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Instruments / Technical Area	Publication Details	Published
E01-JEM ARM 200CF E02-JEM ARM 300CF	Cd/Pt precursor solution for solar H2 production and in-situ photochemical synthesis of Pt single-atom decorated CdS nanoparticles Pankaj Sharma , Monika Sharma , Malcolm Dearg , Martin Wilding , Thomas J. A. Slater , C. Richard A. Catlow Angewandte Chemie International Edition DOI: 10.1002/anie.202301239 Diamond Proposal Number(s): [31082] Show Abstract ▼ Abstract: Despite extensive efforts to develop high-performance H2 evolution catalysts, this remains a major challenge. Here, we demonstrate the use of Cd/Pt precursor solutions for significant photocatalytic H2 production (154.7 mmol g-1 h-1), removing the need for a pre-synthesized photocatalyst. In addition, we also report simultaneous in-situ synthesis of Pt single-atoms anchored CdS nanoparticles (PtSA-CdSIS) during photoirradiation. The highly dispersed in-situ incorporation of extensive Pt single atoms on CdSIS enables the enhancement of active sites and suppresses charge recombination, which results in exceptionally high solar-to-hydrogen conversion efficiency of ~1% and an apparent quantum yield of over 91% (365 nm) for H2 production. Our work not only provides a promising strategy for maximising H2 production efficiency but also provides a green process for H2 production and the synthesis of highly photoactive PtSA-CdSIS nanoparticles.	Feb 2023
I22-Small angle scattering & Diffraction	Understanding the emergence of the boson peak in molecular glasses Mario Gonzalez-Jimenez , Trent Barnard , Ben A. Russell , Nikita V. Tukachev , Uroš Javornik , Laure-Anne Hayes , Andrew J. Farrell , Sarah Guinane , Hans M. Senn , Andrew J. Smith , Martin Wilding , Gregor Mali , Motohiro Nakano , Yuji Miyazaki , Paul Mcmillan , Gabriele C. Sosso , Klaas Wynne Nature Communications 14 DOI: 10.1038/s41467-023-35878-6 Diamond Proposal Number(s): [28529] Open Access Show Abstract ▼ Abstract: A common feature of glasses is the “boson peak”, observed as an excess in the heat capacity over the crystal or as an additional peak in the terahertz vibrational spectrum. The microscopic origins of this peak are not well understood; the emergence of locally ordered structures has been put forward as a possible candidate. Here, we show that depolarised Raman scattering in liquids consisting of highly symmetric molecules can be used to isolate the boson peak, allowing its detailed observation from the liquid into the glass. The boson peak in the vibrational spectrum matches the excess heat capacity. As the boson peak intensifies on cooling, wide-angle x-ray scattering shows the simultaneous appearance of a pre-peak due to molecular clusters consisting of circa 20 molecules. Atomistic molecular dynamics simulations indicate that these are caused by over-coordinated molecules. These findings represent an essential step toward our understanding of the physics of vitrification.	Jan 2023
I20-EDE-Energy Dispersive EXAFS (EDE)	A novel fuel cell design for operando energy-dispersive X-ray absorption measurements Andrew S. Leach , Jennifer Hack , Monica Amboage , Sofia Diaz-Moreno , Haoliang Huang , Patrick L. Cullen , Martin Wilding , Emanuele Magliocca , Thomas Miller , Christopher Howard , Daniel Brett , Paul Shearing , Paul F. Mcmillan , Andrea E. Russell , Rhodri Jervis Journal Of Physics: Condensed Matter DOI: 10.1088/1361-648X/ac0476 Diamond Proposal Number(s): [22008, 15650] Open Access Show Abstract ▼ Abstract: A polymer electrolyte fuel cell (PEFC) has been designed to allow operando X-ray absorption spectroscopy (XAS) measurements of catalysts. The cell has been developed to operate under standard fuel cell conditions, with elevated temperatures and humidification of the gas-phase reactants, both of which greatly impact the catalyst utilisation. X-ray windows in the endplates of the cell facilitate collection of XAS spectra during fuel cell operation while maintaining good compression in the area of measurement. Results of polarisation curves and cyclic voltammograms (CVs) showed that the operando cell performs well as a fuel cell, while also providing XAS data of suitable quality for robust XANES analysis. The cell has produced comparable XAS results when performing a cyclic voltammogram to an established in situ cell when measuring the Pt LIII edge. Similar trends of Pt oxidation, and reduction of the formed Pt oxide, have been presented with a time resolution of 5 seconds for each spectrum, paving the way for time-resolved spectral measurements of fuel cell catalysts in a fully-operating fuel cell.	May 2021
I15-1-X-ray Pair Distribution Function (XPDF)	Understanding the local structure of Eu3+- and Y3+-stabilized zirconia: insights from luminescence and X-ray absorption spectroscopic investigations M. Eibl , S. Shaw , D. Prieur , A. Rossberg , M. C. Wilding , C. Hennig , K. Morris , J. Rothe , T. Stumpf , N. Huittinen Journal Of Materials Science 55, 10095 - 10120 DOI: 10.1007/s10853-020-04768-3 Diamond Proposal Number(s): [21208] Open Access Show Abstract ▼ Abstract: This study combines bulk structural and spectroscopic investigations of Eu3+- or Y3+/Eu3+ co-doped tetragonal and cubic zirconia polymorphs to gain an in-depth understanding of the solid solution formation process. Our bulk structural characterizations show that the dopant is homogenously distributed in the ZrO2 host structure resulting in an increase of the bulk symmetry with increasing dopant substitution (from 8 to 26 mol%). The local site symmetry around the Eu3+ dopant, however, determined with luminescence spectroscopy (TRLFS), remains low in all samples. Results obtained with X-ray pair distribution function and X-ray absorption spectroscopy show that the average coordination environment in the stabilized zirconia structures remains practically unchanged. Despite this very constant average dopant environment, site-selective TRLFS data show the presence of three nonequivalent Eu3+ environments in the ZrO2 solid structures. These Eu3+ environments are assumed to arise from Eu3+ incorporation at superficial sites, which increase in abundance as the size of the crystallites decrease, and incorporation on two bulk sites differing in the location of the oxygen vacancies with respect to the dopant cation.	May 2020
	Polyamorphism and liquid–liquid phase transitions in amorphous silicon and supercooled Al2O3–Y2O3 liquids Paul F. Mcmillan , G. Neville Greaves , Mark Wilson , Martin C. Wilding , Dominik Daisenberger DOI: 10.1002/9781118540350.ch12	Apr 2013

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