B21-High Throughput SAXS
labSAXS-Offline SAXS and Sample Environment Development
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Abshar
Hasan
,
Andrey
Chuvilin
,
Alexander
Van Teijlingen
,
Helena
Rouco
,
Christopher
Parmenter
,
Federica
Venturi
,
Michael
Fay
,
Gabriele
Greco
,
Nicola M.
Pugno
,
Jan
Ruben
,
Charlotte J. C.
Edwards-Gayle
,
Benjamin
Myers
,
Ingrid
Dreveny
,
Nathan
Cowieson
,
Adam
Winter
,
Sara
Gamea
,
X. Frank
Walboomers
,
Tanvir
Hussain
,
José Carlos
Rodríguez-Cabello
,
Frankie
Rawson
,
Tell
Tuttle
,
Sherif
Elsharkawy
,
Avijit
Banerjee
,
Stefan
Habelitz
,
Alvaro
Mata
Diamond Proposal Number(s):
[32387]
Open Access
Abstract: Tooth enamel is characterised by an intricate hierarchical organization of apatite nanocrystals that bestows high stiffness, hardness, and fracture toughness. However, enamel does not possess the ability to regenerate, and achieving the artificial restoration of its microstructure and mechanical properties in clinical settings has proven challenging. To tackle this issue, we engineer a tuneable and resilient supramolecular matrix based on elastin-like recombinamers (ELRs) that imitates the structure and function of the enamel-developing matrix. When applied as a coating on the surface of teeth exhibiting different levels of erosion, the matrix is stable and can trigger epitaxial growth of apatite nanocrystals, recreating the microarchitecture of the different anatomical regions of enamel and restoring the mechanical properties. The study demonstrates the translational potential of our mineralising technology for treating loss of enamel in clinical settings such as the treatment of enamel erosion and dental hypersensitivity.
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Nov 2025
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B21-High Throughput SAXS
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Athanasia
Pylostomou
,
Jacek K.
Wychowaniec
,
Riccardo
Tognato
,
Sarah T.
Egger
,
Gion U.
Alig
,
Charlotte J. C.
Edwards-Gayle
,
Fatemeh
Safari
,
Jennifer R.
Weiser
,
Dagnija
Loca
,
Matteo
D'Este
,
Tiziano
Serra
,
Andrea J.
Vernengo
Diamond Proposal Number(s):
[29767]
Open Access
Abstract: Complex tissue engineering requires precise spatial cell organization, but static or isotropic hydrogels hinder long-term pattern maintenance due to random cell migration. We developed EXtrusion Patterned Embedded ConstruCT (EXPECT), a thermosensitive hydrogel embedding medium for 3D bioprinting, integrating Carbopol® 940 and gelatin for rheological properties and print fidelity, with poly(N-isopropylacrylamide)-graft-chondroitin sulfate (pNIPAAm-CS) for biocompatibility and temperature-responsive behavior (∼32°C lower critical solution temperature (LCST)). Rheological and small-angle X-ray scattering (SAXS) analyses confirmed EXPECT’s self-healing printability and reversible LCST-driven transitions from hydrophobic (above ∼32°C) to hydrophilic (below ∼32°C) states. Temperature actuation (15 min at 25°C every ∼5 days, otherwise 37°C) in 10 mm toroid channels embedded within EXPECT guided cellular organization of cells seeded in these channels. In chondrogenic medium, actuated single mesenchymal stromal cells (MSCs) showed ∼50% narrower patterns by day 7, sustained to day 36 (p < 0.001 vs. static, which widened to 137 ± 20%). Actuated MSC spheroids elongated, forming bipedal shapes and fusing into extended patterns (length 480 ± 158 μm, p < 0.0001) over 36 days. In 14-day human umbilical vein endothelial cells (HUVEC)-MSC co-cultures (10:1), actuation reduced pattern width by 27.5% (p = 0.0236), promoted early protrusions, and decreased cell circularity (vs. 2% increase in static, p = 0.0173), indicating enhanced elongation and potential vascularization. EXPECT’s dynamic, actuation-mediated control of anisotropic cell organization overcomes limitations of static hydrogels, offering significant potential for engineering complex, organized tissues in regenerative medicine.
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Sep 2025
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B21-High Throughput SAXS
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Diamond Proposal Number(s):
[28884, 32784]
Open Access
Abstract: Molecular solar thermal energy storage (MOST) materials are a promising method for renewable energy storage that captures solar energy and releases it on demand as heat. Azobenzene is attractive for MOST applications due to its photoreversible E–Z isomerization. Recently, phase-change materials have been formed using azobenzene to increase their energy-storage capacity; however, these condensed phases often lower the isomerization degree, which is only recovered on dissolution. In this work, sparing solvent addition is used to drive the self-assembly of azobenzene photosurfactants (AzoPS) into lyotropic liquid crystal (LLC) phases, which are explored for MOST applications for the first time. Using small-angle X-ray scattering (SAXS), polarized optical microscopy, and differential scanning calorimetry (DSC), we show that the structure-isomerization behavior, and energy-storage properties of these light-responsive LLCs can be systematically tuned by adjusting the photosurfactant structure, solvent, and concentration. Furthermore, by developing a method that combines SAXS with in situ DSC, we directly correlate the isomerization-induced LLC phase transitions to their energy-storage contributions. The formation of LLC phases through solvent addition both enhances the degree of isomerization (by up to 20%) and amplifies the structural disordering on isomerization, resulting in energy-storage densities of up to 123 J g–1. The ability to tune both the structure and isomerization properties in LLC materials suggests significant promise for MOST applications. In addition, the combination of advanced characterization methods used to establish the structure–isomerization–enthalpy (LLC-photoswitch-phase change) relationships provides unique insight into these multicomponent systems and accelerates the design pathways to future iterations for competitive solar energy storage devices.
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Aug 2025
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B21-High Throughput SAXS
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Jacek K.
Wychowaniec
,
Ezgi Irem
Bektas
,
Marcia
Muerner
,
Jiranuwat
Sapudom
,
Martin
Šrejber
,
Marielle
Airoldi
,
Roland
Schmidt
,
Andrea J.
Vernengo
,
Charlotte J. C.
Edwards-Gayle
,
Paul Sean
Tipay
,
Michal
Otyepka
,
Jeremy
Teo
,
David
Eglin
,
Matteo
D'Este
Diamond Proposal Number(s):
[29767]
Open Access
Abstract: Self-assembling peptides (SAPs) are fully defined nanobiomaterials offering unprecedented opportunities to control nanostructure and chemical attributes to investigate and manipulate cellular signals. To investigate the influence of chemical and morphological characteristics on inflammatory signaling in native immunity, we designed five β-sheet SAPs: EFEFKFEFK (EF8), YEFEFKFEFK (YEF8), EFEFKFEFKY (EF8Y), YEFEFKFEFKY (YEF8Y), and EYEFKFEFK (EYF8) (F: phenylalanine; E: glutamic acid; K: lysine, Y: tyrosine). The position of tyrosine in the peptide sequence dictated the self-assembly into nanostructures, with all SAPs self-assembling into thin constituent nanofibers with d ≈ 3.8 ± 0.4 nm, and sequences YEF8 and EF8 showing a propensity for associative bundling. These distinct SAPs induced contrasting inflammatory responses of monocytic model THP-1 cells-derived macrophages (MΦs). Presence of soluble EF8 nanofibers (at 2 mM) induced an anti-inflammatory response and polarization toward an M2 state, whereas YEF8 (at 2 mM) displayed a tendency for inducing a pro-inflammatory response and polarization toward an M1 state. EF8Y, YEF8Y, and EYF8 SAPs did not induce an inflammatory response in our models. These results were validated using peripheral blood mononuclear cells (PBMCs)-derived MΦs from human donors, confirming the critical role of EF8 and YEF8 SAPs as possible orchestrators of the repair of tissues or inducers of pro-inflammatory state, respectively. The same MΦs polarization responses from THP-1-derived MΦs cultured on 20 mM hydrogels were obtained. These findings will facilitate the utilization of this family of SAPs as immunomodulatory nanobiomaterials potentially changing the course of inflammation during the progression of various diseases.
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Apr 2025
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B21-High Throughput SAXS
I22-Small angle scattering & Diffraction
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Mohamed A. N.
Soliman
,
Abdulwahhab
Khedr
,
Tarsem
Sahota
,
Rachel
Armitage
,
Raymond
Allan
,
Katie
Laird
,
Natalie
Allcock
,
Fatmah I.
Ghuloum
,
Mahetab H.
Amer
,
Reem
Alazragi
,
Charlotte J. C.
Edwards-Gayle
,
Jacek K.
Wychowaniec
,
Attilio V.
Vargiu
,
Mohamed A.
Elsawy
Diamond Proposal Number(s):
[28287, 28806]
Open Access
Abstract: Guiding molecular assembly of peptides into rationally engineered nanostructures remains a major hurdle against the development of functional peptide-based nanomaterials. Various non-covalent interactions come into play to drive the formation and stabilization of these assemblies, of which electrostatic interactions are key. Here, the atomistic mechanisms by which electrostatic interactions contribute toward controlling self-assembly and lateral association of ultrashort β-sheet forming peptides are deciphered. Our results show that this is governed by charge distribution and ionic complementarity, both affecting the interaction patterns between charged residues: terminal, core, and/or terminal-to-core attraction/repulsion. Controlling electrostatic interactions enabled fine-tuning nanofiber morphology for the 16 examined peptides, resulting into versatile nanostructures ranging from extended thin fibrils and thick bundles to twisted helical “braids” and short pseudocrystalline nanosheets. This in turn affected the physical appearance and viscoelasticity of the formed materials, varying from turbid colloidal dispersions and viscous solutions to soft and stiff self-supportive hydrogels, as revealed from oscillatory rheology. Atomistic mechanisms of electrostatic interaction patterns were confirmed by molecular dynamic simulations, validating molecular and nanoscopic characterization of the developed materials. In essence, detailed mechanisms of electrostatic interactions emphasizing the impact of charge distribution and ionic complementarity on self-assembly, nanostructure formation, and hydrogelation are reported.
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Jan 2025
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B21-High Throughput SAXS
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Beatrice E.
Jones
,
Ann
Fitzpatrick
,
Kieran
Fowell
,
Charlotte J. C.
Edwards-Gayle
,
Nikul
Khunti
,
Katsuaki
Inoue
,
Steven
Daniels
,
Eugene
Williams
,
Camille
Blayo
,
Rachel C.
Evans
,
Nathan
Cowieson
Open Access
Abstract: Beamline B21 at the Diamond Light Source synchrotron in the UK is a small-angle X-ray scattering (SAXS) beamline that specializes in high-throughput measurements via automated sample delivery systems. A system has been developed whereby a sample can be illuminated by a focused beam of light coincident with the X-ray beam. The system is compatible with the highly automated sample delivery system at the beamline and allows a beamline user to select a light source from a broad range of wavelengths across the UV and visible spectrum and to control the timing and duration of the light pulse with respect to the X-ray exposure of the SAXS measurement. The intensity of the light source has been characterized across the wavelength range enabling experiments where a quantitative measure of dose is important. Finally, the utility of the system is demonstrated via measurement of several light-responsive samples.
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Jul 2024
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B21-High Throughput SAXS
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Diamond Proposal Number(s):
[26698]
Abstract: Hydrogels (HGs) with enhanced structural and mechanical properties can be generated by combining two or more different building blocks in the same matrix. It has been widely demonstrated that the addition of peptides, proteins, sugars, or polymers to the low molecular weight hydrogelator Fmoc-FF [(fluorenyl methyloxycarbonyl)-diphenylalanine] can significantly modify the chemical and structural features of the resulting HGs. In this context, the formulation of multicomponent HGs has been previously described, in which Fmoc-FF is mixed with telechelic diacrylate α-/ω-substituted polyethylene-glycol derivatives (PEGDAs) with a molecular weight of 575 (PEGDA1) or 250 Da (PEGDA2). Here, we investigate the possibility to generate Fmoc-FF-based interpenetrated networks performing the cross-link reaction of PEGDA monomers in supramolecular peptide hydrogels. This approach can allow the modulation of the final properties of the material, in terms of water behavior, topography, and rigidity. The results indicate that the polymerization time, the polymer length, and the Fmoc-FF/PEGDA ratio play a crucial role in the chemistry of the materials and, consequently, of their potential application.
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Jun 2024
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B21-High Throughput SAXS
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Diamond Proposal Number(s):
[28287]
Abstract: A library of composite polymer networks (CPNs) were formed by combining Pluronic F127, as the primary gelator, with a range of di-acrylate functionalised PEG polymers, which tune the rheological properties and provide UV crosslinkability. A coarse-grained sol–gel room temperature phase diagram was constructed for the CPN library, which identifies PEG-dependent disruption of micelles as leading to liquefication. Small angle X-ray scattering and rheological measurements provide detailed insight into; (i) micelle-micelle ordering; (ii) micelle-micelle disruption, and; (iii) acrylate-micelle disruption; with contributions that depend on composition, including weak PEG chain length and end group effects. The influence of composition on 3D extrusion printability through modulation of the cohesive/hydrophobic interactions was assessed. It was found that only micelle content provides consistent changes in printing fidelity, controlled largely by printing conditions (pressure and feed rate). Finally, the hydrogels were shown to be UV photo-crosslinkable, which further improves fidelity and structural integrity, and usefully reduces the mesh size. Our results provide a guide for design of 3D-printable CPN inks for future biomedical applications.
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Jan 2024
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B21-High Throughput SAXS
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Diamond Proposal Number(s):
[29985]
Open Access
Abstract: harge repulsion can be used to control and fine tune the supramolecular aggregation of amino acid substituted diketopyrrolopyrroles in water. This is a simple method to access a number of different aggregation states with distinct photophysical properties without the need for extensive synthetic tuning, process engineering, or solvent optimisation. Most importantly, these different aggregates show different optical gaps, HOMO-LUMO gaps, electroactivity, and exciton binding energies. These systems expand the absorbance range achieved from one chromophore unit and also create systems with large Stokes shifts. This work therefore answers the demand for tailoring aggregate structures by manipulating charge repulsion in an aqueous environment.
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Jan 2024
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B21-High Throughput SAXS
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Diamond Proposal Number(s):
[29767]
Open Access
Abstract: Sterilisation of implantable biomaterials such as hydrogels remains a key step towards their clinical translation. Standard sterilisation methods can significantly alter hydrogels' physicochemical and biological performance. Previously, we developed composite hydrogels based on ε-polylysine (ε-PL) and hyaluronic acid (HA). The developed hydrogels demonstrated promising antibacterial activity and in vitro cell viability and their variable properties depending on the chosen ε-PL to HA ratio. In this study, we fabricated a series of chemically cross-linked ԑ-PL/HA hydrogels with expanded ԑ-PL to HA mass ratios.
Using small-angle X-ray scattering (SAXS), we unravelled the topological differences between physically and chemically crosslinked hydrogels. We then selected the chemically crosslinked hydrogel ԑ-PL/HA series of 60:40 wt%, 70:30 wt%, and 80:20 wt% ratios, with similar network topologies, to evaluate the impact of steam sterilisation on their physicochemical and viscoelastic properties. The antibacterial activity of the sterilized hydrogels was also evaluated against Gram-negative and Gram-positive bacteria. Our results showed that steam sterilisation minimally affects structure and physicochemical properties of ԑ-PL/HA hydrogels. Furthermore, the developed hydrogel ԑ-PL/HA series of 60:40 wt%, 70:30 wt%, and 80:20 wt% ratios showed pronounced antibacterial activity against Gram-negative and Gram-positive pathogenic bacteria. We expect our results will contribute to the growing understanding of using sterilisation methods for antibacterial hydrogels that have the potential for wider tissue engineering applications.
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Dec 2023
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