I12-JEEP: Joint Engineering, Environmental and Processing
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Ronan
Docherty
,
Sam
Riley
,
John D.
Morley
,
Evangelos
Papoutsellis
,
Antonia
Bobitan
,
Jack
Donoghue
,
Kathryn
Rankin
,
Fernando
Alvarez-Borges
,
Luis E.
Salinas Farran
,
Stefan
Michalik
,
Alexander
Liptak
,
Genoveva
Burca
,
Pierre-Olivier
Autran
,
Jonathan
Wright
,
Winfred
Kockelmann
,
Olof
Gutowski
,
Ann-Christin
Dippel
,
Martin
Von Zimmermann
,
Dorota
Matras
,
Bartlomiej
Winiarski
,
John S.
Mangum
,
Melissa
Popeil
,
Donal P.
Finegan
,
James A.
Gott
,
Daniela
Proprentner
,
Geoff
West
,
Louis F. J.
Piper
,
Hongyang
Dong
,
Matthew P.
Jones
,
Francesco
Iacoviello
,
Alice V.
Llewellyn
,
Rhodri
Jervis
,
Yuta
Kimura
,
Koji
Amezawa
,
Oki
Sekizawa
,
Mahmoud
Ardakani
,
Aigerim
Omirkhan
,
Mary P.
Ryan
,
James O.
Douglas
,
Siyang
Wang
,
Finn
Giuliani
,
Neil
Mulcahy
,
Shelly
Conroy
,
Chandramohan
George
,
Andrew M.
Beale
,
Simon
Jacques
,
Samuel J.
Cooper
,
Antonios
Vamvakeros
Diamond Proposal Number(s):
[36699, 38628]
Open Access
Abstract: Battery research increasingly relies on advanced imaging, yet open access to such data remains rare, scattered across various sources, and difficult to find. The Battery Imaging Library (BIL) is the first open, curated collection of multi-modal and multi-length scale battery imaging datasets, accompanied by a searchable, FAIR-compliant website. Distinctive features include the release of raw experimental data (radiographs, sinograms, X-ray and electron diffraction patterns) together with rare operando and multi-resolution datasets. Each dataset is linked to Zenodo DOIs with metadata, ensuring persistence and citability; open-source Python scripts for preprocessing and reconstruction are also provided for various CT modalities. BIL enables algorithm benchmarking, machine learning, and teaching using experimental and industrially relevant data. By combining coverage across modalities, length scales, and chemistries with raw data accessibility and a FAIR-aligned web platform, the Battery Imaging Library provides a foundation for openness and reproducibility in battery imaging. The library is available here: https://www.batteryimaginglibrary.com
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Sep 2026
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B18-Core EXAFS
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Diamond Proposal Number(s):
[45829]
Open Access
Abstract: Glycerol is an underutilized waste product that is abundantly available from the biodiesel industry. Electrocatalytic oxidation of glycerol (GOR) to formate offers an environmentally friendly and cost-effective approach to valorizing glycerol. In this study, we have developed new types of metal-doped cobalt metal-organic frameworks, which are grown directly on a carbon matrix via a one-pot synthesis as electrocatalyst precursors. In-depth structural analysis has revealed that, in the Ni-doped cobalt MOF, Ni substitutes a fraction of Co sites isomorphically, forming isolated Ni(II) centers, while Cu is present as a mixture of Cu(II) and metallic Cu, with the majority in the oxidized form as highly dispersed species and a small fraction forming nanoparticles. These materials were then subjected to a controlled potential-induced surface reconstruction to produce mixed-metal oxide/oxyhydroxide-like environments interconnected through M-O-M motifs, the extent of the reconstruction depending strongly on the dopant metal. The metal-doped derivatives were tested as electrocatalysts for the alkaline electrooxidation of glycerol using in-house designed electrochemical reactors with different cell configurations and operating modes. We demonstrated that metal-doped derivative phases exhibit improved electrocatalytic activity for GOR compared to the monometallic counterpart. These catalysts yield significant glycerol conversion rates under single-pass operation, with improved Faradaic efficiencies towards formate (up to 70%) and low energy consumption (< 320 kWh kmol−1), while suppressing the complete oxidation of glycerol to carbonate or CO2. This work provides new insight into the rational design of metal-doped MOF derivatives as highly active and selective electrocatalysts for the practical glycerol valorization.
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Aug 2026
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B18-Core EXAFS
E02-JEM ARM 300CF
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Donato
Decarolis
,
Sahra
Ahmed
,
James
King
,
Alin-Marin
Elena
,
Linda
Zhang
,
Jeff
Armstrong
,
Ines
Lezcano-Gonzalez
,
Mohsen
Danaie
,
Michael
Hirscher
,
Simone
Meloni
,
Andrew M.
Beale
,
Petra A.
Szilagyi
Diamond Proposal Number(s):
[42564]
Open Access
Abstract: Metal–organic frameworks have been intensively investigated for their ability to effectively control the growth and surface chemistry of nanosized guests, with their pores acting as templates and potentially providing anchoring sites. Since the speciation, as determined by the geometry and surface chemistry of hydride-forming metals, such as Pd, under particular conditions (T, p), is controlled by their size at and beyond the nanoscale, metal–organic frameworks are a prospective matrix for speciation or phase selection. This is of relevance because the role and characteristics of the phases in hydrogenation reactions involving hydride-forming Pd catalysts are open questions. In particular, it is a matter of debate which palladium phase is the most active and most selective, as they often occur simultaneously under catalytic conditions. For the first time, our thorough investigation, including operando XAFS and computer simulations, demonstrates that by embedding Pd nanoclusters, ≤1 nm in diameter, in the pores of the NH2–UiO-66 metal–organic framework, the speciation of subnanometric Pd particles can be controlled, such that the active particles only exist in their metallic state under reaction conditions; in fact, the Pd–H2 mixture only affords surface-bound hydrogen atoms. This control of Pd speciation consequently enables the direct probing of the phase activity and selectivity in the model reaction of 1,3-butadiene hydrogenation to butenes, wherein it showed no deactivation and improved selectivity compared to conventionally prepared catalytic systems. This result shows that the metallic phase can be stabilized through subnanometric size control and that it is more selective and less prone to overhydrogenating the butadiene reactant to butane, resulting in a purer product.
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Jun 2026
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I15-1-X-ray Pair Distribution Function (XPDF)
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Danial
Farooq
,
Lucy
Costley-Wood
,
Sebastian
Stockenhuber
,
Antonis
Vamvakeros
,
Stephen
Price
,
Lisa
Allen
,
Jakub
Drnec
,
James
Paterson
,
Mark
Peacock
,
Daniel J. M.
Irving
,
Philip A.
Chater
,
Andrew M.
Beale
Diamond Proposal Number(s):
[30639]
Open Access
Abstract: The transition to net-zero emissions hinges on circular economy strategies that valorize waste and enhance resource efficiency. Among X-to-liquid (XTL) technologies, the Fischer-Tropsch (FT) process stands out for converting biomass, waste, and CO2 into hydrocarbons and chemicals, especially when powered by renewable hydrogen. Cobalt-based catalysts are preferred in FT synthesis due to their efficiency and CO2 tolerance, yet their catalytic performance is closely tied to their polymorphic structures─face-centered cubic (FCC), hexagonal close-packed (HCP), and stacking-faulted intergrowths thereof. HCP cobalt has been shown to exhibit high activity and selectivity for higher hydrocarbons and oxygenates, particularly when transformed into cobalt carbide (Co2C), which forms more readily at low H2/CO ratios. This study presents a quantitative analysis of cobalt polymorphs and stacking faults in Mn-promoted Co/TiO2 FT catalysts from in situ powder X-ray diffraction (XRD) data and X-ray Diffraction Computed Tomography (XRD-CT) data from spent catalysts in order to obtain a more complete correlation of structural features with catalytic performance. By modeling stacking fault probabilities using supercell simulations, the proportion of faulted FCC and HCP domains was determined across varying Mn loadings (0–5%). Increased Mn loading was found to decrease stacking faults in the FCC phase while increasing them in HCP, promoting the formation of HCP domains and ultimately Co2C under reaction conditions. Notably, the 3% Mn-loaded sample showed a marked rise in HCP content and Co2C formation, correlating with the highest observed alcohol and olefin selectivity. These findings highlight a critical structure–function relationship: Mn facilitates a transformation from FCC to HCP and then to Co2C, this final transition driven by similar stacking sequences and metal–support interactions. The findings show that Mn promotion not only stabilizes smaller Co particles and enhances its dispersion, but also modulates the distribution of Co polymorphs and stacking faults, leading to altered catalytic behavior. This highlights the importance of stacking fault characterization for optimizing FT catalyst design and performance, and suggests pathways to more efficient and selective carbon-neutral fuel production through engineered polymorphic and interfacial structures.
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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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E01-JEM ARM 200CF
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Naomi
Lawes
,
Igor
Kowalec
,
Sofia
Mediavilla-Madrigal
,
Kieran J.
Aggett
,
Louise R.
Smith
,
Malcolm
Dearg
,
Thomas J. A.
Slater
,
Eimear
Mccarthy
,
Herzain I.
Rivera-Arrieta
,
Matthias
Scheffler
,
David J.
Morgan
,
David J.
Willock
,
Andrew M.
Beale
,
Andrew J.
Logsdail
,
Nicholas F.
Dummer
,
Michael
Bowker
,
C. Richard A.
Catlow
,
Stuart H.
Taylor
,
Graham J.
Hutchings
Diamond Proposal Number(s):
[3104]
Open Access
Abstract: A series of PdZn/TiO2 catalysts prepared by chemical vapor impregnation (CVI) were tested for CO2 hydrogenation at 20 bar pressure and at temperatures of 230–270 °C. Changing the Pd and Zn molar ratio (Zn:Pd = 0–20) in a PdZn/TiO2 catalyst has a dramatic effect on selectivity for the CO2 hydrogenation reaction. Pd alone shows three main products: methanol, CO, and methane. Addition of small quantities of Zn results in the formation of a PdZn alloy, preventing methanation. At equimolar ratios of Pd and Zn, a 1:1 β-PdZn alloy is formed and a reverse water gas shift catalyst is produced. Adding Zn in excess relative to the Pd loading results in the formation of ZnO on the TiO2 surface in addition to the PdZn alloy, dramatically increasing methanol selectivity from 5% at Zn:Pd = 1 to 55% for Zn:Pd = 2. Through a combination of theory and experiment, the active site for methanol synthesis is concluded to be the interface between PdZn nanoparticles and the ZnO overlayer on the TiO2, where interfacial formate can react with hydrogen dissociated by the metal nanoparticle.
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Jan 2026
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B18-Core EXAFS
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Diamond Proposal Number(s):
[29948]
Open Access
Abstract: Direct hydrogenation of carbon dioxide to methanol is a promising strategy for carbon capture and utilization (CCU). Copper–zinc–alumina (CZA) catalysts are widely used for this transformation, yet the nature of the active Cu and Zn species and the reaction intermediates remains debated due to their sensitivity to feed composition and temperature. This challenge is compounded by the high metal loading in conventional CZA catalysts, which obscures active species signals with background contributions from spectator species. To address this, we synthesized model CuZn/Al2O3 catalysts using bimetallic coordination complexes, achieving low metal loadings that yield small Cu clusters and Cu+ single atoms adjacent to isolated Zn2+ sites. In situ XANES and UV–vis data were analyzed using multivariate curve resolution–alternating least-squares (MCR–ALS), revealing that Cu dispersion and reagglomeration─phenomena suspected in industrial systems─also occur at low loadings. Operando and modulation excitation with phase sensitive detection DRIFTS (ME-PSD-DRIFTS) showed: (a) Cu clusters dissociate H2 and activate CO2 via monodentate formate; (b) Al2O3 stabilizes Cu+ under reducing conditions, with Cu content correlating with methanol productivity via CO hydrogenation; and (c) Zn in ZnAl2O4 promotes CO2 activation through reactive carbonate formation and enhances oxygenate conversion kinetics. ZnAl2O4 also acts as a structural promoter, facilitating CO2 conversion via reverse water gas shift (RWGS) and CO hydrogenation. These findings reveal new structure–activity relationships, highlighting the role of the mixed-metal interface in stabilizing transient intermediates and providing some guidance in the rational design of improved catalysts for CO2 valorization.
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Nov 2025
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B18-Core EXAFS
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Diamond Proposal Number(s):
[38597]
Open Access
Abstract: Extra-large-pore Ge-containing GTM chiral zeolite catalysts have recently proved useful asymmetric catalysts, with chirality emerging from their chiral confined nanospace. However, so far these exceptional materials have suffered from low framework stability in the presence of water and moderate catalytic enantioselectivity in the ring-opening of chiral trans-stilbene oxide with 1-butanol used as a test reaction. Here, we report that these chiral zeolite catalysts can be easily stabilized upon exposure of the calcined material to 1-butanol, providing stability against water and, most importantly, prompting a preactivation of the chiral active sites that boosts their enantioselective properties, reaching unprecedented enantiomeric excesses up to 88% where one enantiomer reacts 16 times more than the other. A range of physicochemical studies, including in situ Fourier transform infrared (FTIR) and X-ray absorption spectroscopy, indicates that framework Ge sites increase their coordination environment upon interaction with 1-butanol molecules, which after a thermal treatment above 100 °C remain irreversibly bound to Ge as a consequence of a condensation and dehydration reaction, providing a route to easily functionalize these materials. These preactivated GTM asymmetric catalysts act similarly to enzymes by controlling the confinement of the chiral reactants in particular orientations through coordination with Ge and development of H-bonds with nearby hydroxyl groups, thus attaining enantioselective catalytic activities close to those reached by enzymatic systems but with the crucial advantage associated with heterogeneous catalysts and, notably, the possibility of preparing both enantiomeric versions of the catalyst by using an easily accessible alkaloid.
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Oct 2025
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B18-Core EXAFS
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Diamond Proposal Number(s):
[42561]
Open Access
Abstract: A novel methodology is presented for preparing non-noble metal-based heterogeneous catalysts doped with low amounts of noble metals, yielding highly active and reusable materials for sustainable organic transformations. A new Co–Ru@C catalyst was developed by incorporating small ruthenium nanoparticles (1 wt %) and cobalt nanoparticles (10 wt %) on Vulcan carbon via pyrolysis of a ruthenium-doped cobalt metal–organic framework supported on carbon (2D-Co(Ru)MOF/C). Advanced characterization (in situ PXRD and XAS, HAADF-STEM, HRTEM) confirmed strong Co–Ru interactions, enhancing catalytic activity. The catalyst was evaluated in the one-pot reductive amination of dinitrobenzenes to benzimidazoles using molecular hydrogen and water, which is in line with green chemistry. The synergistic effect between Co and Ru enabled quantitative product yields under significantly milder reaction conditions than the existing ones. In addition, ruthenium was found to facilitate hydrogen activation in the bimetallic material compared with its undoped Co@C counterpart. Regarding stability, the Co–Ru@C catalyst retained its activity over at least five consecutive cycles without metal leaching or structural degradation. This material demonstrated a broad substrate scope, affording over 20 functionalized benzimidazoles in high yields. Half-gram-scale syntheses of commercial Diabazole and Fuberidazole further validated the scalability of this approach.
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Sep 2025
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B18-Core EXAFS
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Diamond Proposal Number(s):
[40577]
Open Access
Abstract: Mitigating climate change is one of the biggest challenges of today's society. The most direct way to achieve this goal is to capture and use CO2 as a source of energy and chemicals. This work, inspired by previous publications focused on homogeneous catalysis, proposes the transformation of the easy-to-prepare CO2 derivatives dialkylureas into C1 chemicals using Ru-MOFs as heterogeneous catalysts. This choice is due to (i) the well-known ability of Ru to catalyze hydrogenation reactions and (ii) that Ru-complexes were the pioneer homogenous catalyst in converting CO2 into an added-value C1 chemical, methanol. Apart from the already reported MOF Ru-HKUST-1, we have prepared a new Ru-MOF material, denoted Ru-BTC, analogous to the semiamorphous Fe-BTC. It has been found by XAS that Ru-BTC and Ru-HKUST-1 have different metal environment and oxidation states: only 3+ in Ru-BTC, a 50:50 mixture of 2+ and 3+ in Ru-HKUST-1. Both Ru-MOFs catalyzed the hydrogenation of N,N’-dimethylurea under relatively mild conditions, giving methane as the main product. Ru-BTC was particularly efficient: 67 % conversion and 96 % selectivity to CH4 at 150 ºC and 30 bars of H2 using a Ru/dimethylurea weight ratio of 1 %. Ru-MOFs were also able to transform CO2 into CH4, again being Ru-BTC the most effective catalyst, but giving much poorer selectivity to CH4. Ru-MOFs, particularly Ru-BTC, were damaged under reaction conditions, but no significant Ru leaching was observed.
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Jul 2025
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