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Instruments / Technical Area	Publication Details	Published	Actions
B18-Core EXAFS I11-High Resolution Powder Diffraction	Anion redox as a means to derive layered manganese oxychalcogenides with exotic intergrowth structures Shunsuke Sasaki , Souvik Giri , Simon J. Cassidy , Sunita Dey , Maria Batuk , Daphne Vandemeulebroucke , Giannantonio Cibin , Ronald I. Smith , Philip Holdship , Clare P. Grey , Joke Hadermann , Simon J. Clarke Nature Communications 14 DOI: 10.1038/s41467-023-38489-3 Diamond Proposal Number(s): [25166, 14239] Open Access Show Abstract ▼ Abstract: Topochemistry enables step-by-step conversions of solid-state materials often leading to metastable structures that retain initial structural motifs. Recent advances in this field revealed many examples where relatively bulky anionic constituents were actively involved in redox reactions during (de)intercalation processes. Such reactions are often accompanied by anion-anion bond formation, which heralds possibilities to design novel structure types disparate from known precursors, in a controlled manner. Here we present the multistep conversion of layered oxychalcogenides Sr2MnO2Cu1.5Ch2 (Ch = S, Se) into Cu-deintercalated phases where antifluorite type [Cu1.5Ch2]2.5- slabs collapsed into two-dimensional arrays of chalcogen dimers. The collapse of the chalcogenide layers on deintercalation led to various stacking types of Sr2MnO2Ch2 slabs, which formed polychalcogenide structures unattainable by conventional high-temperature syntheses. Anion-redox topochemistry is demonstrated to be of interest not only for electrochemical applications but also as a means to design complex layered architectures.	May 2023
B18-Core EXAFS I15-1-X-ray Pair Distribution Function (XPDF)	Exploring cation–anion redox processes in one-dimensional linear chain vanadium tetrasulfide rechargeable magnesium ion cathodes Sunita Dey , Jeongjae Lee , Sylvia Britto , Joshua M. Stratford , Evan N. Keyzer , Matthew T. Dunstan , Giannantonio Cibin , Simon J. Cassidy , Mahmoud Elgaml , Clare P. Grey Journal Of The American Chemical Society DOI: 10.1021/jacs.0c08222 Diamond Proposal Number(s): [22856, 22930, 24676] Open Access Show Abstract ▼ Abstract: For magnesium ion batteries (MIBs) to be used commercially, new cathodes must be developed that show stable reversible Mg intercalation. VS4 is one such promising material, with vanadium and disulfide anions [S2]2– forming one-dimensional linear chains, with a large interchain spacing (5.83 Å) enabling reversible Mg insertion. However, little is known about the details of the redox processes and structural transformations that occur upon Mg intercalation and deintercalation. Here, employing a suite of local structure characterization methods including X-ray photoelectron spectroscopy (XPS), V and S X-ray absorption near-edge spectroscopy (XANES), and 51V Hahn echo and magic-angle turning with phase-adjusted sideband separation (MATPASS) NMR, we show that the reaction proceeds via internal electron transfer from V4+ to [S2]2–, resulting in the simultaneous and coupled oxidation of V4+ to V5+ and reduction of [S2]2– to S2–. We report the formation of a previously unknown intermediate in the Mg–V–S compositional space, Mg3V2S8, comprising [VS4]3– tetrahedral units, identified by using density functional theory coupled with an evolutionary structure-predicting algorithm. The structure is verified experimentally via X-ray pair distribution function analysis. The voltage associated with the competing conversion reaction to form MgS plus V metal directly is similar to that of intermediate formation, resulting in two competing reaction pathways. Partial reversibility is seen to re-form the V5+ and S2– containing intermediate on charging instead of VS4. This work showcases the possibility of developing a family of transition metal polychalcogenides functioning via coupled cationic–anionic redox processes as a potential way of achieving higher capacities for MIBs.	Oct 2020

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