As NIB anode, PDC provides a storage capacity of 173 mAh g- 1 at 1 A g- 1 in half-cell and 84 mAh g- 1 at 1C (1C = 128 mAhg- 1) in full-cell with Na3V2(PO4)2F3 (NVPF) cathode. As Na metal anode (NMA) host, a high columbic efficiency (C.E.) of 99.45\% for over 1000 cycles at 6 mA cm- 2_4 mAh cm-2 is obtained. Furthermore, fascinating wide temperature (50 degrees C and -20 degrees C) sodiumion storage is successfully demonstrated by PDC. Advanced X-ray photoelectron spectroscopy (XPS) confirmed the formation of stable and uniform solid electrolyte interphase (SEI) composed of inorganic and organic components, X-ray microtomography confirmed uniform Na plating throughout the volume of the electrode analogous to Brunauer-Emmett-Teller (BET) surface area, Raman spectroscopy, X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) results. A sustainable and scalable promising biphasic NIB anode and sodiophilic host for Na metal was possible due to larger d-spacing, partial graphitization, high mesoporosity, N-doping, presence of surface functional groups, better charge transfer, and diffusion properties.

}, keywords = {Full-cell, Low and elevated temperatures, Na metal host, Polymer-derived carbon, Sodium-ion battery, X-ray tomography}, issn = {2468-5194}, doi = {10.1016/j.mtchem.2024.101978}, author = {Yadav, Poonam and Das, Anoushka K. and Torris, Arun and Wasnik, Kundan and Koppisetti, Heramba Venkata Sai Rama Murthy and Pol, Vilas G. and Shelke, Vilas and Shelke, Manjusha} } @article {49833, title = {Enhanced stability of sodium metal anodes in covalent triazine frameworks via progressive nucleation with optimized conducting composite matrix}, journal = {Small}, volume = {21}, year = {2025}, month = {AUG}, type = {Article}, abstract = {

Organic materials offer exciting possibilities to improve rechargeable battery performance in multiple ways. This study explores the Covalent Triazine Framework (CTF) as an interlayer to modulate progressive sodium nucleation and subsequent recurrent deposition/extraction in an anode-less sodium battery. The optimized composite, C60R40, which combines CTF with reduced graphene oxide (rGO), has demonstrated its effectiveness as a host. In half cell Na electrodeposition, the C60R40 host exhibits 99.9\% coulombic efficiency at an applied current density and areal capacity of 6 mA cm-2 and 2 mAh cm-2, respectively, for 500 cycles. The stable performance is also observed in both full-cell and anode-less battery configurations. When paired with Na3V2(PO4)2F3, the sodium-plated C60R40 demonstrated a stable discharge capacity of 110 mAh g-1. Furthermore, the anode-less sodium battery configuration, with Na3V2(PO4)3 cathode, achieved a promising discharge capacity exceeding 50 mAh g-1 without any additional modifications. These findings highlight the significant role of organic materials in improving the performance of rechargeable sodium metal batteries.

}, keywords = {anode-less batteries, CTF, instantaneous and progressive nucleation, Nucleation and growth, SEI}, issn = {1613-6810}, doi = {10.1002/smll.202502636}, author = {Wasnik, Kundan and Bhatt, Rajesh C. and Shelke, Manjusha V.} } @article {49952, title = {Insights into electrolyte-solvent interactions and SEI formation for sustainable sodium-ion battery operation at low temperatures}, journal = {Small Methods}, volume = {9}, year = {2025}, month = {SEP}, type = {Article}, abstract = {

Sodium-ion batteries (SIBs) show promise as an alternative to lithium-ion batteries. However, they face performance challenges at ultra-low temperatures (\<-40 degrees C) due to slow Na+ transfer kinetics with conventional electrolytes. This limitation restricts their use in extreme environments such as polar regions and outer space. The presented systematic study addresses this challenge by modulating and tailoring the electrolyte composition for SIBs, enabling ultra-low temperature operation down to -110 degrees C for the first time. The comprehensive molecular dynamic and density functional theory calculations combined with experimental Raman spectroscopy and nuclear magnetic resonance studies of advanced electrolytes provided a deeper mechanistic understanding of the solvation structures and their impact on electrochemical performance. By varying the solvent composition with a combination of tetrahydrofuran and 2-Methyltetrahydrofuran solvents and sodium hexafluorophosphate (NaPF6) salt, the freezing point, solubility, and Na+ solvation structure of the electrolyte is modulated and studied in detail. The extensive anion engagement in the optimized mix solvent electrolyte facilitated the formation of a stable and inorganic-rich solid electrolyte interphase layer, ensuring low overpotentials and uniform Na+ deposition, yielding superior cycling stability. As a result, the developed electrolyte enables SIBs to achieve reversible capacities of 88 mAh g(-1) at -60 degrees C and 50 mAh g(-1) at -100 degrees C. These insights may contribute to developing improved energy storage devices suitable for challenging environmental conditions.

}, keywords = {contact-ion pair, solid electrolyte interphase (SEI), solvation, ultra-low temperature, XPS-depth Profiling}, issn = {2366-9608}, doi = {10.1002/smtd.202402142}, author = {Kim, Soohwan and Mirzapure, Vinay and Atwi, Rasha and Koppisetti, Heramba V. S. R. M. and Wasnik, Kundan and Rajput, Nav Nidhi and Shelke, Manjusha and Pol, Vilas G.} } @article {49526, title = {Investigations into the nucleation dynamics of the stable Na-metal anode: revealing the role of a tin-infused carbon nanofiber interlayer}, journal = {ACS Applied Materials \& Interfaces}, volume = {17}, year = {2025}, month = {FEB}, pages = {12281-12290}, type = {Article}, abstract = {

Fundamental understanding and controlling of sodium nucleation are essential for enhancing the performance, safety, and longevity of sodium metal batteries, which is not yet clearly understood in the case of sodium metal batteries. The present study showcases how a modification in the host material influences nucleation kinetics. Current-time transient studies on copper, carbon nanofiber, and tin-embedded carbon nanofiber interlayers employing the Scharifker-Hills model elucidate the mode of nucleation. This work tries to delve deep and presents a case study on how a tin-based interlayer can not only minimize the barrier for sodium nucleation but also direct the sequential progressive and instantaneous nucleation of sodium metal while reducing the overpotential substantially, resulting in crystalline, uniform Na-metal deposition. Further, to account for the complex dynamics of solid electrolyte interphase (SEI) formation distinctly associated with alkali metal deposition, the SEI-fracture model has been included, and the quantification of electrochemical nucleation parameters is obtained. The results provide important insights into the sodium nucleation mechanism, paving the way to counter dendrite formation and SEI dissolution issues of the Na-metal anode.

}, keywords = {overpotential, progressiveand instantaneous nucleation, Scharifker-Hills model, SEI-fracture model, tin interlayer}, issn = {1944-8244}, doi = {10.1021/acsami.4c21837}, author = {Wasnik, Kundan and Yadav, Poonam and Ahuja, Manuj and Mirzapure, Vinay and Johari, Priya and Shelke, Manjusha V.} }