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We report a novel delithiation process for epitaxial thin films of LiCoO(001) cathodes using only physical methods, based on ion sputtering and annealing cycles. Preferential Li sputtering followed by annealing produces a surface layer with a Li molar fraction in the range 0.5 < < 1, characterized by good crystalline quality. This delithiation procedure allows the unambiguous identification of the effects of Li extraction without chemical byproducts and experimental complications caused by electrolyte interaction with the LiCoO surface. An analysis by X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) provides a detailed description of the delithiation process and the role of O and Co atoms in charge compensation. We observe the simultaneous formation of Co ions and of holes localized near O atoms upon Li removal, while the surface shows a (2 × 1) reconstruction. The delithiation method described here can be applied to other crystalline battery elements and provide information on their properties that is otherwise difficult to obtain.
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http://dx.doi.org/10.1021/acsami.3c06147 | DOI Listing |
Angew Chem Int Ed Engl
September 2025
Key Laboratory of Molecular Nanostructure and Nanotechnology, Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, P.R. China.
Alloy anodes with high specific capacity are extensively utilized in all-solid-state batteries (ASSBs). However, they are challenged by interfacial kinetic and mechanical issues. Real-time investigation of interfacial failure mechanisms at the nanoscale is crucial for optimizing the alloy anodes.
View Article and Find Full Text PDFAdv Mater
August 2025
State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
To improve the energy density of Li-ion batteries, conventional sacrificial prelithiation agents (LiFeO, LiO and LiCO, etc.) are introduced to compensate for active lithium loss, but they undergo serious volumetric shrinkage during decomposition, generating voids that compromise electrode architecture integrity and deteriorate electrochemical performance. Herein, the typical Li-rich layered oxide cathode is converted into Li-rich disordered rocksalt oxide (LRDO) prelithiation agent, achieving 330 mAh g charge capacity and retaining 130 mAh g reversible capacity (contributing 200 mAh g irreversible prelithiation capacity).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2025
School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826, Republic of Korea.
Sulfide-based all-solid-state batteries (ASSBs) exhibit distinct degradation dynamics characterized by intricate interfacial cascade reactions that differ markedly from those of conventional lithium-ion batteries (LIBs). Despite being technologically promising, these systems currently lack robust health diagnostic frameworks to capture their critical failure mechanisms. Various physicochemical analyses based on cell disassembly are available and provide useful health-related information; but, because of their destructive nature, they render cells unusable for continuous health monitoring over long-term cycling.
View Article and Find Full Text PDFAnal Chem
August 2025
State Key Laboratory of Analytical Chemistry for Life Science, Chemistry and Biomedicine Innovation Center (ChemBIC), School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.
Understanding the volume changes in lithium-ion batteries (LIBs) during charge and discharge cycles is crucial for improving battery lifespan and safety. These changes primarily originate from deformations in the electrode sheets, which are expected to be heterogeneous. However, existing methods often lacked spatial resolution and thus are insufficient in mapping this nonuniformity.
View Article and Find Full Text PDFACS Appl Mater Interfaces
August 2025
College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, P. R. China.
The commercial application of silicon-carbon microparticles (Si/C) as anode materials in advanced high-energy-density lithium-ion batteries (LIBs) has been hindered by suboptimal interfacial stability and insufficient cycling durability, which are primarily attributed to the detrimental stress generated during the lithiation and delithiation processes. In this study, a polymeric binder (PTR) was developed for Si/C anodes in lithium-ion batteries. The PTR binder was fabricated by integrating rigid poly(acrylic acid) (PAA) with flexible carboxylated styrene-butadiene rubber (XSBR) through cross-linking with tannic acid (TA), thereby forming a stable molecular architecture.
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