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      Chemo-mechanical expansion of lithium electrode materials – on the route to mechanically optimized all-solid-state batteries

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          Abstract

          The volume effects of electrode materials can cause local stress development, contact loss and particle cracking in the rigid environment of a solid-state battery.

          Abstract

          Charge and discharge of lithium ion battery electrodes is accompanied by severe volume changes. In a confined space, the volume cannot expand, leading to significant pressures induced by local microstructural changes within the battery. While volume changes appear to be less critical in batteries with liquid electrolytes, they will be more critical in the case of lithium ion batteries with solid electrolytes and they will be even more critical and detrimental in the case of all-solid-state batteries with a lithium metal electrode. In this work we first summarize, compare, and analyze the volume changes occurring in state of the art electrode materials, based on crystallographic studies. A quantitative analysis follows that is based on the evaluation of the partial molar volume of lithium as a function of the degree of lithiation for different electrode materials. Second, the reaction volumes of operating full cells (“charge/discharge volumes”) are experimentally determined from pressure-dependent open-circuit voltage measurements. The resulting changes in the open-circuit voltage are in the order of 1 mV/100 MPa, are well measurable, and agree with changes observed in the crystallographic data. Third, the pressure changes within solid-state batteries are approximated under the assumption of incompressibility, i.e. for constant volume of the cell casing, and are compared to experimental data obtained from model-type full cells. In addition to the understanding of the occurring volume changes of electrode materials and resulting pressure changes in solid-state batteries, we propose “mechanical” blending of electrode materials to achieve better cycling performance when aiming at “zero-strain” electrodes.

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          Berechnung der Fließgrenze von Mischkristallen auf Grund der Plastizitätsbedingung für Einkristalle .

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            Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction.

            This Review is focused on ion-transport mechanisms and fundamental properties of solid-state electrolytes to be used in electrochemical energy-storage systems. Properties of the migrating species significantly affecting diffusion, including the valency and ionic radius, are discussed. The natures of the ligand and metal composing the skeleton of the host framework are analyzed and shown to have large impacts on the performance of solid-state electrolytes. A comprehensive identification of the candidate migrating species and structures is carried out. Not only the bulk properties of the conductors are explored, but the concept of tuning the conductivity through interfacial effects-specifically controlling grain boundaries and strain at the interfaces-is introduced. High-frequency dielectric constants and frequencies of low-energy optical phonons are shown as examples of properties that correlate with activation energy across many classes of ionic conductors. Experimental studies and theoretical results are discussed in parallel to give a pathway for further improvement of solid-state electrolytes. Through this discussion, the present Review aims to provide insight into the physical parameters affecting the diffusion process, to allow for more efficient and target-oriented research on improving solid-state ion conductors.
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              Ageing mechanisms in lithium-ion batteries

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                Author and article information

                Journal
                EESNBY
                Energy & Environmental Science
                Energy Environ. Sci.
                Royal Society of Chemistry (RSC)
                1754-5692
                1754-5706
                2018
                2018
                : 11
                : 8
                : 2142-2158
                Affiliations
                [1 ]Institute of Physical Chemistry
                [2 ]Justus-Liebig-University Giessen
                [3 ]35392 Giessen
                [4 ]Germany
                [5 ]Center for Materials Research (LaMa)
                [6 ]Battery and Electrochemistry Laboratory (BELLA)
                [7 ]Institute of Nanotechnology
                [8 ]Karlsruhe Institute of Technology
                [9 ]76344 Eggenstein-Leopoldshafen
                [10 ]BASF SE
                [11 ]67056 Ludwigshafen am Rhein
                [12 ]Institute of Mechanics and Materials
                [13 ]Technische Hochschule Mittelhessen
                [14 ]35390 Giessen
                Article
                10.1039/C8EE00907D
                a2f2ea2b-8b78-4df9-85fa-62f9c7244a54
                © 2018

                http://rsc.li/journals-terms-of-use

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