@article{sarkar_mukherjee_2024, title={Probing Asymmetric Plating and Stripping Behavior of Symmetric Sodium Metal Batteries}, volume={1}, ISSN={["1543-1851"]}, url={https://doi.org/10.1007/s11837-023-06359-4}, DOI={10.1007/s11837-023-06359-4}, journal={JOM}, author={Sarkar, Susmita and Mukherjee, Partha P.}, year={2024}, month={Jan} } @article{sarkar_lefler_vishnugopi_nuwayhid_love_carter_mukherjee_2023, title={Fluorinated ethylene carbonate as additive to glyme electrolytes for robust sodium solid electrolyte interface}, url={http://dx.doi.org/10.1016/j.xcrp.2023.101356}, DOI={10.1016/j.xcrp.2023.101356}, abstractNote={The utilization of alkali metal anodes is hindered by an inherent instability in organic electrolytes. Sodium is of growing interest due to its high natural abundance, but the carbonate electrolytes popular in lithium systems cannot form a stable solid electrolyte interphase (SEI) with a sodium electrode. Using half-cell and symmetric-cell analysis, we identify specific glyme (chain ether) electrolytes that produce thin, predominantly inorganic SEI at the sodium metal interface, and we study the effect of ethylene carbonate and fluoroethylene carbonate (FEC) additives on the SEI formed in these systems via X-ray photoelectron spectroscopy. Through in situ optical microscopy, we observe the onset and growth of sodium dendrites in these electrolytes. We determine that the SEI formed by glyme alone may not support extensive or extreme cycling conditions, but the addition of FEC provides a more robust SEI to facilitate numerous consistent sodium plating and stripping cycles.}, journal={Cell Reports Physical Science}, author={Sarkar, Susmita and Lefler, Matthew J. and Vishnugopi, Bairav S. and Nuwayhid, R. Blake and Love, Corey T. and Carter, Rachel and Mukherjee, Partha P.}, year={2023}, month={Apr} } @article{sarkar_chatterjee_goswami_mukherjee_2022, title={Celebrating Women in Electrochemical Sciences and Engineering (WIESE)}, url={http://dx.doi.org/10.1021/acsenergylett.2c01026}, DOI={10.1021/acsenergylett.2c01026}, abstractNote={ADVERTISEMENT RETURN TO ISSUEPREVEnergy FocusNEXTCelebrating Women in Electrochemical Sciences and Engineering (WIESE)Susmita SarkarSusmita SarkarSchool of Mechanical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Susmita Sarkar, Debanjali ChatterjeeDebanjali ChatterjeeSchool of Mechanical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Debanjali Chatterjee, Navneet GoswamiNavneet GoswamiSchool of Mechanical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Navneet Goswami, and Partha P. Mukherjee*Partha P. MukherjeeSchool of Mechanical Engineering, Purdue University, West Lafayette, Indiana 47907, United States*Email: [email protected]More by Partha P. Mukherjeehttps://orcid.org/0000-0001-7900-7261Cite this: ACS Energy Lett. 2022, 7, 6, 2105–2112Publication Date (Web):May 27, 2022Publication History Received2 May 2022Accepted9 May 2022Published online27 May 2022Published inissue 10 June 2022https://doi.org/10.1021/acsenergylett.2c01026Copyright © Published 2022 by American Chemical SocietyRIGHTS & PERMISSIONSArticle Views1937Altmetric-Citations-LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.Citations are the number of other articles citing this article, calculated by Crossref and updated daily. 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Share Add toView InAdd Full Text with ReferenceAdd Description ExportRISCitationCitation and abstractCitation and referencesMore Options Share onFacebookTwitterWechatLinked InReddit PDF (9 MB) Get e-AlertsSUBJECTS:Batteries,Electrical energy,Electrodes,Electrolytes,Students Get e-Alerts}, journal={ACS Energy Letters}, author={Sarkar, Susmita and Chatterjee, Debanjali and Goswami, Navneet and Mukherjee, Partha}, year={2022}, month={Jun} } @article{luo_bai_mistry_zhang_zhao_sarkar_handy_rezaei_chuang_carrillo_et al._2022, title={Effect of crystallite geometries on electrochemical performance of porous intercalation electrodes by multiscale operando investigation}, url={https://doi.org/10.1038/s41563-021-01151-8}, DOI={10.1038/s41563-021-01151-8}, journal={Nature Materials}, author={Luo, Yuting and Bai, Yang and Mistry, Aashutosh and Zhang, Yuwei and Zhao, Dexin and Sarkar, Susmita and Handy, Joseph V. and Rezaei, Shahed and Chuang, Andrew Chihpin and Carrillo, Luis and et al.}, year={2022}, month={Feb} } @article{sarkar_malabet_flannagin_alex_shevchenko_nelson_mukherjee_2022, title={Multiscale Electrochemomechanics Interaction and Degradation Analytics of Sn Electrodes for Sodium-Ion Batteries}, url={http://dx.doi.org/10.1021/acsami.2c02772}, DOI={10.1021/acsami.2c02772}, abstractNote={Sodium-ion batteries have emerged as a strong contender among the beyond lithium-ion chemistries due to elemental abundance and the low cost of sodium. Tin (Sn) is a promising alloying electrode with high capacity, redox reversibility, and earth abundance. Tin electrodes, however, undergo a series of intermediate reactions exhibiting multiple voltage plateaus upon sodiation/desodiation. Phase transformations related to incomplete sodiation in tin during cycling, in the presence of a frail solid electrolyte interphase layer, can quickly weaken the structural stability. The structural dynamics and reactivity of the electrode/electrolyte interface, being further dependent on the size and morphology of the active material particle in the presence of different electrolytes, dictate the electrode degradation and survivability during cycling. In this study, we paint a comprehensive picture of the underpinnings of the electrochemical and mechanics coupling and electrode/electrolyte interfacial interactions in alloying Sn electrodes. We elicit the fundamental role of electrode/electrolyte complexations in the Sn electrode structure-property-performance relationship based on multimodal analytics, including electrochemical, microscopy, and tomography analyses.}, journal={ACS Applied Materials & Interfaces}, author={Sarkar, Susmita and Malabet, Hernando Gonzalez and Flannagin, Megan and Alex, L’Antigua and Shevchenko, Pavel D. and Nelson, George and Mukherjee, Partha}, year={2022}, month={Jul} } @article{rangarajan_sarkar_barsukov_mukherjee_2021, title={3ε–A Versatile Operando Analytics Toolbox in Energy Storage}, url={http://dx.doi.org/10.1021/acsomega.1c05494}, DOI={10.1021/acsomega.1c05494}, abstractNote={The performance and safety of lithium-ion batteries are plagued by several diverse, nonlinear aging mechanisms influenced by the electrochemical thermal interactions at the electrodes, usage history, and operating conditions. Understanding and deconvoluting the fundamental reaction mechanisms responsible for electrode degradation are key for developing technologies in Li-ion battery diagnostics and prognostics. Hence, there exists a need for high-precision operando techniques to investigate and characterize distinct electrode degradation modes over a gamut of operational variability. Cells embedded with a stable, nonpolarizable reference electrode offer an in situ and operando tool to decouple the complex electrochemical interplay between the electrode pair by measuring individual electrode responses simultaneously with the cell response in the time and frequency domains. This perspective comprehensively looks at 3-electrode (3ε) analytics as a versatile toolbox, highlighting recent techniques and parameters developed with an emphasis on degradation diagnostics and control strategies that is expected to drive the futuristic design of battery management systems.}, journal={ACS Omega}, author={Rangarajan, Sobana P. and Sarkar, Susmita and Barsukov, Yevgen and Mukherjee, Partha}, year={2021}, month={Dec} } @article{sarkar_hoffmann_park_2021, title={Micro-macroscopic modeling of a lithium-ion battery by considering grain boundaries of active materials}, url={http://dx.doi.org/10.1016/j.electacta.2021.139052}, DOI={10.1016/j.electacta.2021.139052}, abstractNote={Many important properties of electrode materials are profoundly sensitive to deviations from the crystalline perfection. Among them are grain boundaries, which play an important role on battery performance by altering the distributions of ions inside the particles and changing the corresponding stress level. This paper explores the mechanical and microstructural aspects of battery behavior by developing a cell-level model that incorporates grain boundary diffusion in the electrode particles for the anode and cathode. The developed model is compared against a grainless model at various operating conditions to understand how grain boundaries influence capacity and stress generation. The results from the model revealed that the location of the maximum stress might not necessarily occur at the separator interface at any given time as the particles with heterogeneous diffusion paths displayed gradual changes in flux profile, which has just been believed in practice. The grain structure geometry variability showed that less diffusive particles at the rear side endure more stress than high diffusive frontal particles. Also, the results show an appreciable effect of grain boundary diffusion on the voltage profile of the cell for the tested parameters and, overall, a significant reduction in the maximum induced stress in the cell. Stress behavior between the anode and cathode differ significantly and show that the effective diffusivity of a particle might matter much more significantly than its location in the cell. With heterogeneous particle shape modeling capabilities, this approach can be next-generation battery model that improves understanding of battery materials and electrodes.}, journal={Electrochimica Acta}, author={Sarkar, Susmita and Hoffmann, John Alexander and Park, Jonghyun}, year={2021}, month={Oct} } @article{sarkar_verma_mukherjee_2021, title={Quantifying Sodiation Kinetics in Alloying Tin Electrodes for Sodium-Ion Batteries}, volume={168}, url={https://doi.org/10.1149/1945-7111/ac2708}, DOI={10.1149/1945-7111/ac2708}, abstractNote={Sodium-ion batteries (SIBs) are promising next-generation energy storage devices because of the elemental abundance and low sodium cost. However, the lower storage capacity and short lifespan of SIBs necessitate the need for a fundamental understanding of the sodiation/de-sodiation kinetics complexation due to the inherent electrode materials and electrolyte interactions. This study comprehensively studied the kinetics of the sodium alloying and de-alloying mechanism in tin (Sn) electrodes, a promising anode, relying on GITT-based (galvanostatic intermittent titration technique) analytics. This study includes a limited combinatorial analysis of sodium salts, namely, NaPF6 and NaClO4, in conjunction with different carbonate solvents. This comprehensive analysis elicits a comparative paradigm of diffusivity, charge transfer resistance, intercalation rate constant, and exchange current density for the salt/solvent combinations. Overall, NaClO4 exhibits better kinetic and transport properties as compared to NaPF6. This study further elucidates the variation of ionic mobility and reaction rate with interfacial passivation due to excess fluorine donation from additives. The effect of active particle size reveals that nanoparticles exhibit reduced electrochemical (charge/discharge) hysteresis than microparticles. Overall, this study demonstrates a more considerable sensitivity of the charge transfer resistance, exchange current density, and reaction rate constants compared to the diffusivity.}, number={9}, journal={Journal of The Electrochemical Society}, publisher={The Electrochemical Society}, author={Sarkar, Susmita and Verma, Ankit and Mukherjee, Partha P.}, year={2021}, month={Sep}, pages={090550} } @article{sarkar_mukherjee_2021, title={Synergistic voltage and electrolyte mediation improves sodiation kinetics in µ-Sn alloy-anodes}, url={http://dx.doi.org/10.1016/j.ensm.2021.09.014}, DOI={10.1016/j.ensm.2021.09.014}, abstractNote={Alloying electrodes, such as tin (Sn), are promising candidates for sodium-ion batteries because of their high specific capacity, electronic conductivity, and low sodium insertion voltage. However, sizeable volumetric change and electrode-electrolyte interface evolution in Sn preclude prolonged performance. The electrochemical potential window, compounded by the choice of electrolyte and additive combination, plays a critical role in the interface instability, which yet remains unresolved. This study, based on a comprehensive set of electrochemical, microscopy, and spectroscopic analyses, sheds light into the interface instability and reveals that the use of fluoroethylene carbonate additives in carbonate-based electrolytes can dramatically improve the interface stability of such alloying anodes. Electrochemical and morphological analyses show that without the additive, a higher end-of-charge voltage can cause breakdown and reformation of an unstable passivating layer, leading to rapid electrochemical performance decay. A novel three-electrode-based analytics reveals that superior interphase stability with higher microstructural integrity of the Sn electrode can alleviate the detriments from the upper cut-off voltage restrictions. Addressing the hitherto unresolved role of the electrochemical potential window, this study comprehensively examines and elucidates the causality of interfacial instability and the underpinnings of electrochemical complexations in sodium-alloying anodes.}, journal={Energy Storage Materials}, author={Sarkar, Susmita and Mukherjee, Partha P.}, year={2021}, month={Dec} } @article{he_pham_gao_patel_sarkar_liang_park_2020, title={Discovery of an Unexpected Metal Dissolution of Thin‐Coated Cathode Particles and Its Theoretical Explanation}, url={http://dx.doi.org/10.1002/adts.202000002}, DOI={10.1002/adts.202000002}, abstractNote={Abstract}, journal={Advanced Theory and Simulations}, author={He, Yufang and Pham, Hiep and Gao, Yan and Patel, Rajankumar L. and Sarkar, Susmita and Liang, Xinhua and Park, Jonghyun}, year={2020}, month={May} } @article{yu_liu_pham_sarkar_ludwig_chen_everhart_park_wang_pan_2019, title={Customizable Nonplanar Printing of Lithium‐Ion Batteries}, url={http://dx.doi.org/10.1002/admt.201900645}, DOI={10.1002/admt.201900645}, abstractNote={Abstract}, journal={Advanced Materials Technologies}, author={Yu, Xiaowei and Liu, Yangtao and Pham, Hiep and Sarkar, Susmita and Ludwig, Brandon and Chen, I‐Meng and Everhart, Wesley and Park, Jonghyun and Wang, Yan and Pan, Heng}, year={2019}, month={Nov} } @article{sarkar_patel_liang_park_2017, title={Unveiling the Role of CeO2 Atomic Layer Deposition Coatings on LiMn2O4 Cathode Materials: An Experimental and Theoretical Study}, url={http://dx.doi.org/10.1021/acsami.7b06988}, DOI={10.1021/acsami.7b06988}, abstractNote={An atomic layer deposition (ALD) coating on active materials of a lithium ion battery is a more effective strategy for improving battery performance than other coating technologies. However, substantial uncertainty still remains about the underlying physics and role of the ALD coating in improving battery performance. Although improvement in the stability and capacity of CeO2 thin film coated particles for batteries has been reported, a detailed and accurate description of the mechanism has not been provided. We have developed a multiphysics-based model that takes into consideration stress mechanics, diffusion of lithium ion, and dissolution of transition-metal ions of spinel LiMn2O4 cathode. The model analyzes how different coating thicknesses affect diffusion-induced stress generation and, ultimately, crack propagation. Experimentally measured diffusivity and dissolution rates were incorporated into the model to account for a trade-off between delayed transport and prevention of side reactions. Along with experimental results, density functional theory results are used to explain how a change in volume, due to dissolution of active material, can affect battery performance. The predicted behavior from the model is well-matched with experimental results obtained on coated and uncoated LiMn2O4-Li foil cells. The proposed approach and explanations will serve as important guidelines for thin film coating strategies for various battery materials.}, journal={ACS Applied Materials & Interfaces}, author={Sarkar, Susmita and Patel, Rajankumar L. and Liang, Xinhua and Park, Jonghyun}, year={2017}, month={Sep} }