Due to its high theoretical capacity and low anode potential advantages, lithium is becoming the ideal high-capacity anode of next generation batteries. Nevertheless, the satisfactory long-term cyclability of lithium metal batteries is still not achieved. Inspired by the intrinsic soft nature of the lithium metal, we have developed a simple room temperature solid-state deformation route to overcome the lithium dendrite issue, and the cycle life of the deformation treated lithium anode is 5 times that of the untreated lithium anode. It is demonstrated that microscale lithium grains are divided into nanoscale lithium grains by directional friction forces of solid-state deformation. The lithium grain boundaries are lithiophilic active sites towards Li ions, which regulate homogeneous deposition of Li ions to form a thin and stable SEI film, eventually overcoming the lithium dendrite issue and enhancing the cyclability of lithium batteries. Overcoming the challenges in conventional tedious chemical routes to grow high-density grain boundary active sites for catalysis, the room temperature solid-state deformation route will pave a new road to grow high-density grain boundaries for fuel cells and metal-based batteries.
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http://dx.doi.org/10.1039/d3cc04217k | 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
School of Energy and Power Engineering, Huazhong University of Science & Technology, Wuhan, Hubei 430074, China.
ACS Omega
December 2024
HUN-REN Research Centre for Natural Sciences, Institute of Materials and Environmental Chemistry, Magyar Tudósok Körútja 2, 1117 Budapest, Hungary.
Lithium phosphorus oxynitride (LiPON) is a crucial electrolyte for all-solid-state thin-film batteries due to its sufficient ionic conductivity. Understanding the mechanical behavior of LiPON films is crucial for further technological development. Previous studies noted unexpected ductility and strain recovery in amorphous LiPON during sharp-ended tip indentations revealing pile-up formation and densification as the main deformation mechanisms.
View Article and Find Full Text PDFNat Mater
January 2025
School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA, USA.
Anode-free solid-state batteries contain no active material at the negative electrode in the as-manufactured state, yielding high energy densities for use in long-range electric vehicles. The mechanisms governing charge-discharge cycling of anode-free batteries are largely controlled by electro-chemo-mechanical phenomena at solid-solid interfaces, and there are important mechanistic differences when compared with conventional lithium-excess batteries. This Perspective provides an overview of the factors governing lithium nucleation, growth, stripping and cycling in anode-free solid-state batteries, including mechanical deformation of lithium, the chemical and mechanical properties of the current collector, microstructural effects, and stripping dynamics.
View Article and Find Full Text PDFLangmuir
December 2024
Key Laboratory of Functional Polymer Materials of Ministry of Education and College of Chemistry, Nankai University, Tianjin 300071, China.
Polyelectrolyte complex (PEC) hydrogels provide a promising strategy to develop a class of physically cross-linked networks characterized by exceptional toughness and self-healing properties. However, the precise control of the microstructure and the enhancement of mechanical properties still pose challenges in the field of PEC hydrogels. Herein, we propose a strategy to manipulate the structure of PEC with competitively charged surfactant micelles, leveraging the spatially confined surface charge and excluded volume effects to overcome coacervation issues associated with the PEC, thus achieving a simple one-step preparation of macroscopically uniform and tough PEC hydrogels.
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