I14-Hard X-ray Nanoprobe
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F.
Dal Molin
,
D.
Hunt
,
A.
Dewar
,
S.
Lozach
,
C.
Phillips
,
B.
Thomas
,
L.
Warford
,
J. E.
Parker
,
J.
Walker
,
M.
Chocholek
,
D. M.
Paterson
,
H.
Woodward-Rowe
,
N.
Hicks
Diamond Proposal Number(s):
[35954]
Open Access
Abstract: Although oil and gas (O&G) derived produced waters and drill cuttings are known to contain enhanced levels of naturally occurring radium-228 (228Ra) and radium-226 (226Ra), most relevant ecological impact assessments have excluded radiological hazards and focus on other important contaminants, such as hydrocarbons and metals. Also, due to restricted access to the delimiting safety zone around operational O&G platforms, the few previous radioecological risk assessment studies have been conducted using seawater samples collected far from the main discharge point and applying default dilution and transfer factors to estimate concentrations of contaminants in biota. In this case study, sediment cores were collected close to a former O&G platform, Northwest Hutton (NWH), that used to be in the UK North Sea (61.11N, 1.31E). The sediment materials were analysed by gamma spectrometry and ICP-MS to confirm the presence of particles enriched in natural radioactivity. Benthic macrofaunal assemblages in the surrounding seabed were also characterised and one of the dominant species was selected for additional nano-hard X-Ray Fluorescence (nano-XRF) imaging to confirm the exposure pathways and refine the radioecological risk assessment using the ERICA tool. This novel approach for estimating dose rates was found to be less conservative than more traditional approaches using the ERICA default concentration ratio for 228Ra and 226Ra. The dose rate estimations were confirmed to be significantly lower than the ERICA screening level of 10μGy/h, in agreement with findings from previous studies.
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Mar 2025
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I18-Microfocus Spectroscopy
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Diamond Proposal Number(s):
[29808]
Open Access
Abstract: Historical disposal of coal mine wastes in the coastal zone has left a significant environmental pollution legacy. Climate change is increasing the likelihood that erosion of these wastes will lead to release of metal(loid)s to coastal environments. Whilst previous research has focussed on the generation of acidic, metal-rich waters from coal mine wastes in freshwater environments, a comprehensive investigation of metal(loid) leaching from such wastes in the coastal zone has not been undertaken. This study investigated the leaching behaviour of coal mine wastes under freshwater and saline conditions and determined the impacts of spatial heterogeneity of waste composition on such behaviour. The degree of leaching varied considerably within and between sites due to the heterogenous nature of the waste. Leachate pH varied from 1.80 to 6.99 with acidic leachates particularly enriched in Fe (≤17,000 mg/kg dry waste) and sulfate (≤48,000 mg/kg dry waste) due to dissolution of acid sulfate phases. Dissolution of Fe and Mn oxides, hydroxides and oxyhydroxides also led to release of surface adsorbed metal(loid)s such as As (≤21 mg/kg dry waste), Zn (≤86 mg/kg dry waste) and Cu (≤14 mg/kg dry waste). Adsorption of As to high surface area minerals was confirmed by X-ray Absorption Near Edge Spectroscopy (XANES) analysis. Metal(loid) release was typically lower in the presence of seawater than deionised water due to the greater pH buffering capacity of seawater. This research provides an insight into the considerable challenges faced by coastal managers globally as they seek to mitigate the risks from such legacy pollution.
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Mar 2025
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I14-Hard X-ray Nanoprobe
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Diamond Proposal Number(s):
[28688]
Open Access
Abstract: Understanding the interactions between metal-based nanoparticles and biological systems in complex environments (e.g., the human body, soils, and marine settings) remains challenging, especially at the single-cell and nanoscale levels. Capturing the dynamics of these interactions, such as metal distribution, nanoparticle growth, or degradation, in their native state (in vivo) is particularly difficult. Here, we demonstrate the direct measurement of iron content in hydrated, magnetite-biomineralizing magnetotactic bacteria using synchrotron-based nanobeam–scanning X-ray fluorescence microscopy combined with a liquid cell environment. In addition to X-ray fluorescence imaging, we collected iron chemical speciation information from individual bacteria in liquid using X-ray absorption spectroscopy. To follow biomineralization in situ, we developed a microfluidic device to track magnetite nanoparticle formation over several hours under the X-ray beam. This approach highlights the potential of X-ray fluorescence microscopy in liquid cell setups to provide elemental and chemical insights into biological processes at the single-cell level. Combining X-ray nanobeam techniques with liquid cell devices will enable more “on-chip” experiments on metals in biological contexts to be conducted at the synchrotron.
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Mar 2025
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I14-Hard X-ray Nanoprobe
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Diamond Proposal Number(s):
[23602, 28688]
Open Access
Abstract: Coccolithophore microalgae intracellularly produce nanostructured calcitic platelets, known as coccoliths, through a biologically-controlled mineralization process. Mature coccoliths are secreted to the cell surface and assembled into a shell that envelops the cell. The large-scale global production of coccoliths, followed by their sedimentation to the ocean floor, significantly contributes to carbon cycling. Despite progress in understanding the biomineralization pathway of coccoliths, we are still limited in our ability to predict how future climate conditions will impact coccolith formation and thus ocean carbon fluxes. Investigating coccolith biomineralization at the single-cell level is therefore critical to advance our understanding but remains challenging since current imaging techniques lack the combined spatial and temporal resolution coupled with element-specific detection to follow processes in situ. In light of this gap, nanobeam-scanning X-ray fluorescence microscopy (nano-XRF) in the hard X-ray regime is employed here to investigate the intracellular elemental distribution of the coccolithophore Gephyrocapsa huxleyi (formerly Emiliania huxleyi) achieving a resolution of 100 nm and elemental detection from phosphorus (P) to zinc (Zn). Calcium- and phosphorus-rich intracellular bodies, previously proposed to be involved in coccolith biomineralization, were observed in cells initially prepared ex situ by drying. Interestingly, nano-XRF imaging reveals metal species (e.g., Mn, Fe, Zn) within these bodies that were not detected in earlier studies, suggesting multiple biological roles for these structures. Moving towards native-state imaging, G. huxleyi was then imaged in hydrated state using a dedicated liquid cell device. Measurements were performed on G. huxleyi cells both with and without coccolith shell in sea water medium and compared to those of dried cells, demonstrating comparable image quality. The future potential and limitations of liquid cell nano-XRF imaging for coccolithophores and other microorganisms are further discussed.
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Mar 2025
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I14-Hard X-ray Nanoprobe
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Dominic
Blackburn
,
Nathan S.
Hill
,
Christopher J.
Wood
,
Tamilselvan
Velusamy
,
Balder A.
Nieto-Díaz
,
Caitlin
Woolley
,
Andy
Brown
,
Loukas
Zampelis
,
Trevor
Mcardle
,
Molly
Worth
,
Timothy
Thornber
,
Ibrahim
Albariqi
,
Rachel C.
Kilbride
,
Tingxiang
Yang
,
C. Neil
Hunter
,
Graham J.
Leggett
,
George
Koutsourakis
,
James C.
Blakesley
,
Fernando A.
Castro
,
David
Beynon
,
Trystan M.
Watson
,
Dumitru
Sirbu
,
David G.
Lidzey
Diamond Proposal Number(s):
[32789]
Open Access
Abstract: We fabricate a type of back-contact perovskite solar cell based on 1.5 μm-width grooves that are embossed into a plastic film whose opposing “walls” are selectively coated with either n- or p-type contacts. A perovskite precursor solution is then deposited into the grooves, creating individual photovoltaic devices. Each groove device is series-connected to its neighbors, creating minimodules consisting of hundreds of connected grooves. Here, we report on the fabrication of groove-based devices using slot-die coating to deposit the perovskite precursor and explore the structure of the perovskite in the grooves using a range of microscopy and spectroscopy techniques. Significantly, our devices do not contain any expensive or scarce elements such as indium, indicating that this technology is both sustainable and low-cost. Furthermore, all coating processes explored here were performed using roll-to-roll processing techniques. Our technology is therefore completely scalable and is consistent with high-throughput, low-cost manufacturing.
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Feb 2025
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I18-Microfocus Spectroscopy
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Thomas
Barthelay
,
Robert
Gray
,
Howard
Richards
,
Paloma
Rodriguez Santana
,
Sylvia
Britto
,
Kalotina
Geraki
,
Zhenyuan
Xia
,
Johanna
Xu
,
Leif E.
Asp
,
Chris
Bowen
,
Frank
Marken
,
Alexander
Lunt
,
Andrew
Rhead
Diamond Proposal Number(s):
[30127]
Open Access
Abstract: Structural batteries utilise the bifunctionality of carbon fibres to act as a load-bearing structure, but also as a conductive current collector for a battery electrode. Lithium-ion transport during the cycling of structural battery cathodes coated with different morphologies is investigated using Iron X-Ray Absorption Near Edge Spectroscopy (Fe XANES) and correlated to electrochemical performance. Two contrasting morphologies were produced using slurry coating and electrophoretic deposition (EPD) of lithium-iron phosphate (LFP) onto continuous carbon fibres. The ability to study the different structural battery cathode morphologies operando allows for a comparative analysis of their impact on cycling performance. The EPD-coated fibres exhibited a more homogeneous, thinner coating around the fibre compared to the thick, one-sided coating produced using slurry coating. Despite a lower initial capacity and 30 % lithium re-intercalation loss in the first cycle, EPD-coated fibres exhibited more stable capacity retention over time compared to slurry-coated counterparts. Electrochemical Impedance Spectroscopy (EIS) revealed initially high ionic resistance for the EPD-coated fibres, but a larger increase in resistance in the slurry coated electrodes over multiple cycles. This study demonstrated an innovative and novel method of analysing in greater detail, the cycling ability of the coated cathode material on carbon fibres using synchrotron radiation.
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Feb 2025
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I14-Hard X-ray Nanoprobe
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Ruwei
Chen
,
Yunpeng
Zhong
,
Peie
Jiang
,
Hao
Tang
,
Fei
Guo
,
Yuhang
Dai
,
Jie
Chen
,
Jingyi
Wang
,
Jiyang
Liu
,
Song
Wei
,
Wei
Zhang
,
Wei
Zong
,
Fangjia
Zhao
,
Jichao
Zhang
,
Zhengxiao
Guo
,
Xiaohui
Wang
,
Guanjie
He
Diamond Proposal Number(s):
[36785]
Open Access
Abstract: Long-standing challenges including notorious side reactions at the Zn anode, low Zn anode utilization, and rapid cathode degradation at low current densities hinder the advancement of aqueous zinc-ion batteries (AZIBs). Inspired by the critical role of capping agents in nanomaterials synthesis and bulk crystal growth, a series of capping agents are employed to demonstrate their applicability in AZIBs. Here, it is shown that the preferential adsorption of capping agents on different Zn crystal planes, coordination between capping agents and Zn2+ ions, and interactions with metal oxide cathodes enable preferred Zn (002) deposition, water-deficient Zn2+ ion solvation structure, and a dynamic cathode-electrolyte interface. Benefiting from the multi-functional role of capping agents, dendrite-free Zn plating and stripping with an improved Coulombic efficiency of 99.2% and enhanced long-term cycling stability are realized. Remarkable capacity retention of 91% is achieved for cathodes after more than 500 cycles under a low current density of 200 mA g−1, marking one of the best cycling stabilities to date. This work provides a proof-of-concept of capping agents in manipulating electrochemical behaviors, which should inspire and pave a new avenue of research to address the challenges in practical energy storage beyond AZIBs.
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Jan 2025
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I18-Microfocus Spectroscopy
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Diamond Proposal Number(s):
[35162]
Open Access
Abstract: The quantitative characterization of the structure of biomineral surfaces is needed for guiding regenerative strategies. Current techniques are compromised by a requirement for extensive sample preparation, limited length-scales, or the inability to repeatedly measure the same surface over time and monitor structural changes. We aim to address these deficiencies by developing Calcium (Ca) K-edge Polarisation Induced Contrast X-ray Fluorescence (PIC-XRF) to quantify hydroxyapatite (HAp) crystallite structural arrangements in high and low textured surfaces. Minimally prepared human dental enamel was used as an exemplar to quantify initial surface structures, and the disruption caused by short dietary acid exposures. By measuring surfaces at different rotational angles relative to a polarised focused (2x2µm) monochromatic X-ray source (at either 4049.2 and 4051.1 eV) it was possible to discriminate the principal and secondary orientations of surface crystallites, along with their texture. It was also possible to quantify the organisation of crystallites in both low (enamel cross-sections) and highly textured (facial enamel) surfaces including the identification of crystallites aligned perpendicular to the surface—a challenge for other synchrotron techniques. Surface modifications following short term acid erosion (affecting <20µm of the enamel surface depth) were detected as significant shifts in principal crystallite orientation (p<0.001) and as a marked reduction in surface texture (p<0.001). Findings suggest preferential dissolution of HAp based on crystallite angular orientation. We demonstrate that PIC-XRF is a powerful tool to quantify biomineral surfaces, with minimal sample preparation that enables monitoring of surface structural changes through repeated measurements.
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Jan 2025
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I14-Hard X-ray Nanoprobe
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Diamond Proposal Number(s):
[27292]
Open Access
Abstract: Soil aggregation is a dynamic process influenced by physical, chemical and biological factors; however, their individual and combined effect on the formation and turnover of aggregates is not well understood. The aim of this study was to examine incorporation of fresh litter inputs of different physicochemical properties including their carbon-to-nitrogen (C/N) ratio – maize (C/N = 12) and straw (C/N = 103) - into aggregates, de novo formed from mineral soil with or without the presence of microbiota. Using rare-earth element oxides, we labelled structures formed during a four-week incubation with a single litter type and traced their incorporation into newly formed aggregates after mixing them together and incubating for a subsequent seven-week period. To visualize them, we used synchrotron-based X-ray fluorescence microspectroscopy, which allowed us to demonstrate that presence of the plant-derived particulate organic matter was the key factor for the aggregate formation. Within the timescale of the experiment, neither microbial abundance nor the community composition had any significant effect. However, the relative increase in straw-associated soil in aggregates larger than 250 μm provided support for our hypothesis regarding impact of carbon-rich organic matter on macroaggregation, likely via promotion of fungal growth and hyphal enmeshing. Phospholipid fatty acid analysis further confirmed relatively higher abundance of fungi in macroaggregates in straw-containing soil. All in all, our study provides insights into the initial stages of aggregate formation following litter additions and development of associated microbial community. The spatial analysis enabled by the X-ray fluorescence microspectroscopy enabled visualization of internal aggregate structures, shedding light on the processes involved, which is not possible with bulk analysis alone.
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Dec 2024
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I13-2-Diamond Manchester Imaging
I14-Hard X-ray Nanoprobe
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Kamila
Iskhakova
,
Hanna
Cwieka
,
Svenja
Meers
,
Heike
Helmholz
,
Anton
Davydok
,
Malte
Storm
,
Ivo Matteo
Baltruschat
,
Silvia
Galli
,
Daniel
Pröfrock
,
Olga
Will
,
Mirko
Gerle
,
Timo
Damm
,
Sandra
Sefa
,
Weilue
He
,
Keith
Macrenaris
,
Malte
Soujon
,
Felix
Beckmann
,
Julian
Moosmann
,
Thomas
O'Hallaran
,
Roger J.
Guillory
,
D. C. Florian
Wieland
,
Berit
Zeller-Plumhoff
,
Regine
Willumeit-Römer
Diamond Proposal Number(s):
[25078]
Open Access
Abstract: Magnesium (Mg) – based alloys are becoming attractive materials for medical applications as temporary bone implants for support of fracture healing, e.g. as a suture anchor. Due to their mechanical properties and biocompatibility, they may replace titanium or stainless-steel implants, commonly used in orthopedic field. Nevertheless, patient safety has to be assured by finding a long-term balance between metal degradation, osseointegration, bone ultrastructure adaptation and element distribution in organs. In order to determine the implant behavior and its influence on bone and tissues, we investigated two Mg alloys with gadolinium contents of 5 and 10 wt percent in comparison to permanent materials titanium and polyether ether ketone. The implants were present in rat tibia for 10, 20 and 32 weeks before sacrifice of the animal. Synchrotron radiation-based micro computed tomography enables the distinction of features like residual metal, degradation layer and bone structure. Additionally, X-ray diffraction and X-ray fluorescence yield information on parameters describing the bone ultrastructure and elemental composition at the bone-to-implant interface. Finally, with element specific mass spectrometry, the elements and their accumulation in the main organs and tissues are traced. The results show that Mg-xGd implants degrade in vivo under the formation of a stable degradation layer with bone remodeling similar to that of Ti after 10 weeks. No accumulation of Mg and Gd was observed in selected organs, except for the interfacial bone after 8 months of healing. Thus, we confirm that Mg-5Gd and Mg-10Gd are suitable material choices for bone implants.
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Nov 2024
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