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We propose a promising electrochemical analysis tool based on the distribution of relaxation times (DRT) to quantify interfacial resistances towards a comprehensive understanding of complex solid-state interfacial phenomena in sulfide-based all-solid-state batteries (ASSBs). Using DRT-assisted impedance analysis, we identify a new resistance component in the range of 10-10 Hz of 3.5 and 0.9 Ω in the absence and presence of a LiNbO layer, respectively, at 1C-rate. Experimental and computational studies confirm that this interfacial resistance results from lithium depletion in sulfide solid electrolytes. Furthermore, we expect our approach to provide new insights into complex interfacial phenomena in ASSBs.
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http://dx.doi.org/10.1039/d0cc08367d | DOI Listing |
Bioresour Technol
September 2025
Department of Earth Resources and Environmental Engineering, Hanyang University, Seoul 04763, Republic of Korea. Electronic address:
The rapid increase of electronic waste, particularly battery waste, presents significant environmental challenges such as pollutant emissions and resource depletion, emphasizing the need for effective valorization and reuse strategies. This study introduces a novel approach for repurposing end-of-life lithium iron phosphate (LFP) batteries as catalysts in the pyrolysis of walnut shells (WS). Characterization analyses revealed that LFP provides both Lewis and Brønsted acid sites, which alter the thermal decomposition pathway of WS.
View Article and Find Full Text PDFNat Commun
August 2025
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, Shenzhen, PR China.
Lithium metal negative electrodes are highly promising for high-specific-energy batteries due to their low electrochemical potential and high capacity. However, dendrite growth due to limited Li transport at the interface hinder their performance and safety. Enhancing interfacial Li transport can prevent Li depletion and ensure uniform Li deposition.
View Article and Find Full Text PDFJ Chem Phys
August 2025
Institute of Physical Chemistry, University of Münster, Corrensstraße 28/30, 48149 Münster, Germany.
We present molecular dynamics simulations on localized high-concentration electrolytes (LHCE) based on the conducting salt lithium bis(fluorosulfonyl)imide (LiFSI) or lithium bis(trifluoromethanesulfonyl)imide dissolved in the solvent 1,2-dimethoxyethane and diluted to two different degrees with the diluent 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether. Due to the immiscibility of the conducting salt phase (salt + solvent) and the diluent phase, LHCEs feature a complex microstructure of two phases forming an internal interface. In this study, we not only investigate the lithium coordination structure in the conducting salt phase but also the size and composition of its interface to the diluent phase by Voronoi tessellations.
View Article and Find Full Text PDFJ Am Chem Soc
August 2025
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Solid electrolyte interphase (SEI) critically governs lithium (Li) battery performance. Yet, understanding the native SEI remains challenging due to the lack of techniques capable of depth profiling of the interphase layer under electrolyte conditions (wet-SEI). In this work, cryogenic X-ray photoelectron spectroscopy (cryo-XPS) coupled with argon gas cluster ion beam (GCIB) sputtering was developed to extensively investigate the vitrified wet-SEI of Li metal batteries without chemical damage.
View Article and Find Full Text PDFJ Am Chem Soc
August 2025
Advanced Separation & Conversion on Engineered Nanopore Dynamics Laboratory, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China.
Lithium (Li) dendrite formation in Li metal batteries intrinsically challenges Coulombic efficiency (CE) and safety. While constructing an anode protective layer offers a potential solution for dendrite suppression, existing approaches are limited by insufficient molecular-level control over both Li and anion dynamics simultaneously. Herein, we construct a binary cooperative magnesium porphyrin-based covalent organic framework (Mg-Por-COF) protective layer designed for synergetic cation-anion regulation at the anode-electrolyte interface.
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