skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: (Invited) Advanced Insitu Electron Microscopy for Batteries: Insights for Lithium-Ion and Beyond
Rechargeable batteries are crucial for energy storage across consumer electronics and automobile propulsion applications, facilitating the transition towards carbon neutrality and advancing clean energy technologies. Despite great success of Li-ion batteries (LIBs) in the commercial market, alternative technologies based on beyond-Li chemistry are highly demanded for large-scale and power-intensive applications necessitating enhanced energy density, lifetime, and safety, where fundamental understanding of the structure-property relationship of novel battery materials is critically needed. Transmission electron microscopy (TEM) is an indispensable method to characterize materials structures and compositions at the atomic scale, which is of particular importance for battery research to investigate crystal lattices, defects, as well as microstructural and chemical heterogeneities within materials used in electrodes, electrolytes, and their interfaces. Further, with rapid technical development, in-situ TEM has enabled real-time observations of various dynamical phenomena and chemical processes during battery cycling and phase transformations. Leveraging advanced in-situ TEM techniques, our collaborative endeavors with Dr. Marca Doeff have enabled us to conduct comparative analyses of Li and Na reactions within battery electrodes, offering unique insights into in early-stage beyond-Li chemistry. Herein, we present a systematic exploration of in-situ TEM studies for LIBs and beyond, focusing on electrode materials through intercalation, alloying, and conversion reaction mechanisms. By direct comparison between electrochemical reactions with Li and Na, we found substantial differences in reaction mechanisms, pathways, and kinetics between lithiation and sodiation processes, which are fundamentally related to various factors, such as ionic diffusion barrier, electrochemically induced stress, and geometric constraints. This concept has been demonstrated in multiple case studies that allows us to enhance the sodiation kinetics by tuning the overall reaction energetics through nanostructure optimization and interfacial engineering. We envision that the knowledge learned from in-situ TEM will provide valuable insights into understanding the alkali-ion electrochemistry and kinetics, thereby serving as foundational principles guiding the advancement of beyond Li-ion battery technologies.  more » « less
Award ID(s):
2239598
PAR ID:
10573975
Author(s) / Creator(s):
Publisher / Repository:
IOP Publishing
Date Published:
Journal Name:
ECS Meeting Abstracts
Volume:
MA2024-02
Issue:
2
ISSN:
2151-2043
Page Range / eLocation ID:
210
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; (, Advanced Materials)
    Abstract Conversion‐type materials have been considered as potentially high‐energy‐density alternatives to commercially dominant intercalation‐based electrodes for rechargeable ion batteries and have attracted tremendous research effort to meet the performance for viable energy‐storage technologies. In situ transmission electron microscopy (TEM) has been extensively employed to provide mechanistic insights into understanding the behavior of battery materials. Noticeably, a great portion of previous in situ TEM studies has been focused on conversion‐type materials, but a dedicated review for this group of materials is missing in the literature. Herein, recent developments of in situ TEM techniques for investigation of dynamic phase transformation and associated structural, morphological, and chemical evolutions during conversion reactions with alkali ions in secondary batteries are comprehensively summarized. The materials of interest broadly cover metal oxides, chalcogenides, fluorides, phosphides, nitrides, and silicates with specific emphasis on spinel metal oxides and recently emerged 2D metal chalcogenides. Special focus is placed on the scientific findings that are uniquely obtained by in situ TEM to address fundamental questions and practical issues regarding phase transformation, structural evolution, electrochemical redox, reaction mechanism, kinetics, and degradation. Critical challenges and perspectives are discussed for advancing new knowledge that can bridge the gap between prototype materials and real‐world applications. 
    more » « less
  2. ; ; ; ; (, ChemElectroChem)
    Abstract The solid electrolyte interphase (SEI) is a dynamic, electronically insulating film that forms on the negative electrode of Li+batteries (LIBs) and enables ion movement to/from the interface while preventing electrolyte breakdown. However, there is limited comparative understanding of LIB SEIs with respect to those formed on Na+and K+electrolytes for emerging battery concepts. We used scanning electrochemical microscopy (SECM) for the in situ interfacial analysis of incipient SEIs in Li+, K+and Na+electrolytes formed on multi‐layer graphene. Feedback images using 300 nm SECM probes and ion‐sensitive measurements indicated a superior passivation and highest cation flux for a Li+‐SEI in contrast to Na+and K+‐SEIs. Ex situ X‐ray photoelectron spectroscopy indicated significant fluoride formation for only Li+and Na+‐SEIs, enabling correlation to in situ SECM measurements. While SEI chemistry remains complex, these electroanalytical methods reveal links between chemical variables and the interfacial properties of materials for energy storage. 
    more » « less
  3. ; ; (, JOM)
    The battery chemistry must be diversified to achieve a sustainable energy landscape by effectively utilizing renewable energy sources. Alkali metal-ion, all-solid-state, metal-air batteries, and multivalent batteries offer unique cost, safety, raw material abundance, energy, and power density solutions. However, realizing these “Beyond Li-ion batteries” must uncover their working principles and performance & property relationship. In this aspect, mitigating chemo-mechanical instabilities in the structure and surface of the electrodes plays a crucial role in their performance. Unfortunately, the coupling between electrochemical and mechanical interactions is often poorly understood due to a lack of operando characterization. This review article explains the working principles of curvature measurement and digital image correlation for measuring stress and strain generations in battery materials. We provided specific examples of how these operando mechanical measurements shed light on instabilities in alkali-metal ion electrodes, solid electrolytes, Li-O2 batteries, and aqueous Zn-ion batteries. Operando mechanical measurements offer an effective way to map changes in the physical fingerprint of the battery materials, therefore providing crucial information to elucidate instabilities in battery materials. 
    more » « less
  4. ; ; ; ; (, Journal of Physics D: Applied Physics)
    Abstract Lithium-ion batteries (LIBs) have solidified their position as primary energy storage solutions for applications ranging from portable electronics to electric vehicles. As power-intensive applications expand, achieving fast charging/discharging performance is increasingly critical for high-energy-density batteries. However, the increased thickness of electrodes in LIBs presents significant challenges for charge (Li⁺ and electron) transfer kinetics, as longer charge migration distances hinder fast charging and discharging performance. Enormous efforts have been made to summarize advancements in materials chemistry—optimizing ionic pathways and crystal structure—to enhance Li⁺ transfer within the bulk of electrode materials. Yet, materials design and modifications fall short of fully addressing Li+and electron transport limitations in thick electrodes. Despite the significance of potentially offering a solution to these constraints, the strategic engineering of electrode architecture has been rarely discussed. In this mini-review, we highlight recent innovations in electrode structural design for fast-charging applications, examining gradient architectures, low-tortuosity structures, and novel current collector designs. By exploring these advanced approaches and offering perspectives on future developments, we aim to promote further advancements toward achieving high-energy-density, fast-charging LIBs. 
    more » « less
  5. ; (, Journal of advanced technological education)
    Lithium-ion batteries (LIBs) are central in modern life, where they are found in products from smartphones to laptops to electric vehicles. The demand for efficient and sustainable batteries is higher than ever, with the predicted depletion of lithium sources after 2050 [1-3]. As an alternative to LIBs, next-generation fluoride-ion batteries (FIBs) are now being studied since fluorine is more abundant than lithium. While the majority of FIBs reported use solid electrolytes, liquid electrolytes are of interest for room-temperature applications and they are the focus of this article. This article begins by providing a concise background on specific concepts of battery chemistry that can be used as a basis to expand micro/nanotechnology education curricula to include alternative battery technologies. Key points on defining battery components, battery capacity, and redox reactions at play (including differences between redox reactions in LIBs vs FIBs) are presented. A survey on recent developments of liquid electrolytes in FIBs is derived, where three chemical strategies for designing liquid electrolytes for FIB are determined. This analysis of FIB liquid electrolytes studied so far provides a perspective to holistically improve room-temperature FIBs by tailoring the anode, cathode, and electrolyte combination. Ultimately, the survey of literature developed in the article can have an exemplary role in bibliographic research on alternative battery technologies for students in secondary, two-year, or four-year higher education institutions. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email