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High-Throughput Combinatorial Analysis of the Spatiotemporal Dynamics of Nanoscale Lithium Metal Plating.

ABSTRACT: The development of Li metal batteries requires a detailed understanding of complex nucleation and growth processes during electrodeposition. In situ techniques offer a framework to study these phenomena by visualizing structural dynamics that can inform the design of uniform plating morphologies. Herein, we combine scanning electrochemical cell microscopy (SECCM) with in situ interference reflection microscopy (IRM) for a comprehensive investigation of Li nucleation and growth on lithiophilic thin-film gold electrodes. This multimicroscopy approach enables nanoscale spatiotemporal monitoring of Li plating and stripping, along with high-throughput capabilities for screening experimental conditions. We reveal the accumulation of inactive Li nanoparticles in specific electrode regions, yet these regions remain functional in subsequent plating cycles, suggesting that growth does not preferentially occur from particle tips. Optical-electrochemical correlations enabled nanoscale mapping of Coulombic Efficiency (CE), showing that regions prone to inactive Li accumulation require more cycles to achieve higher CE. We demonstrate that electrochemical nucleation time (t_nuc) is a lagging indicator of nucleation and introduce an optical method to determine t_nuc at earlier stages with nanoscale resolution. Plating at higher current densities yielded smaller Li nanoparticles and increased areal density, and was not affected by heterogeneous topographical features, being potentially beneficial to achieve a more uniform plating at longer time scales. These results enhance the understanding of Li plating on lithiophilic surfaces and offer promising strategies for uniform nucleation and growth. Our multimicroscopy approach has broad applicability to study nanoscale metal plating and stripping phenomena, with relevance in the battery and electroplating fields.

SUBMITTER: Martin-Yerga D

PROVIDER: S-EPMC11363218 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature

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High-Throughput Combinatorial Analysis of the Spatiotemporal Dynamics of Nanoscale Lithium Metal Plating.

Martín-Yerga Daniel D Xu Xiangdong X Valavanis Dimitrios D West Geoff G Walker Marc M Unwin Patrick R PR

ACS nano 20240813 34

The development of Li metal batteries requires a detailed understanding of complex nucleation and growth processes during electrodeposition. <i>In situ</i> techniques offer a framework to study these phenomena by visualizing structural dynamics that can inform the design of uniform plating morphologies. Herein, we combine scanning electrochemical cell microscopy (SECCM) with <i>in situ</i> interference reflection microscopy (IRM) for a comprehensive investigation of Li nucleation and growth on l ...[more]

PMID: 39136274

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Project description:We present a novel method utilizing "saltless" pH gradient weak cation exchange-hydrophilic interaction liquid chromatography directly coupled to electron transfer dissociation (ETD) mass spectrometry for the automated on-line high throughput characterization of hypermodified combinatorial histone codes. This technique, performed on a low resolution mass spectrometer, displays an improvement over existing methods with an approximately 100-fold reduction in sample requirements and analysis time. The scheme presented is capable of identifying all of the major combinatorial histone codes present in a sample in a 2-h analysis. The large N-terminal histone peptides are eluted by the pH and organic solvent weak cation exchange-hydrophilic interaction liquid chromatography gradient and directly introduced via nanoelectrospray ionization into a benchtop linear quadrupole ion trap mass spectrometer equipped with ETD. Each polypeptide is sequenced, and the modification sites are identified by ETD fragmentation. The isobaric trimethyl and acetyl modifications are resolved chromatographically and confidently distinguished by the synthesis of mass spectrometric and chromatographic information. We demonstrate the utility of the method by complete characterization of human histone H3.2 and histone H4 from butyrate-treated cells, but it is generally applicable to the analysis of highly modified peptides. We find this methodology very useful for chromatographic separation of isomeric species that cannot be separated well by any other chromatographic means, leading to less complicated tandem mass spectra. The improved separation and increased sensitivity generated novel information about much less abundant forms. In this method demonstration we report over 200 H3.2 forms and 70 H4 forms, including forms not yet detected in human cells, such as the remarkably highly modified histone H3.2 K4me3K9acK14acK18acK23acK27acK36me3. Such detail provided by our proteomics platform will be essential for determining how histone modifications occur and act in combination to propagate the histone code during transcriptional events and could greatly enable sequencing of the histone component of human epigenomes.

Dataset Information

High-Throughput Combinatorial Analysis of the Spatiotemporal Dynamics of Nanoscale Lithium Metal Plating.

Publications

High-Throughput Combinatorial Analysis of the Spatiotemporal Dynamics of Nanoscale Lithium Metal Plating.

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