Irregular Li deposition is the major reason for poor reversibility and cycle instability in Li metal batteries, even leading to safety hazards, the causes of which have been extensively explored. The structural disconnection induced by completely dissolving Li in the traditional testing protocol is a key factor accounting for irregular Li growth during the subsequent deposition process. Herein, the critical role played by the structural connectivity of electrochemical Li reservoir in subsequent Li deposition behaviors is elucidated and a morphology-performance correlation is established. The structural connection and resultant well-distributed morphology of the in situ electrochemical Li reservoir ensure efficient electron transfer and Li diffusion pathway, finally leading to homogenized Li nucleation and growth. Tailoring the geometry of Li reservoir can improve the coulombic efficiency and cyclability of anode-free Li metal batteries by optimizing Li deposition behavior.
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http://dx.doi.org/10.1002/anie.202319847 | DOI Listing |
J Phys Chem Lett
January 2025
Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
Cu-based catalysts for the electrochemical reduction of CO and CO exhibit a perplexingly unique reactivity toward multicarbon based products compared to other studied electrocatalysts. Here we use insights gained from a recent phenomenological 3-site microkinetic model and grand-canonical density functional theory calculations to clarify the importance of an underemphasized aspect critical to Cu's unique reactivity: a population of so-called "reservoir" sites. Using model Cu surface motifs, we discuss how these types can be represented by undercoordinated structural defects like step edges and grain boundaries which form a network of highly anisotropic migration channels.
View Article and Find Full Text PDFNanoscale
January 2025
Department of Electronic Materials Engineering, Kwangwoon University, Seoul 01897, Republic of Korea.
To achieve both excellent analog switching for training and retention for inference simultaneously, we investigated elevated-temperature (ET) training of PrCaMnO (PCMO) electrochemical random access memory (ECRAM). Improved weight update characteristics can be obtained by thermally reduced ionic resistivity of the HfO electrolyte at ET (413 K). Furthermore, excellent retention characteristics (10 s) were observed at room temperature, which can be explained by enhanced ion storage within the reservoir (or channel) layer ET training.
View Article and Find Full Text PDFAdv Mater
December 2024
School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, 518055, China.
Single-crystal high-nickel oxide with an integral structure can prevent intergranular cracks and the associated detrimental reactions. Yet, its low surface-to-volume ratio makes surficial degradation a more critical factor in electrochemical performance. Herein, artificial proton-rich (ammonium bicarbonate) shell is successfully introduced on the nickel-rich LiNiCoMnO single crystals for in situ electrochemically conversing into inorganic maskant to enhance stability of cathode.
View Article and Find Full Text PDFChem Sci
December 2024
Institute of Condensed Matter and Nanosciences, Molecular Chemistry, Materials and Catalysis, Université Catholique de Louvain Louvain-la-Neuve Belgium
Facilitating rapid charge transfer in electrode materials necessitates the optimization of their ionic transport properties. Currently, only a limited number of Li/Na-ion organic cathode materials have been identified, and those exhibiting intrinsic solid-phase ionic conductivity are even rarer. In this study, we present tetra-lithium and sodium salts with the generic formulae: A-Ph-CHP and A-Ph-PhP, wherein A = Li, Na; Ph-CHP = 2,5-dioxido-1,4-phenylene bis(methylphosphinate); Ph-PhP = 2,5-dioxido-1,4-phenylene bis(phenylphosphinate), as novel alkali-ion reservoir cathode materials.
View Article and Find Full Text PDFSoft Robot
December 2024
Department of Mechanical Engineering, Seoul National University, Seoul, South Korea.
Based on the analysis of the structures of robots and electronics developed so far, it should be noted that a majority of them need a reservoir for electrical energy storage. Unfortunately, most off-the-shelf devices commercially available nowadays are based on rigid parts that heavily limit the possibilities of incorporating such products into soft robots and wearable electronics. To address these issues, a new type of flexible structure for electrical energy storage, which consists of small battery cells connected by liquid metal paths, was proposed.
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