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      Direct Realization of Complete Conversion and Agglomeration Dynamics of SnO 2 Nanoparticles in Liquid Electrolyte

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          Abstract

          The conversion reaction is important in lithium-ion batteries because it governs the overall battery performance, such as initial Coulombic efficiency, capacity retention, and rate capability. Here, we have demonstrated in situ observation of the complete conversion reaction and agglomeration of nanoparticles (NPs) upon lithiation by using graphene liquid cell transmission electron microscopy. The observation reveals that the Sn NPs are nucleated from the surface of SnO 2, followed by merging with each other. We demonstrate that the agglomeration has a stepwise process, including rotation of a NP, formation of necks, and subsequent merging of individual NPs.

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          Most cited references35

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          In situ observation of the electrochemical lithiation of a single SnO₂ nanowire electrode.

          We report the creation of a nanoscale electrochemical device inside a transmission electron microscope--consisting of a single tin dioxide (SnO(2)) nanowire anode, an ionic liquid electrolyte, and a bulk lithium cobalt dioxide (LiCoO(2)) cathode--and the in situ observation of the lithiation of the SnO(2) nanowire during electrochemical charging. Upon charging, a reaction front propagated progressively along the nanowire, causing the nanowire to swell, elongate, and spiral. The reaction front is a "Medusa zone" containing a high density of mobile dislocations, which are continuously nucleated and absorbed at the moving front. This dislocation cloud indicates large in-plane misfit stresses and is a structural precursor to electrochemically driven solid-state amorphization. Because lithiation-induced volume expansion, plasticity, and pulverization of electrode materials are the major mechanical effects that plague the performance and lifetime of high-capacity anodes in lithium-ion batteries, our observations provide important mechanistic insight for the design of advanced batteries.
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            Single-layered ultrasmall nanoplates of MoS2 embedded in carbon nanofibers with excellent electrochemical performance for lithium and sodium storage.

            The preparation and electrochemical storage behavior of MoS2 nanodots--more precisely single-layered ultrasmall nanoplates--embedded in carbon nanowires has been studied. The preparation is achieved by an electrospinning process that can be easily scaled up. The rate performance and cycling stability of both lithium and sodium storage were found to be outstanding. The storage behavior is, moreover, highly exciting from a fundamental point of view, as the differences between the usual storage modes--insertion, conversion, interfacial storage--are beneficially blurred. The restriction to ultrasmall reaction domains allows for an almost diffusion-less and nucleation-free "conversion", thereby resulting in a high capacity and a remarkable cycling performance.
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              High-resolution EM of colloidal nanocrystal growth using graphene liquid cells.

              We introduce a new type of liquid cell for in situ transmission electron microscopy (TEM) based on entrapment of a liquid film between layers of graphene. The graphene liquid cell facilitates atomic-level resolution imaging while sustaining the most realistic liquid conditions achievable under electron-beam radiation. We employ this cell to explore the mechanism of colloidal platinum nanocrystal growth. Direct atomic-resolution imaging allows us to visualize critical steps in the process, including site-selective coalescence, structural reshaping after coalescence, and surface faceting.
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                Author and article information

                Journal
                ACS Omega
                ACS Omega
                ao
                acsodf
                ACS Omega
                American Chemical Society
                2470-1343
                03 October 2017
                31 October 2017
                : 2
                : 10
                : 6329-6336
                Affiliations
                []Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS) , 1689 Yuseong Dae-ro 70, Daejeon 305-701, Republic of Korea
                []Department of Materials Science & Engineering, Korea Advanced Institute of Science & Technology , 335 Science Road, Daejeon 305-701, Republic of Korea
                Author notes
                [* ]E-mail: idkim@ 123456kaist.ac.kr (I.-D.K.).
                [* ]E-mail: j.y.lee@ 123456kaist.ac.kr (J.Y.L.).
                Article
                10.1021/acsomega.7b01046
                6645017
                b21b360e-86e8-4aca-b8a7-074e26328cdb
                Copyright © 2017 American Chemical Society

                This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

                History
                : 21 July 2017
                : 22 September 2017
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                ao7b01046
                ao-2017-01046f

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