The electrochemical interface formed between an electrode and an electrolyte significantly affects the rate and mechanism of the electrode reaction through its structure and properties, which vary across the interface. The scope of the interface has been expanded, along with the development of energy electrochemistry, where a solid-electrolyte interphase may form on the electrode and the active materials change properties near the surface region. Developing a comprehensive understanding of electrochemical interfaces and interphases necessitates three-dimensional spatial resolution characterization. Atomic force microscopy (AFM) offers advantages of imaging and long-range force measurements. Here we assess the capabilities of AFM by comparing the force curves of different regimes and various imaging modes for in situ characterizing of electrochemical interfaces and interphases. Selected examples of progress on work related to the structures and processes of electrode surfaces, electrical double layers, and lithium battery systems are subsequently illustrated. Finally, this review provides perspectives on the future development of electrochemical AFM.
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http://dx.doi.org/10.1146/annurev-anchem-061422-020428 | DOI Listing |
ACS Nano
January 2025
Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, Fudan University, Shanghai 200438, China.
The utilization of sulfide-based solid electrolytes represents an attractive avenue for high safety and energy density all-solid-state batteries. However, the potential has been impeded by electrochemical and mechanical stability at the interface of oxide cathodes. Plastic crystals, a class of organic materials exhibiting remarkable elasticity, chemical stability, and ionic conductivity, have previously been underutilized due to their susceptibility to dissolution in liquid electrolytes.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Department of Chemical and Biological Engineering and Institute of Chemical Processes, College of Engineering, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea.
Due to the extremely high energy density of Li metal, Li metal batteries are regarded as one of the most promising candidates for next-generation energy storage systems. However, interfacial issues, particularly the unstable solid electrolyte interphase (SEI) and lithium dendritic growth, hinder practical application. Herein, we induce an anion-rich interface near the Li metal by introducing positively charged self-assembled monolayers (SAMs) on ceramic-coated separators to simultaneously stabilize the SEI and homogenize the Li deposition.
View Article and Find Full Text PDFAdv Mater
January 2025
Materials Science and Engineering Program, Walker Department of Mechanical Engineering and Texas Materials Institute, The University of Texas at Austin, Austin, TX, 78712, USA.
Anode-free all solid-state batteries (AF-ASSBs) employ "empty" current collector with three active interfaces that determine electrochemical stability; lithium metal - Solid electrolyte (SE) interphase (SEI-1), lithium - current collector interface, and collector - SE interphase (SEI-2). Argyrodite LiPSCl (LPSCl) solid electrolyte (SE) displays SEI-2 containing copper sulfides, formed even at open circuit. Bilayer of 140 nm magnesium/30 nm tungsten (Mg/W-Cu) controls the three interfaces and allows for state-of-the-art electrochemical performance in half-cells and fullcells.
View Article and Find Full Text PDFSmall
January 2025
School of Environment and Energy, Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, South China University of Technology, Guangzhou, 510006, P. R. China.
In situ polymerization of cyclic ethers is a promising strategy to construct solid-state lithium (Li) metal batteries with high energy density and safety. However, their practical applications are plagued by the unsatisfactory electrochemical properties of polymer electrolytes and the unstable solid electrolyte interphase (SEI). Herein, organic perfluorodecanoic acid (PFDA) is proposed as a new initiator to polymerize 1,3-dioxolane electrolyte (PDOL), which enables the as-obtained PDOL electrolyte to deliver greatly enhanced ionic conductivity and broadened electrochemical window.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
College of Materials Science and Engineering, Nanjing Tech University, Nanjing, Jiangsu 211816, China; Jiangsu Collaborative Innovation Center for Advanced Inorganic Function Composites, Nanjing Tech University, Nanjing 211816, China. Electronic address:
Sodium metal is heralded as a premier anode candidate poised to supplant lithium in next-generation rechargeable batteries due to its abundant availability, cost-effectiveness, and superior energy density. Due to the highly reactive nature of metallic sodium, an unstable solid electrolyte interphase (SEI) forms spontaneously on the Na metal anode. This instability leads to non-uniform sodium deposition during cycling, promoting dendrite growth and the accumulation of "dead" sodium.
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