The mechanisms of Li deposition behaviors, which overwhelmingly affect battery performances and safety, are far to be understood in solid-state batteries. Here, using in situ micro-nano electrochemical scanning electron microscopy (SEM) manipulation platform, dynamic Li plating behaviors on 10 metallic substrates have been tracked, and the underlying mechanisms for dendrite-free Li plating are elucidated. Distinct Li deposition behaviors on Cu, Ti, Ni, Bi, Cr, In, Ag, Au, Pd, and Al are revealed quantitatively in nucleation densities, growth rates, and anisotropic ratios. For Li alloyable metals, the dynamic Li alloying process before Li growth is visually captured. It is concluded that a good affinity for Li and appropriate lattice compatibility between the substrate and Li are needed to facilitate homogeneous Li plating. Our work not only uncovers the Li plating dynamics, shedding light on the design of solid-state batteries, but also provides a powerful integrated SEM platform for future in-depth investigation of solid-state batteries.
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http://dx.doi.org/10.1126/sciadv.add2000 | DOI Listing |
J Am Chem Soc
January 2025
Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, School of Chemical Engineering and Technology, National Industry-Education Integration Platform of Energy Storage, and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin University, Tianjin 300072, China.
In situ polymerization strategies hold great promise for enhancing the physical interfacial stability in solid-state batteries, yet (electro)chemical degradation of polymerized interfaces, especially at high voltages, remains a critical challenge. Herein, we find interphase engineering is crucial for the polymerization process and polymer stability and pioneer an in situ polymerization-fluorination (Poly-FR) strategy to create durable interfaces with excellent physical and (electro)chemical stabilities, achieved by designing a bifunctional initiator for both polymerization and on-surface lithium donor reactions. The integrated in situ fluorination converts LiCO impurities on LiNiCoMnO (NCM811) surfaces into LiF-rich interphases, effectively inhibiting the aggressive (de)lithiation intermediates and protecting the interface from underlying chemical degradation, thereby surpassing the stability limitations of polymerization alone.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
UT Austin: The University of Texas at Austin, Materials Science and Engineering, 1 University Station C2200, 78712, Austin, UNITED STATES OF AMERICA.
The extensive commercialization of practical solid-state batteries (SSBs) necessitates the development of high-loading solid-state cathodes with fast charging capability. However, electrochemical kinetics are severely delayed in thick cathodes due to tortuous ion transport pathways and slow solid-solid ion diffusion, which limit the achievable capacity of SSBs at high current densities. In this work, we propose a conductivity gradient cathode with low-tortuosity to enable facile ion transport and counterbalance ion concentration gradient, thereby overcoming the kinetic limitations and achieving fast charging capabilities in thick cathodes.
View Article and Find Full Text PDFNat Commun
January 2025
State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, PR China.
Polyether electrolytes have been widely recognized for their favorable compatibility with lithium-metal, yet they are hampered by intrinsically low oxidation thresholds, limiting their potential for realizing high-energy Li-metal batteries. Here, we report a general approach involving the bridge joints between non-lithium metal ions and ethereal oxygen, which significantly enhances the oxidation stability of various polyether electrolyte systems. To demonstrate the feasibility of the ion-bridging strategy, a Zn ion-bridged polyether electrolyte (Zn-IBPE) with an extending electrochemical stability window of over 5 V is prepared, which enables good cyclability in 4.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, P. R. China.
Electric aircraft such as electric aircraft and electric vehicles play a key role in the future electric aviation industry, but they put forward huge requirements for battery energy density. However, the current high-energy-density lithium battery technology still needs to be broken through. Herein, through the molecular structure design of the polymer electrolyte, a strategy of a fast migration channel and wide electrochemical window is proposed to fabricate high-voltage-resistant solid polymer electrolyte (HVPE) via in situ polymerization.
View Article and Find Full Text PDFChem Commun (Camb)
January 2025
College of Physics, Qingdao University, Qingdao 266071, China.
A polyvinylidene carbonate:BN layer was constructed between LiAlTi(PO) (LATP) and the lithium (Li) electrode, improving interfacial compatibility and thermal stability. The LiN-rich solid electrolyte interphase regulates Li deposition behaviors. The solid-state Li metal batteries (SSLMBs) show remarkable electrochemical performance, exhibiting endurance for 800 hours of cycling at 0.
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