B07-B1-Versatile Soft X-ray beamline: High Throughput ES1
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Diamond Proposal Number(s):
[43895]
Open Access
Abstract: X-ray photoelectron spectroscopy (XPS) is a major technique in catalyst research due to its ability to determine chemical states on the surface. Near ambient pressure XPS (NAP-XPS) enables in situ analysis, offering valuable insight into catalytic processes. However, modern catalysts are often supported on non-conductive supports such as TiO2 or SiO2, which can present significant challenges for XPS analysis due to charging and differential charging. These issues can distort spectral data, rendering data unusable and wasting valuable instrument time. While several sample preparation strategies exist, many are limited by not allowing high temperature analysis, the risk of sample loss (e.g., from powder flaking off), or continued susceptibility to charging. In this work, we introduce a simple, robust, and time-efficient method for mounting catalyst powders by compressing them between aluminium foil disks. This approach provides excellent sample hold, minimises charging effects, and is suitable for high-temperature NAP-XPS analysis and synchrotron x-ray sources. The method addresses key limitations of conventional preparation techniques and enables more reliable characterisation of insulating catalyst materials.
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Aug 2026
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E02-JEM ARM 300CF
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Sam
Sullivan-Allsop
,
Nick
Clark
,
Wendong
Wang
,
Rongsheng
Cai
,
William
Thornley
,
David G.
Hopkinson
,
James G.
Mchugh
,
Ben
Davies
,
Samuel
Pattisson
,
Nicholas F.
Dummer
,
Rui
Zhang
,
Matthew
Lindley
,
Gareth
Tainton
,
Jack
Harrison
,
Hugo
De Latour
,
Joseph
Parker
,
Joshua
Swindell
,
Eli G.
Castanon
,
Amy
Carl
,
David J.
Lewis
,
Natalia
Martsinovich
,
Christopher S.
Allen
,
Mohsen
Danaie
,
Andrew J.
Logsdail
,
Vladimir
Fal’ko
,
Graham J.
Hutchings
,
Alex
Summerfield
,
Roman
Gorbachev
,
Sarah J.
Haigh
Diamond Proposal Number(s):
[33252, 35552]
Abstract: The structure and dynamics of adsorbed atoms (adatoms) at solid-liquid interfaces determine the performance of advanced catalysts, electrochemical devices, molecular separation technologies, and metal extraction from waste streams. However, in situ investigations of atomically dispersed metals in various chemical environments have been prevented by insufficient imaging resolution and solvent incompatibility. In this study, we combined a specimen design that provides atomic resolution in liquid-phase electron microscopy with deep learning–enabled analysis to explore the interactions between gold adatoms, graphite support, and the solvent collectively. We tracked the locations of >106 graphite-supported gold adatoms, dimers, and larger clusters in five solvents. Although their initial atomic dispersion was determined by the solvent polarity, fast drying kinetics at low temperature was required for optimizing catalytic performance.
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Apr 2026
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E02-JEM ARM 300CF
I05-ARPES
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Amy
Carl
,
Nicholas
Clark
,
David G.
Hopkinson
,
Matthew
Hamer
,
Matthew
Watson
,
Laxman
Nagireddy
,
James E.
Nunn
,
Alexei
Barinov
,
Yichao
Zou
,
William
Thornley
,
Casey
Cheung
,
Wendong
Wang
,
Sam
Sullivan-Allsop
,
Xiao
Li
,
Astrid
Weston
,
Eli G.
Castanon
,
Andrey V.
Kretinin
,
Cephise
Cacho
,
Neil R.
Wilson
,
Sarah J.
Haigh
,
Roman
Gorbachev
Diamond Proposal Number(s):
[21597, 21981, 24290, 24338]
Open Access
Abstract: Magnetic two-dimensional materials are a promising platform for novel nano-electronic device architectures. One such layered crystal is the ferromagnetic semiconductor chromium germanium telluride (Cr2Ge2Te6) which recently attracted interest due to its potential for spintronics and memory applications. Here we investigate its properties from the structural standpoint using atomic resolution Scanning Transmission Electron Microscopy (STEM) and present the first atomic resolution images down to its monolayer limit. We develop a novel technique that allows one to map the local tilt with unprecedented spatial resolution using only high-resolution images, enabling mapping of the topography and morphological variation of atomically thin crystals. Using it, we show that the Cr2Ge2Te6 monolayer has an unusually large out-of-plane rippling, with local tilt variation reaching 20° over few nm length scales. We hypothesize that such a strongly buckled structure originates from both point and extended lattice defects which are more prevalent in monolayer crystals. In addition, we correlate the structural observations with the band structure measurements using Angle-Resolved Photoemission Spectroscopy (ARPES). We believe that both the atomic scale insights we have gained on Cr2Ge2Te6 and our novel approach to nanoscale topography mapping will benefit the development of van der Waals heterostructures in both fundamental and applied research.
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Feb 2026
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B18-Core EXAFS
I15-1-X-ray Pair Distribution Function (XPDF)
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Shanshan
Xu
,
Matthew E.
Potter
,
Raquel
Simancas
,
Lucy
Costley-Wood
,
Boya
Qiu
,
Xuzhao
Liu
,
Cristina
Stere
,
M. Asuncion
Molina
,
Danial
Farooq
,
Floriana
Tuna
,
Dingyue
Zhang
,
Shuanglin
Zhang
,
Huanhao
Chen
,
Shengzhe
Ding
,
Xinrui
Wang
,
Sarayute
Chansai
,
Matthew
Lindley
,
Sarah J.
Haigh
,
Armando
Ibraliu
,
Lan
Lan
,
Piu
Chawdhury
,
Mariyam
Bi
,
Otis
Leahair
,
Yilai
Jiao
,
Min
Hu
,
Qiang
Liu
,
Toru
Wakihara
,
Xiaolei
Fan
,
Andrew M.
Beale
,
Christopher
Hardacre
Diamond Proposal Number(s):
[33381, 32971, 36241]
Open Access
Abstract: Methanol synthesis via non-thermal plasma (NTP) catalytic CO2 hydrogenation provides a sustainable approach to chemical and fuel production with potential in carbon emissions reduction. However, the underlying mechanisms remain unclear. Here we evaluate the mechanism of NTP-catalytic CO2 hydrogenation over Cu–Zn/ZSM-5 through operando X-ray absorption spectroscopy, diffuse reflectance infrared Fourier transform spectroscopy and in situ X-ray pair distribution function. We found that Zn enhances Cu dispersion and reducibility, as well as forming active Cu/ZnO interfacial sites. Beyond the conventional formate pathway on metallic Cu, these interfaces enable an additional CO hydrogenation route, enhancing methanol yield. NTP also promotes gas-phase CO2 dissociation to CO, bypassing the reverse water–gas shift step required in thermal catalysis. No Cu/Zn alloy formation was observed, underscoring the importance of metallic Cu and Cu/ZnO interfaces under NTP conditions. Furthermore, NTP stabilizes reduced Cu species, preventing re-oxidation and ensuring sustained catalytic activity. These findings advance the mechanistic understanding of NTP-assisted catalysis.
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Feb 2026
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B07-B1-Versatile Soft X-ray beamline: High Throughput ES1
B18-Core EXAFS
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Caiwu
Liang
,
Lucas
Garcia Verga
,
Benjamin
Moss
,
Santosh
Kumar
,
Soren B.
Scott
,
Mark A.
Turner
,
Pilar
Ferrer
,
Veronica
Celorrio
,
David C.
Grinter
,
Yemin
Tao
,
Sid
Halder
,
Yifeng
Wang
,
Cindy
Tseng
,
Guangmeimei
Yang
,
Georg
Held
,
Sarah J.
Haigh
,
Aron
Walsh
,
Ifan E. L.
Stephens
,
James R.
Durrant
,
Reshma R.
Rao
Diamond Proposal Number(s):
[34803, 30396, 31886]
Open Access
Abstract: Oxidation states underpin the understanding of active states, reaction mechanisms and catalytic performance of electrocatalysts. However, determining them at complex solid–liquid interfaces is challenging. Here we use multimodal spectroscopy to investigate polarized iridium oxide (IrOx) electrodes, a model water oxidation catalyst, to identify potential-dependent iridium and oxygen oxidation states. By integrating multiple operando spectroscopies (optical (ultraviolet–visible), Ir L-edge and O K-edge X-ray absorption spectroscopy) with electrochemistry mass spectrometry and density functional theory calculations, we identify the sequential depletion of electron densities from the Ir5d band (corresponding to Ir3+→Ir4+→Ir5+), followed by electron removal from the O2p band, forming electrophilic oxygen species (O−1) due to enhanced Ir–O covalency and electronic state overlap. Time-resolved measurements reveal distinct lifetimes for Ir5+ and O−1 states under water oxidation conditions, Ir5+ remains unreactive whereas O−1 is consumed at a time constant commensurate with the reaction rate, indicating that O−1 drives the oxygen evolution reaction. These findings demonstrate the necessity of using multiple operando techniques to gain a unified understanding of the evolution of oxidation states and active sites with potential for water oxidation on oxide catalysts.
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Feb 2026
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E02-JEM ARM 300CF
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Wendong
Wang
,
Gareth R.
Tainton
,
Nicholas J.
Clark
,
James G.
Mchugh
,
Xue
Li
,
Sam
Sullivan-Allsop
,
David G.
Hopkinson
,
Oldrich
Cicvárek
,
Francisco
Selles
,
Rui
Zhang
,
Joshua D.
Swindell
,
Alex
Summerfield
,
David J.
Lewis
,
Vladimir I.
Fal'Ko
,
Zdenek
Sofer
,
Sarah
Haigh
,
Roman
Gorbachev
Diamond Proposal Number(s):
[39088]
Abstract: Transition metal diiodides such as FeI2, NiI2, and CoI2 are an emerging class of 2D magnets exhibiting rich and diverse magnetic behavior, but their study at the monolayer limit has been severely hindered by fabrication challenges due to their air-sensitivity. Here, we introduce a polymer-free method for clean, rapid, and high-yield assembly of hermetically encapsulated suspended samples of air-sensitive monolayers. Applied to diiodides, it enables atomic resolution characterization of thin samples down to the monolayer limit using transmission electron microscopy. Our imaging, combined with complementary first-principles calculations, reveals an unusually small energy barrier between alternate stable stacking polytypes in few-layer films, enabling extrinsic control of the stacking phase. We also observe stable isolated iodine vacancies that do not aggregate to form extended structures and identify and verify the stability of the various edge configurations of thin samples. These results establish the structural characteristics of these materials in the thin limit and more broadly demonstrate the utility of our transfer platform for creating atomically clean suspended van der Waals heterostructures.
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Jan 2026
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[33252]
Open Access
Abstract: The Noise2Void technique is demonstrated for successful denoising of atomic resolution scanning transmission electron microscopy (STEM) images. The technique is applied to denoising atomic resolution images and videos of gold adatoms on a graphene surface within a graphene liquid-cell, with the denoised experimental data qualitatively demonstrating improved visibility of both the Au adatoms and the graphene lattice. The denoising performance is quantified by comparison to similar simulated data and the approach is found to significantly outperform both total variation and simple Gaussian blurring. Compared to other denoising methods, the Noise2Void technique has the combined advantages that it requires no manual intervention during training or denoising, no prior knowledge of the sample and is compatible with real-time data acquisition rates of at least 45 frames per second.
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Jan 2026
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B18-Core EXAFS
I11-High Resolution Powder Diffraction
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Zhaodong
Zhu
,
Xin
Lian
,
Xue
Han
,
Zi
Wang
,
Siyu
Zhou
,
Meng
He
,
Tianze
Zhou
,
Yuting
Chen
,
Mengtian
Fan
,
Wenyuan
Huang
,
Yuhang
Yang
,
Shaojun
Xu
,
Yongqiang
Cheng
,
Luke L.
Daemen
,
Jeff
Armstrong
,
Svemir
Rudic
,
William
Thornley
,
Evan
Tillotson
,
Daniel
Lee
,
Sarah
Haigh
,
Shiyu
Fu
,
Floriana
Tuna
,
Eric J. L.
Mcinnes
,
Sihai
Yang
Diamond Proposal Number(s):
[37887, 31729, 36450]
Abstract: Catalytic hydrodeoxygenation (HDO) is critical for bio-oil upgrading, yet the selective cleavage of stable C(sp2)–OH bonds in lignin-derived substrates under aqueous conditions remains a challenge. Here, we report a heteroatomic zeolite catalyst, RuFA/SAPO-34-Nb, featuring few-atom Ru clusters on a Nb(V)-modified SAPO-34 framework, which achieves highly efficient HDO of lignin-derived creosol (2-methoxy-4-methylphenol) in water. Under mild conditions (250 °C, 7 bar H2, 24 h), this catalyst delivers quantitative conversion of creosol to toluene (99.2% conversion, 99.6% selectivity), fully preserving the aromaticity of lignin-derived feedstocks─a key requirement for sustainable production of chemicals. Synchrotron X-ray diffraction, X-ray absorption spectroscopy, and inelastic neutron scattering, combined with theoretical modeling, elucidate the cooperative mechanism: the Nb(V) sites selectively cleave the strong C–O bonds, while the few-atom Ru cluster generates hydrogen species with an exceptionally low rotational barrier of 65 cm–1. This synergistic interaction enables the direct and selective HDO of C(sp2)–O bonds without saturation of the aromatic ring. This work establishes a promissing strategy for aqueous-phase HDO catalysis and provides a general approach for designing bimetallic zeolite catalysts to convert lignin-derived compounds to value-added aromatic chemicals, advancing sustainable biorefinery processes.
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Jan 2026
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E02-JEM ARM 300CF
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Evan David Innes
Tillotson
,
William
Thornley
,
William
Talbott
,
Alexander S.
Eggeman
,
Daria
Kriuchkova
,
Sam
Sullivan-Allsop
,
Matthew
Smith
,
Xuzhao
Liu
,
Ashley
Slattery
,
Pei Lay
Yap
,
Dusan
Losic
,
Zhun
Xu
,
Huan
Wang
,
Jim
Ciston
,
Alexander
Rakowski
,
Stephanie M.
Ribet
,
Benjamin H
Savitzky
,
Manfred Erwin
Schuster
,
Christopher S.
Allen
,
Danielle
Douglas-Henry
,
Valeria
Nicolosi
,
Andrew
Herzing
,
Jacques
O'Connell
,
Ezra J.
Olivier
,
Jan
Neethling
,
Yichao
Zou
,
Ercin Cagan
Duran
,
Rongsheng
Cai
,
Duc-The
Ngo
,
Roman
Gorbachev
,
Jonas
Haas
,
Michael
Schlegel
,
Jannik C.
Meyer
,
Alba
Centeno
,
Amaia
Pesquera
,
Amaia
Zurutuza
,
Sungsu
Kang
,
Jungwon
Park
,
Ivan
Erofeev
,
Utkur
Mirsaidov
,
Colin
Ophus
,
Christian
Rentenberger
,
Thomas
Waitz
,
Jani
Kotakoski
,
Abhijit
Roy
,
Raul
Arenal
,
Andrew
Pollard
,
Sarah
Haigh
Diamond Proposal Number(s):
[29951]
Open Access
Abstract: Standardisation of data collection and analysis is essential to enable commercialisation of 2D materials in a wide range of technologies. Selected area electron diffraction (SAED) in the transmission electron microscope (TEM) is one of the key methods for distinguishing monolayer from bilayer and few-layer graphene by comparing the 1st and 2nd order diffraction spot intensities. Yet there are many factors that can affect the reliability of data collection and interpretation, causing the measurement of monolayer samples to deviate from the literature boundary condition of I{-2110}/I{1-100}<1 for monolayer graphene. Here we present the results of a large interlaboratory SAED comparison study, where 15 international laboratories measured and analysed nominally identical samples of chemical vapour deposited (CVD) graphene. Large variations were observed in the measured ratios of diffraction spot intensities, with the largest variance associated with poor quality SAED data resulting from poor specimen handling and storage. To inform the reliable determination of monolayer thickness from SAED patterns we provide a description of best practice for specimen handling, TEM operation, data collection and analysis. This work was undertaken within VAMAS Technical Working Area (TWA) 41: Graphene and related 2D materials - Project 9, the results of which have been directly incorporated into ISO/TS 21356-2 for the characterisation of graphene sheets. We find that when this methodology is followed, monolayer graphene can be distinguished from bilayer or thicker material with high confidence where analysis of a single SAED pattern gives I{-2110}/I{1-100}<1.2, even in the absence of precise specimen tilting.
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Dec 2025
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E02-JEM ARM 300CF
I09-Surface and Interface Structural Analysis
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Benedikt P.
Klein
,
Matthew A.
Stoodley
,
Joel
Deyerling
,
Luke A.
Rochford
,
Dylan B.
Morgan
,
David G.
Hopkinson
,
Sam
Sullivan-Allsop
,
Henry
Thake
,
Fulden
Eratam
,
Lars
Sattler
,
Sebastian M.
Weber
,
Gerhard
Hilt
,
Alexander
Generalov
,
Alexei
Preobrajenski
,
Thomas
Liddy
,
Leon B. S.
Williams
,
Mhairi A.
Buchan
,
Graham A
Rance
,
Tien-Lin
Lee
,
Alex
Saywell
,
Roman
Gorbachev
,
Sarah J.
Haigh
,
Christopher S.
Allen
,
Willi
Auwärter
,
Reinhard
Maurer
,
David A.
Duncan
Diamond Proposal Number(s):
[25379, 30875, 31695, 31165, 33709]
Open Access
Abstract: Chemical vapour deposition enables large-domain growth of ideal graphene, yet many applications of graphene require the controlled inclusion of specific defects. We present a one-step chemical vapour deposition procedure aimed at retaining the precursor topology when incorporated into the grown carbonaceous film. When azupyrene, the molecular analogue of the Stone–Wales defect in graphene, is used as a precursor, carbonaceous monolayers with a range of morphologies are produced as a function of the copper substrate growth temperature. The higher the substrate temperature during deposition, the closer the resulting monolayer is to ideal graphene. Analysis, with a set of complementary materials characterisation techniques, reveals morphological changes closely correlated with changes in the atomic adsorption heights, network topology, and concentration of 5-/7-membered carbon rings. The engineered defective carbon monolayers can be transferred to different substrates, potentially enabling applications in nanoelectronics, sensorics, and catalysis.
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Sep 2025
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