More Like this

1. Electrodeposition Stability Landscape for Solid–Solid Interfaces

   https://doi.org/10.1002/advs.202307455  

   Chatterjee, Debanjali; Naik, Kaustubh G.; Vishnugopi, Bairav S.; Mukherjee, Partha P. (December 2023, Advanced Science)

   Abstract As solid‐state batteries (SSBs) with lithium (Li) metal anodes gain increasing traction as promising next‐generation energy storage systems, a fundamental understanding of coupled electro‐chemo‐mechanical interactions is essential to design stable solid‐solid interfaces. Notably, uneven electrodeposition at the Li metal/solid electrolyte (SE) interface arising from intrinsic electrochemical and mechanical heterogeneities remains a significant challenge. In this work, the thermodynamic origins of mechanics‐coupled reaction kinetics at the Li/SE interface are investigated and its implications on electrodeposition stability are unveiled. It is established that the mechanics‐driven energetic contribution to the free energy landscape of the Li deposition/dissolution redox reaction has a critical influence on the interface stability. The study presents the competing effects of mechanical and electrical overpotential on the reaction distribution, and demarcates the regimes under which stress interactions can be tailored to enable stable electrodeposition. It is revealed that different degrees of mechanics contribution to the forward (dissolution) and backward (deposition) reaction rates result in widely varying stability regimes, and the mechanics‐coupled kinetics scenario exhibited by the Li/SE interface is shown to depend strongly on the thermodynamic and mechanical properties of the SE. This work highlights the importance of discerning the underpinning nature of electro‐chemo‐mechanical coupling toward achieving stable solid/solid interfaces in SSBs. 

   more » « less
2. Glassy solid-state electrolytes for all-solid state batteries

   Wheaton, Jacob; Olson, Madison; Torres, Victor M; Martin, Steve W (January 2023, American Ceramic Society bulletin)

   Glassy solid-state electrolytes present several advantages over other classes of solid-state electrolytes, but some material and design challenges must be overcome prior to commercialization. 

   more » « less
3. In situ characterizations of solid–solid interfaces in solid‐state batteries using synchrotron X‐ray techniques

   https://doi.org/10.1002/cey2.131  

   Lucero, Marcos; Qiu, Shen; Feng, Zhenxing (July 2021, Carbon Energy)

   Abstract The solid–solid electrode–electrolyte interface represents an important component in solid‐state batteries (SSBs), as ionic diffusion, reaction, transformation, and restructuring could all take place. As these processes strongly influence the battery performance, studying the evolution of the solid–solid interfaces, particularly in situ during battery operation, can provide insights to establish the structure–property relationship for SSBs. Synchrotron X‐ray techniques, owing to their unique penetration power and diverse approaches, are suitable to investigate the buried interfaces and examine structural, compositional, and morphological changes. In this review, we will discuss various surface‐sensitive synchrotron‐based scattering, spectroscopy, and imaging methods for the in situ characterization of solid–solid interfaces and how this information can be correlated to the electrochemical properties of SSBs. The goal is to overview the advantages and disadvantages of each technique by highlighting representative examples, so that similar strategies can be applied by battery researchers and beyond to study similar solid‐solid interface systems. 

   more » « less
4. Inverse design of compression-induced solid – solid transitions in colloids

   https://doi.org/10.1080/08927022.2020.1798005  

   Du, Chrisy Xiyu; van Anders, Greg; Dshemuchadse, Julia; Dodd, Paul M.; Glotzer, Sharon C. (September 2020, Molecular Simulation)

   null (Ed.)
5. Two-step crystallization and solid–solid transitions in binary colloidal mixtures

   https://doi.org/10.1073/pnas.2008561117  

   Fang, Huang; Hagan, Michael F.; Rogers, W. Benjamin (November 2020, Proceedings of the National Academy of Sciences)

   null (Ed.)

   Crystallization is fundamental to materials science and is central to a variety of applications, ranging from the fabrication of silicon wafers for microelectronics to the determination of protein structures. The basic picture is that a crystal nucleates from a homogeneous fluid by a spontaneous fluctuation that kicks the system over a single free-energy barrier. However, it is becoming apparent that nucleation is often more complicated than this simple picture and, instead, can proceed via multiple transformations of metastable structures along the pathway to the thermodynamic minimum. In this article, we observe, characterize, and model crystallization pathways using DNA-coated colloids. We use optical microscopy to investigate the crystallization of a binary colloidal mixture with single-particle resolution. We observe classical one-step pathways and nonclassical two-step pathways that proceed via a solid–solid transformation of a crystal intermediate. We also use enhanced sampling to compute the free-energy landscapes corresponding to our experiments and show that both one- and two-step pathways are driven by thermodynamics alone. Specifically, the two-step solid–solid transition is governed by a competition between two different crystal phases with free energies that depend on the crystal size. These results extend our understanding of available pathways to crystallization, by showing that size-dependent thermodynamic forces can produce pathways with multiple crystal phases that interconvert without free-energy barriers and could provide approaches to controlling the self-assembly of materials made from colloids. 

   more » « less