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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Fei
Guo
,
Manxi
Gong
,
Longxiang
Liu
,
Bochen
Li
,
Ruwei
Chen
,
Mengjun
Gong
,
Wei
Zong
,
Jianuo
Chen
,
Qi
Li
,
Jing
Li
,
Yunpeng
Zhong
,
Zeyi
Zhang
,
Jianrui
Feng
,
Rhodri
Jervis
,
Guanjie
He
Diamond Proposal Number(s):
[34632]
Open Access
Abstract: Platinum–transition metal (PtM) alloys are among the most promising oxygen reduction reaction (ORR) catalysts, yet their practical deployment in proton-exchange membrane fuel cells (PEMFCs) is hindered by transition-metal dissolution, particle coarsening, and insufficient durability. Moreover, conventional alloying or intermetallic ordering strategies often aggravate these issues by inducing severe nanoparticle aggregation and instability. Here we report a controllable alloying–dealloying strategy to construct PtNi nanoparticles confined in an N-doped carbon framework (Pt1Ni1-x@Nix_NC). Ammonia-assisted dealloying produces a Pt-rich shell with an alloyed core, while the N-doped carbon anchors the released Ni atoms form Ni–N/C moieties, thereby suppressing agglomeration and strengthening metal–support interactions. This coordination–support coupling optimizes Pt 5d orbital occupation, weakens oxygen adsorption, and accelerates ORR kinetics. Consequently, Pt1Ni1-x@Nix_NC exhibits a half-wave potential of 0.932 V and an ultrahigh mass activity of 2.028 A mgPt−1, which is 8.75-fold higher than commercial Pt/C and among the best values reported to date for PtNi-based catalysts. Remarkably, it shows only a 6 mV half-wave potential loss after 30,000 cycles, demonstrating exceptional durability. In PEMFCs, the fuel cell delivers 975 mW cm−2 peak power density and retains 91.9% of initial performance, underscoring a generalizable approach for designing durable, high-performance low-PGM catalysts for next generation PEMFCs.
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Feb 2026
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I13-2-Diamond Manchester Imaging
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Will J.
Dawson
,
Andrew R. T.
Morrison
,
Simon M.
Tonge
,
Matthew P.
Jones
,
Myles Kofi
Coke
,
Isabel C.
Antony
,
Kaz
Wanelik
,
Vyacheslav
Kachkanov
,
Partha P.
Paul
,
Bratislav
Lukić
,
Robert S.
Young
,
Zifa
Zuhair
,
James
Parker
,
Inez
Kesuma
,
Gargi
Giri
,
Liam
Bird
,
Alexander J. E.
Rettie
,
Rhodri
Jervis
,
James B.
Robinson
,
Denis
Cumming
,
Thomas S.
Miller
,
Paul R.
Shearing
Diamond Proposal Number(s):
[33315]
Open Access
Abstract: Drying of slurry cast electrodes is amongst the most energy intensive unit operations in battery manufacture. In spite of this, the optimisation of drying processes has been highly empirical, and there remains limited understanding of the interplay between drying dynamics and resulting microstructure. In this work, we used synchrotron X-ray computed microtomography in order to study the formation of mud cracks during the drying process, and evaluate their impact on the electrode microstructure. This was achieved by applying a reduced drying rate, which proved to be an effective means of studying the drying mechanism with a greater resolution and image contrast than otherwise possible. The rate of crack growth is measured, and the differing crack morphology resultant from changes in thickness (between 300 and 800 µm doctor blade gaps) and the presence of air bubbles in the slurry is demonstrated. Digital volume correlation is utilised to identify the specific location of crack formation before these cracks were visible, suggesting image correlation methods as an appropriate tool for process feedback in order to control or eliminate mud cracking. This new approach which enables direct quantification of the evolving microstructure during dynamic drying, in 3D, is therefore transformative in our understanding of the underlying physical processes and will guide rational optimisation of this industrially significant process.
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Feb 2026
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I13-2-Diamond Manchester Imaging
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Iain
Malone
,
Secil
Unsal
,
R. Scott
Young
,
Matthew P.
Jones
,
Francesco
Spanu
,
Shashidhara
Marathe
,
Rhodri
Jervis
,
Hugh G. C.
Hamilton
,
Christopher M.
Zalitis
,
Thomas S.
Miller
,
Alexander J. E.
Rettie
Diamond Proposal Number(s):
[35192]
Open Access
Abstract: Anion exchange membrane water electrolysers are held back by the low durability of the ionomer in the membrane and catalyst layers. Studying ionomer degradation in these systems is challenging because the main mechanisms - which result in catalyst detachment, membrane thinning, and loss of cationic functionality - have opposing effects on the cell potential. Electrochemical measurements alone are therefore insufficient for elucidating the underlying causes of degradation. To address this, a bespoke miniature-electrolyser-cell is developed for X-ray microtomography imaging of membrane electrode assemblies at 1.6 µm resolution. This setup enables the study of the entire active volume of the electrolyser under static and operando conditions and is validated against standard 5 cm2 laboratory cells. An operando investigation of degradation in Fumasep-based catalyst-coated membranes reveals both significant membrane thinning and loss of membrane ionic conductivity during stability testing, leading to increased ohmic resistance and cell potential. In contrast, a Selemion membrane shows minimal changes in thickness and conductivity and is significantly more stable compared to Fumasep when exposed to synchrotron radiation. This platform has relevance for operando studies of electrochemical materials and devices generally, including proton exchange membrane electrolysers, fuel cells, and CO2 electrolysers using both lab-based and synchrotron X-ray sources.
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Sep 2025
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I13-2-Diamond Manchester Imaging
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Matthew P.
Jones
,
Huw C. W.
Parks
,
Alice V.
Llewellyn
,
Hamish T.
Reid
,
Chun
Tan
,
Aaron
Wade
,
Thomas M. M.
Heenan
,
Francesco
Iacoviello
,
Shashidhara
Marathe
,
Paul R.
Shearing
,
Rhodri
Jervis
Diamond Proposal Number(s):
[28650]
Open Access
Abstract: During battery operation, cracking occurs in Nickel Manganese Cobalt (NMC) oxide secondary particles. Cracked particles appear darker in micro-computed tomography (micro-CT) images due to the partial volume effect, where voxels containing both void and solid yield intermediate grey-levels. This work presents an automated method for tracking grey-level changes caused by this effect in large, statistically meaningful micro-CT datasets containing over 10 000 individual particles. It extends earlier work using the GREAT algorithm to analyze NMC particles in tomography images. The new GREAT2 algorithm increases processing speed, from around 1,400 particles per day with GREAT to over 10 000 particles in under a minute. Furthermore, this work introduces methods for automated tracking of grey-level intensity changes in individual particles through different states of charge in an operando experiment. This capability enables temporal analysis of particle degradation mechanisms. Additional data processing methods are presented that extract useful insights. Through this work we show that the large sample sizes, enabled by this method and GREAT2, allow for statistically robust analysis of particle populations. These advances significantly accelerate the tomographic study of cracking in battery electrodes. The GREAT2 algorithm and associated workflows have been made available as the GRAPES Python toolkit.
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Jun 2025
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I13-2-Diamond Manchester Imaging
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Huw C. W.
Parks
,
Matthew
Jones
,
Aaron
Wade
,
Alice
Llewellyn
,
Chun
Tan
,
Hamish
Reid
,
Ralf
Ziesche
,
Thomas M. M.
Heenan
,
Shashidhara
Marathe
,
Christoph
Rau
,
Paul R.
Shearing
,
Rhodri
Jervis
Diamond Proposal Number(s):
[28650]
Open Access
Abstract: To understand fracture behaviour in battery materials, X-ray computed tomography (X-ray CT) has become the primary technique for non-destructive particle and crack analysis. Cracking causes performance decline in polycrystalline NMC811 by exposing new surfaces for parasitic electrolyte reactions and disconnecting active material from the electrode matrix. First cycle crack formation has been documented, but definitive electrochemically induced particle fracture is challenging to assess due to complex sample preparation and high-resolution X-ray imaging requirements. Presented here is an operando X-ray CT technique that enables accurate observation of fracture behaviour during de-/lithiation. A non-linear relationship between fracture behaviour and cell voltage was uncovered, and evidence of particle reformation during re-lithiation. Using a grey level analysis algorithm for fracture detection, we expedite damage evaluation in several thousands of particles throughout the electrochemical process, understanding crack initiation, propagation, and closure on a large, statistical scale and give the ability to track any one of the thousands of particles through its individual electrochemical history. Additionally, we explore the effects of continued volumetric hysteresis on particle damage. For the first time, we demonstrate the complex plurality of fracture behaviour in commercial lithium-ion battery materials, aiding in designing mitigation strategies against particle fracture.
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Mar 2025
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I13-2-Diamond Manchester Imaging
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Diamond Proposal Number(s):
[25254]
Open Access
Abstract: The engineering of biochars with desired morphologies and pore structures is a far-reaching objective towards sustainable pore-dependent environmental technologies, such as water and soil remediation or catalysis. We hereby report a series of experiments that allow the direct following of the shape and porosity of single biochar particles during pyrolysis. Particles ~ 1–2 mm in diameter of unwashed and water-washed raw walnut shells were continuously 3D imaged during pyrolysis to 575 ℃ at a 10 K min−1 in Ar to obtain time- and temperature-resolved x-ray micro computed tomographies to a 0.82 μm resolution. Results showed visual evidence of a 30% and 70% v/v particle shrinkage for unwashed and washed samples, respectively. Particle swelling between 200 and 300 ℃ in the unwashed sample provided evidence of the softening of native biopolymers associated with lignin in untreated biomass. A purpose-defined parameter Λ shows the temperature-dependence of pore re-distribution towards the center of the particle to be linear for both samples. Λ was found to be in the washed sample, approximately 3.5 times faster than in the unwashed one. Such linear dependence is significantly slower than an exponential Arrhenius-like trend thereby providing a qualitative measure of the heat and mass transport phenomena limiting the chemical reactions in the porous medium. This evidence is key to resolving the pathways to the thermochemical decomposition of biomass leading to preparation of precision-engineered biochars.
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Oct 2024
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I12-JEEP: Joint Engineering, Environmental and Processing
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Donal P.
Finegan
,
Julia
Billman
,
Jacob
Darst
,
Peter
Hughes
,
Jesus
Trillo
,
Matt
Sharp
,
Alex
Benson
,
Martin
Pham
,
Inez
Kesuma
,
Mark
Buckwell
,
Hamish T.
Reid
,
Charlie
Kirchner-Burles
,
Matilda
Fransson
,
David
Petrushenko
,
Thomas M. M.
Heenan
,
Rhodri
Jervis
,
Rhodri
Owen
,
Drasti
Patel
,
Ludovic
Broche
,
Alexander
Rack
,
Oxana
Magdysyuk
,
Matt
Keyser
,
William
Walker
,
Paul
Shearing
,
Eric
Darcy
Diamond Proposal Number(s):
[24112, 20903, 17641]
Open Access
Abstract: The thermal response of Li-ion cells can greatly vary for identical cell designs tested under identical conditions, the distribution of which is costly to fully characterize experimentally. The open-source Battery Failure Databank presented here contains robust, high-quality data from hundreds of abuse tests spanning numerous commercial cell designs and testing conditions. Data was gathered using a fractional thermal runaway calorimeter and contains the fractional breakdown of heat and mass that was ejected, as well as high-speed synchrotron radiography of the internal dynamic response of cells during thermal runaway. The distribution of thermal output, mass ejection, and internal response of commercial cells are compared for different abuse-test conditions, which when normalized on a per amp-hour basis show a strong positive correlation between heat output from cells, the fraction of mass ejected from the cells, their energy- and power-density. Ejected mass was shown to contain 10 × more heat per gram than non-ejected mass. The causes of ‘outlier’ thermal and ejection responses i.e., extreme cases, are elucidated by high-speed radiography which showed how occurrences such as vent clogging can create more hazardous conditions. High-speed radiography also demonstrated how the time-resolved interplay of thermal runaway propagation and mass ejection influences the total heat generated.
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Mar 2024
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I12-JEEP: Joint Engineering, Environmental and Processing
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Arthur
Fordham
,
Zoran
Milojevic
,
Emily
Giles
,
Wenjia
Du
,
Rhodri E.
Owen
,
Stefan
Michalik
,
Philip A.
Chater
,
Prodip K.
Das
,
Pierrot S.
Attidekou
,
Simon M.
Lambert
,
Phoebe K.
Allan
,
Peter R.
Slater
,
Paul A.
Anderson
,
Rhodri
Jervis
,
Paul R.
Shearing
,
Dan J. I.
Brett
Diamond Proposal Number(s):
[27719]
Open Access
Abstract: The growing demand for electric vehicles (EVs) continues to raise concern for the disposal of lithium-ion batteries reaching their end of life (EoL). The cells inside EVs age differently depending on multiple factors. Yet, following extraction, there are significant challenges with characterizing degradation in cells that have been aged from real-world EV usage. We employed four non-destructive techniques—infrared thermography, ultrasonic mapping, X-ray tomography, and synchrotron X-ray diffraction—to analyze the aging of Nissan Leaf large-format pouch cells that were arranged in different orientations and locations within the pack. The combination of these methods provided complementary insights into cell degradation, with rotated/vertically aligned cells exhibiting distinct aging patterns compared with flat/horizontally aligned cells. These findings offer valuable information for pack design and demonstrate how cost-effective non-destructive techniques can provide practical assessment capabilities comparable to synchrotron studies. This approach enables decision support during EoL, enhancing battery production efficiency and minimizing material waste.
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Nov 2023
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I11-High Resolution Powder Diffraction
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Andrew Stephen
Leach
,
Alice
Llewellyn
,
Chao
Xu
,
Chun
Tan
,
Thomas M. M.
Heenan
,
Alex
Dimitrijevic
,
Karin
Kleiner
,
Clare P.
Grey
,
Dan J. L.
Brett
,
Chiu C.
Tang
,
Paul R.
Shearing
,
Rhodri
Jervis
Diamond Proposal Number(s):
[22498, 24122]
Open Access
Abstract: Understanding the performance of commercially relevant cathode materials for lithium-ion (Li-ion) batteries is vital to realize the potential of high-capacity materials for automotive applications. Of particular interest is the spatial variation of crystallographic behavior across (what can be) highly inhomogeneous electrodes. In this work, a high-resolution X-ray diffraction technique was used to obtain operando transmission measurements of Li-ion pouch cells to measure the spatial variances in the cell during electrochemical cycling. Through spatially resolved investigations of the crystallographic structures, the distribution of states of charge has been elucidated. A larger portion of the charging is accounted for by the central parts, with the edges and corners delithiating to a lesser extent for a given average electrode voltage. The cells were cycled to different upper cutoff voltages (4.2 and 4.3 V vs. graphite) and C-rates (0.5, 1, and 3C) to study the effect on the structure of the NMC811 cathode. By combining this rapid data collection method with a detailed Rietveld refinement of degraded NMC811, the spatial dependence of the degradation caused by long-term cycling (900 cycles) has also been shown. The variance shown in the pristine measurements is exaggerated in the aged cells with the edges and corners offering an even lower percentage of the charge. Measurements collected at the very edge of the cell have also highlighted the importance of electrode alignment, with a misalignment of less than 0.5 mm leading to significantly reduced electrochemical activity in that area.
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Jan 2022
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