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Instruments / Technical Area	Publication Details	Published	Actions
B18-Core EXAFS	Effect of metal substitution on the intrinsic activity of iridium-based oxides for the oxygen evolution reaction Yinghao Xu , Yi-Hsuan Wu , Paula M. Abdala , Connor Sherwin , Veronica Celorrio , Diana Piankova , Payal Chaudhary , Vitaly Alexandrov , Agnieszka Kierzkowska , Denis A. Kuznetsov , Christoph R. Müller Chemical Science DOI: 10.1039/D5SC06242J Diamond Proposal Number(s): [36625] Open Access Show Abstract ▼ Abstract: Iridium-based oxides are among the most promising catalysts for the acidic oxygen evolution reaction (OER) owing to their high catalytic activity and stability. Substituting iridium with earth-abundant elements could lower costs and potentially boost its intrinsic activity even further; however, no unambiguous structure–activity relationships describing the physical origins of the effect of the substituent for this class of electrocatalysts have been established. In this work, we utilized a series of IrOx(:M) nanoparticle catalysts to correlate their in situ structural changes with intrinsic OER activity. We observe that IrOx(:M) with M = W and In feature a significantly higher Ir-mass-normalized OER activity than IrOx, however the activity enhancements have a different origin. While the increased activity of IrOx[thin space (1/6-em)]:[thin space (1/6-em)]In stems from a higher number of electrochemically active iridium centers (due to the leaching of indium), IrOx[thin space (1/6-em)]:[thin space (1/6-em)]W features a higher intrinsic OER activity compared to IrOx, due to electronic effects of W on neighboring Ir/O sites. Furthermore, operando electrochemical mass spectrometry experiments and density functional theory (DFT) calculations revealed that the enhanced OER activity of IrOx(:M) does not originate from a promotion of the lattice oxygen coupling mechanism, but is instead associated with a facilitated conventional adsorbate evolution mechanism.	Oct 2025
	Hidden charge order in an iron oxide square-lattice compound Jung-Hwa Kim , Darren C. Peets , Manfred Reehuis , Peter Adler , Andrey Maljuk , Tobias Ritschel , Morgan C. Allison , Jochen Geck , Jose R. L. Mardegan , Pablo J. Bereciartua Perez , Sonia Francoual , Andrew Walters , Thomas Keller , Paula M. Abdala , Philip Pattison , Pinder Dosanjh , Bernhard Keimer Physical Review Letters 127 DOI: 10.1103/PhysRevLett.127.097203 Open Access Show Abstract ▼ Abstract: Since the discovery of charge disproportionation in the FeO 2 square-lattice compound Sr 3 Fe 2 O 7 by Mössbauer spectroscopy more than fifty years ago, the spatial ordering pattern of the disproportionated charges has remained “hidden” to conventional diffraction probes, despite numerous x-ray and neutron scattering studies. We have used neutron Larmor diffraction and Fe K -edge resonant x-ray scattering to demonstrate checkerboard charge order in the FeO 2 planes that vanishes at a sharp second-order phase transition upon heating above 332 K. Stacking disorder of the checkerboard pattern due to frustrated interlayer interactions broadens the corresponding superstructure reflections and greatly reduces their amplitude, thus explaining the difficulty of detecting them by conventional probes. We discuss the implications of these findings for research on “hidden order” in other materials.	Aug 2021

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