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Instruments / Technical Area	Publication Details	Published
B21-High Throughput SAXS	Cross-link of telechelic diacrylate polyethylene-glycol in peptide-based Fmoc-FF hydrogel matrices Elisabetta Rosa , Paolo Pellegrino , Mariafrancesca Cascione , Rosaria Rinaldi , Eliana Gianolio , Charlotte J. C. Edwards-Gayle , Ian W. Hamley , Giancarlo Morelli , Antonella Accardo , Carlo Diaferia Acs Applied Polymer Materials DOI: 10.1021/acsapm.4c01059 Diamond Proposal Number(s): [26698] Show Abstract ▼ 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.	Jun 2024
B23-Circular Dichroism I22-Small angle scattering & Diffraction	Three-dimensional printable enzymatically active plastics William H. Zhang , Graham J. Day , Ioannis Zampetakis , Michele Carrabba , Zhongyang Zhang , Ben M. Carter , Norman Govan , Colin Jackson , Menglin Chen , Adam W. Perriman Acs Applied Polymer Materials DOI: 10.1021/acsapm.1c00845 Diamond Proposal Number(s): [17972, 18006] Open Access Show Abstract ▼ Abstract: Here, we describe a facile route to the synthesis of enzymatically active highly fabricable plastics, where the enzyme is an intrinsic component of the material. This is facilitated by the formation of an electrostatically stabilized enzyme–polymer surfactant nanoconstruct, which, after lyophilization and melting, affords stable macromolecular dispersions in a wide range of organic solvents. A selection of plastics can then be co-dissolved in the dispersions, which provides a route to bespoke 3D enzyme plastic nanocomposite structures using a wide range of fabrication techniques, including melt electrowriting, casting, and piston-driven 3D printing. The resulting constructs comprising active phosphotriesterase (arPTE) readily detoxify organophosphates with persistent activity over repeated cycles and for long time periods. Moreover, we show that the protein guest molecules, such as arPTE or sfGFP, increase the compressive Young’s modulus of the plastics and that the identity of the biomolecule influences the nanomorphology and mechanical properties of the resulting materials. Overall, we demonstrate that these biologically active nanocomposite plastics are compatible with state-of-the-art 3D fabrication techniques and that the methodology could be readily applied to produce robust and on-demand smart nanomaterial structures.	Nov 2021
I22-Small angle scattering & Diffraction	Core-shell spheroidal hydrogels produced via charge-driven interfacial complexation Vincenzo Calabrese , Davide Califano , Marcelo A. Da Silva , Julien Schmitt , Saffron J. Bryant , Kazi M. Zakir Hossain , Ana Maria Percebom , Aurora Perez-Gramatges , Janet Lesley Scott , Karen J. Edler Acs Applied Polymer Materials DOI: 10.1021/acsapm.9b01086 Diamond Proposal Number(s): [20409] Open Access Show Abstract ▼ Abstract: Through charge-driven interfacial complexation, we produced millimetre-sized spheroidal hydrogels (SH) with a core-shell structure allowing long term stability in aqueous media. The SH were fabricated by extruding, drop-wise, a cationic cellulose nanofibril (CCNF) dispersion into an oppositely charged polyacrylic acid (PAA) bath. The SH have a solid-like CCNF-PAA shell, acting as a semi-permeable membrane, and a liquid-like CCNF suspension in the core. Swelling behaviour of the SH was dependent on the osmotic pressure of the ageing media. Swelling could be supressed by increasing the ionic strength of the media as this enhanced interfibrillar interactions and thus strengthened the outer gel membrane. We further validated a potential application of SH as re-usable matrixes for glucose oxidase (GOx) entrapment, where the SH work as “microreactors” from which substrate and product are freely able to migrate, through the SH shell whilst avoiding enzyme leakage.	Feb 2020

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