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Instruments / Technical Area	Publication Details	Published	Actions
I12-JEEP: Joint Engineering, Environmental and Processing	Structural changes in the silver-carbon composite anode interlayer of solid-state batteries Dominic Spencer-Jolly , Varnika Agarwal , Christopher Doerrer , Bingkun Hu , Shengming Zhang , Dominic L. R. Melvin , Hui Gao , Xiangwen Gao , Paul Adamson , Oxana Magdysyuk , Patrick S. Grant , Robert A. House , Peter G. Bruce Joule 1 DOI: 10.1016/j.joule.2023.02.001 Diamond Proposal Number(s): [26082] Open Access Show Abstract ▼ Abstract: Ag-carbon composite interlayers have been reported to enable Li-free (anodeless) cycling of solid-state batteries. Here, we report structural changes in the Ag-graphite interlayer, showing that on charge, Li intercalates electrochemically into graphite, subsequently reacting chemically with Ag to form Li-Ag alloys. Discharge is not the reverse of charge but rather passes through Li-deficient Li-Ag phases. At higher charging rates, Li intercalation into graphite outpaces the chemical reactions with Ag, delaying the formation of the Li-Ag phases and resulting in more Li metal deposition at the current collector. At and above 2.5 mA·cm−2, Li dendrites are not suppressed. Ag nanoparticles do not suppress dendrites more effectively than does an interlayer of graphite alone. Instead, Ag in the carbon interlayer results in more homogeneous Li and Li-Ag formation on the current collector during charge.	Feb 2023
labSAXS-Offline SAXS and Sample Environment Development	Buffering volume change in solid-state battery composite cathodes with CO2-derived block polycarbonate ethers Georgina L. Gregory , Hui Gao , Boyang Liu , Xiangwen Gao , Gregory J. Rees , Mauro Pasta , Peter G. Bruce , Charlotte K. Williams Journal Of The American Chemical Society DOI: 10.1021/jacs.2c06138 Diamond Proposal Number(s): [29810] Open Access Show Abstract ▼ Abstract: Polymers designed with a specific combination of electrochemical, mechanical, and chemical properties could help overcome challenges limiting practical all-solid-state batteries for high-performance next-generation energy storage devices. In composite cathodes, comprising active cathode material, inorganic solid electrolyte, and carbon, battery longevity is limited by active particle volume changes occurring on charge/discharge. To overcome this, impractical high pressures are applied to maintain interfacial contact. Herein, block polymers designed to address these issues combine ionic conductivity, electrochemical stability, and suitable elastomeric mechanical properties, including adhesion. The block polymers have “hard-soft-hard”, ABA, block structures, where the soft “B” block is poly(ethylene oxide) (PEO), known to promote ionic conductivity, and the hard “A” block is a CO2-derived polycarbonate, poly(4-vinyl cyclohexene oxide carbonate), which provides mechanical rigidity and enhances oxidative stability. ABA block polymers featuring controllable PEO and polycarbonate lengths are straightforwardly prepared using hydroxyl telechelic PEO as a macroinitiator for CO2/epoxide ring-opening copolymerization and a well-controlled Mg(II)Co(II) catalyst. The influence of block polymer composition upon electrochemical and mechanical properties is investigated, with phosphonic acid functionalities being installed in the polycarbonate domains for adhesive properties. Three lead polymer materials are identified; these materials show an ambient ionic conductivity of 10 –4 S cm–1, lithium-ion transport (tLi+ 0.3–0.62), oxidative stability (>4 V vs Li+/Li), and elastomeric or plastomer properties (G′ 0.1–67 MPa). The best block polymers are used in composite cathodes with LiNi0.8Mn0.1Co0.1O2 active material and Li6PS5Cl solid electrolyte–the resulting solid-state batteries demonstrate greater capacity retention than equivalent cells featuring no polymer or commercial polyelectrolytes.	Sep 2022

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