Beyond Li-ion Batteries

Batteries are everywhere. From personal electronics to electric vehicles to grid-scale energy storage, the ability to store energy in a compact form has become a vital part of society. Our efforts in this area focus on enabling next-generation (Beyond Li-ion) technologies through improved fundamental understanding of battery behavior, new materials/manufacturing approaches, and rational design of 3D architectures. We utilize a suite of operando electrochemical techniques to gain insight into the coupled morphological evolution and electrochemical behavior of electrode materials as they change dynamically during cycling. The mechanistic understanding gained through this approach has allowed us to predict performance and failure modes without disassembling a cell, enabling rapid screening and design of materials/electrodes with superior performance. To manufacture these new materials, we focus on interfacial designs utilizing thin protective coatings, surface treatments, and 3D architectures to enable improved cycle life, higher rates of charge, and enhanced safety. We utilize a wide range of characterization techniques to observe electrode morphology, composition, phase, mechanical behavior, optical properties, and electrochemical performance, as interfacial performance in battery systems depends on a complex and highly interconnected set of properties, requiring an interdisciplinary approach to research.

Selected Publications:

(32) M. K. Jangid, A. L. Davis, D. W. Liao, N. P. Dasgupta “Improved Rate Capability in Composite Solid-State Battery Electrodes Using 3-D Architectures” ACS Energy Lett. 8, 2522 (2023) [link]

(31) V. Goel, K.-H. Chen, N. P. Dasgupta, K. Thornton “Optimization of Laser-Patterned Electrode Architectures for Fast Charging of Li-ion Batteries using Simulations Parameterized by Machine Learning” Energy Storage Mater. 57, 44 (2023) [link]

(30) K. Lee, E. Kazyak, M. J. Wang, N. P. Dasgupta, J. Sakamoto “Analyzing Void Formation and Rewetting of Thin In Situ-Formed Li Anodes on LLZO” Joule 6, 2547 (2022) [link]

(29) E. Kazyak, M. J. Wang, K. Lee, S. Yadavalli, A. J. Sanchez, M. D. Thouless, J. Sakamoto, N. P. Dasgupta “Understanding the electro-chemo-mechanics of Li plating in anode-free solid-state batteries with operando 3D microscopy” Matter 5, 3912 (2022) [link]

(28) Y. Chen, L.Torres-Castro, K.-H. Chen, D. Penley, J. Lamb, M. Karulkar, N. P. Dasgupta “Operando Detection of Li Plating during Fast Charging of Li-ion Batteries using Incremental Capacity Analysis” J. Power Sources 539, 231601 (2022) [link]

(27) C. Bauer, S. Burkhardt, N. P. Dasgupta, L. Ager-Wick Ellingsen, L. L. Gaines, H. Hao, R. Hischier, L. Hu, Y. Huang, J. Janek, C. Liang, H. Li, J. Li, Y. Li, Y.-C. Lu, W. Luo, L. F. Nazar, E. A. Olivetti, J. F. Peters, J. L. M. Rupp, M. Weil, J. F. Whitacre, S. Xu “Charging Sustainable Batteries” Nature Sustainability 5, 176 (2022) [link]

(26) W. S. LePage, Y. Chen, A. Poli, M. D.Thouless, N. P. Dasgupta “Sodium Mechanics: Effects of Temperature, Strain Rate, and Grain Rotation and Implications for Sodium Metal Batteries” Extreme Mech. Lett. 52, 101644 (2022) [link]

(25) E. Kazyak, K.-H. Chen, Y. Chen, T. H. Cho, N. P. DasguptaEnabling 4C Fast Charging of Lithium-Ion Batteries by Coating Graphite with a Solid-State ElectrolyteAdv. Energy Mater. 12, 2102618 (2022) [link]

(24) Y. Chen, K.-H. Chen, A. J. Sanchez, E. Kazyak, V. Goel, Y. Gorlin, J. Christensen, K. Thornton, N. P. Dasgupta “Operando video microscopy of Li plating and re-intercalation on graphite anodes during fast charging” J. Mater. Chem. A  9, 23522 (2021) [link]

(23) B. S. Vishnugopi, E. Kazyak, J. A. Lewis, J. Nanda, M. T. McDowell, N. P. Dasgupta, P. P. Mukherjee “Challenges and Opportunities for Fast Charging of Solid-State Lithium Metal Batteries” ACS Energy Lett. 6, 3734 (2021) [link]

(22) A. L. Davis, V. Goel, D. W. Liao, M. N. Main, E. Kazyak, J. Lee, K. Thornton, N. P. Dasgupta “Rate Limitations in Composite Solid-State Battery Electrodes: Revealing Heterogeneity with Operando Microscopy” ACS Energy Lett. 6, 2993 (2021) [link]

(20) A. J. Sanchez, E. Kazyak, Y. Chen, J. Lasso, N. P. Dasgupta “Lithium Stripping: Anisotropic Evolution and Faceting of Pits Revealed by Operando 3-D Microscopy” J. Mater Chem. A. 9, 21013 (2021)  [link]

(21) A. L. Davis, E. Kazyak, D. W. Liao, K. N. Wood, N. P. Dasgupta “Operando Analysis of Interphase Dynamics in Anode-Free Solid-State Batteries with Sulfide Electrolytes” J. Electrochem. Soc. 168, 070557 (2021) [link]

(19) B. Kinzer, A. L. Davis, T. Krauskopf, H. Hartmann, W. S. LePage, E. Kazyak, J. Janek, N. P. Dasgupta, J. Sakamoto “Operando Analysis of the Molten Li|LLZO Interface: Understanding how the Physical Properties of Li Affect the Critical Current Density” Matter 4, 1947 (2021).  [link]

(18) K.‐H. Chen, V. Goel, M. J. Namkoong, M. Wied, S. Müller, V. Wood, J. Sakamoto, K. Thornton, N. P. Dasgupta, “Enabling 6C Fast Charging of Li‐Ion Batteries with Graphite/Hard Carbon Hybrid Anodes”, Adv. Energy Mater. 2003336 (2020) [link]

(17) E. Kazyak, M. Shin, W. S. LePage, T. H. Cho, N. P. Dasgupta, “Molecular Layer Deposition of Li-ion Conducting “Lithicone” Solid Electrolytes”, Chem. Commun. 56, 15537 (2020) [link]

(16) A. Gupta, E. Kazyak, N. P. Dasgupta, J. Sakamoto, “Electrochemical and Surface Chemistry Analysis of Lithium Lanthanum Zirconium Tantalum Oxide (LLZTO)/Liquid Electrolyte (LE) Interfaces”, J. Power Sources 474, 228598 (2020) [link]

(15) K.-H. Chen, M. J. Namkoong, V. Goel, C. Yang, S. Kazemiabnavi, S.M. Mortuza, E. Kazyak, J. Mazumder, K. Thornton, J. Sakamoto, N. P. Dasgupta, “Efficient fast-charging of lithium-ion batteries enabled by laser-patterned three-dimensional graphite anode architectures” J. Power Sources 471, 228475 (2020) [link]

(14) A. L. Davis, R. Garcia-Mendez, K. N. Wood, E. Kazyak, K.-H. Chen, G. Teeter, J. Sakamoto, N. P. Dasgupta, “Electro-Chemo-Mechanical Evolution of Sulfide Solid Electrolyte/Li metal Interfaces: Operando Analysis and ALD Interlayer Effects” J. Mater. Chem. A, (2020) [link]

(13) E. Kazyak, R. Garcia-Mendez, W. S. LePage, A. Sharafi, A. L. Davis, A. J. Sanchez, K.-H. Chen, C. Haslam, J. Sakamoto, N. P. Dasgupta, “Li Penetration in Ceramic Solid Electrolytes: Operando Microscopy Analysis of Morphology, Propagation, and Reversibility” Matter  2, 1 (2020) [link]

(12) A. J. Sanchez, E. Kazyak, Y. Chen, K.-H. Chen, E. R. Pattison, N. P. Dasgupta, “Plan-View Operando Video Microscopy of Li Metal Anodes: Identifying the Coupled Relationships among Nucleation, Morphology, and Reversibility” ACS Energy Lett. 5, 994 (2020) [link]

(11) K. B. Hatzell, X. C. Chen, C. L. Cobb, N. P. Dasgupta, M. B. Dixit, L. E. Marbella, M. T. McDowell, P. P. Mukherjee, A. Verma, V. Viswanathan, A. S. Westover, W. G. Zeier, “Challenges in Lithium Metal Anodes for Solid-State Batteries” ACS Energy Lett. 5, 922 (2020) [link]

(10) W. S. LePage, Y. Chen, E. Kazyak, K.-H. Chen, A. J. Sanchez, A. Poli, E. M. Arruda, M. D. Thouless, N. P. Dasgupta, “Lithium Mechanics: Roles of Strain Rate and Temperature and Implications for Lithium Metal Batteries” J. Electrochem. Soc. 166, 89 (2019) [link]

(9) K.‐H. Chen, A. J. Sanchez, E. Kazyak, A. L. Davis, N. P. Dasgupta, “Synergistic Effects of 3D Current Collectors and ALD Surface Modification for High Coulombic Efficiency Lithium Metal Anodes” Adv. Energy Mater. 9, 1802534 (2019) [link]

(8) E. Kazyak, K.-H. Chen, A. L. Davis, S. Yu, A. J. Sanchez, J. Lasso, A. R. Bielinski, T. Thompson, J. Sakamoto, D. J. Siegel, and N. P. Dasgupta, “Atomic Layer Deposition and First Principles Modeling of Glassy Li3BO3-Li2CO3 Electrolytes for Solid-State Li Metal Batteries” J. Mater. Chem. A 6, 19425 (2018) [link]

(7) A. Gupta, E. Kazyak, N. Craig, J. Christensen, N. P. Dasgupta, and J. Sakamoto” Evaluating the Effects of Temperature and Pressure on Li/PEO-LiTFSI Interfacial Stability and Kinetics” J. Electrochem. Soc. 165, A2801(2018) [link]

(6) A. Sharafi, E. Kazyak, A. L. Davis, S. Yu, T Thompson, D. J. Siegel, N. P. Dasgupta, J. Sakamoto, “Surface Chemistry Mechanism of Ultra-Low Interfacial Resistance in the Solid-State Electrolyte Li7La3Zr2O12” Chem. Mater. 29, 7961 (2017) [link]

(5) E. Kazyak, K.-H. Chen, K. N. Wood, A. L. Davis, T. Thompson, A.R. Bielinski, A. J. Sanchez, X. Wang, C. Wang, J. Sakamoto, N. P. Dasgupta, “Atomic Layer Deposition of the Solid Electrolyte Garnet Li7La3Zr2O12Chem. Mater. 29, 3785 (2017) [link]

(4) K.-H. Chen, K. N. Wood, E. Kazyak, W. S. LePage, A. L. Davis, A. J. Sanchez, N. P. Dasgupta, “Dead Lithium: Mass Transport Effects on Voltage, Capacity, and Failure of Lithium Metal Anodes” J. Mater. Chem. A 5, 11671 (2017)  [link]

(3) K. N. Wood, M. Noked, N. P. Dasgupta, “Lithium Metal Anodes: Toward an Improved Understanding of Coupled Morphological, Electrochemical, and Mechanical Behavior” ACS Energy Lett. 2, 664 (2017) [link]

(2) K. N. Wood, E. Kazyak, A. F. Chadwick, K. H. Chen, J. G. Zhang, K. Thornton, N. P. Dasgupta, “Dendrites and Pits: Untangling the Complex Behavior of Lithium Metal Anodes through Operando Video Microscopy”, ACS Central Science 2, 790 (2016). [link]

(1) E. Kazyak*, K. N. Wood* and N. P. Dasgupta, “Improved Cycle Life and Stability of Lithium Metal Anodes through Ultrathin Atomic Layer Deposition Surface Treatments”, Chem. Mater27, 6457 (2015). [link]