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133 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2, 3, 4, 5, 6, 7, 8 [Next/Last]

Instruments / Technical Area	Publication Details	Published
I19-Small Molecule Single Crystal Diffraction	Core-twisted, cationic perylene diimides; homochiral dimerization and chiroptical anion sensing Denis Hartmann , Jamie S. Hillis , Lucy E. Walker , Timothy A. Barendt Chemistry – A European Journal DOI: 10.1002/chem.202501270 Diamond Proposal Number(s): [36069] Open Access Show Abstract ▼ Abstract: Core-twisted perylene diimides (PDIs) are chiral organic dyes that may be exploited for self-assembled chiroptical materials or for the enantioselective recognition and sensing of chiral substrates. Discrete self-assembled dimers and host–guest complexes of core-twisted perylene diimides are important for furthering our understanding of this supramolecular chemistry, yet they are rare because the twisted perylene core significantly weakens intermolecular π–π interactions with the PDI's π-surface. To address this challenge, we have installed hydrogen bond donor groups in the PDI's bay positions, which direct the formation of a robust, co-facial and homochiral intermolecular PDI dimer. The structure of this discrete dimer is distinct from previous aggregates of non-planar PDIs that utilize the imide position for hydrogen bonding. We also uncover the potential of core-twisted, dicationic PDIs for the enantioselective recognition and chiroptical sensing of chiral anions and investigate the basis of this response via chiral complementarity in the discrete host–guest complex.	May 2025
B23-Circular Dichroism	Enhanced protein photo-stability analysis using SRCD in the presence of phospholipid SUVs Claudia Honisch , Martina Rotondo , Mario Monaco , Stefano Tartaggia , Rohanah Hussain , Giuliano Siligardi , Paolo Ruzza Chemistry – A European Journal DOI: 10.1002/chem.202500792 Show Abstract ▼ Abstract: The interaction between lipids and proteins impacts on a multitude of cellular processes and may contribute to the onset of several pathologies and ageing. Such processes are frequently linked to oxidative stress, whereby polyunsaturated fatty acids act as substrates for in vivo lipoxidation. The subsequent lipid peroxidation and/or isomerisation is known to affect membrane organization, as well as to modify proteins and DNA, leading to functional alterations. Aim of this study was to evaluate the capacity of UV denaturation experiments to induce lipid modification and to investigate the influence of lipid presence on the conformational stability of selected soluble model proteins. To this end, the UV-denaturation experiment developed at the B23 beamline of the Diamond Light Source (UK) is employed, which high photon flux and brilliance of the incident beamlight induce protein denaturation when repeated consecutive synchrotron radiation circular dichroism spectra are acquired in the far-UV region, diagnostic of protein folding. This allows the estimation of protein photostability. Our findings show that the presence of lipid vesicles (SUVs) significantly impacts the UV-denaturation of proteins, preserving the native structure in proteins with a high helical content. This suggests that lipids may play a protective role against light-induced damage to proteins.	May 2025
I19-Small Molecule Single Crystal Diffraction	Higher assemblies of coordination cage-catenanes linked by copper(II) chloride clusters: networks and transformations Matthew P. Snelgrove , Natalia N. Sergeeva , Michaele J. Hardie Chemistry – A European Journal DOI: 10.1002/chem.202403692 Diamond Proposal Number(s): [26879] Show Abstract ▼ Abstract: Cage-catenanes are chemical constructs where two or more cage-like molecules or assemblies are mechanically interlocked together. We report a new class of cage-catenanes where dimeric metal-organic cage-catenanes are linked into larger assemblies through additional bridging metal chloride links. These crystalline materials are obtained from the reaction of tris(nicotinoyl)cyclotriguaiacylene (L1) with Cu(II) salts, and all feature a tetramer of cages where two {Cu3(L1)2(X)6} cages (X = anion) are mechanically interlocked, and link to each other and to another {Cu3(L1)2(X)6}2 cage-catenane through a planar, linear tetranuclear {Cu4(μ−Cl)6Cl2} cluster. The complex of discrete tetrameric {Cu3(L1)2(X)6}4 assemblies (dimers of cage-catenanes) transforms through solvent-exchange processes to 1D coordination chain structures through additional {Cu2(μ−Cl)2} bridges between the tetrameric {Cu3(L1)2(X)6}4 assemblies. Complex [Cu6(L1)4Cl12(H2O)3]·(H2O)·15(DMF) C2 features a 2D coordination network of 63 topology linked through three different Cu(II) clusters, namely {Cu4(μ−Cl)6}, {Cu2(μ−Cl)2} and a rare linear {Cu2(μ-Cl)} linkage. Break-down of C2 in water likely proceeds through hydrolysis of this unusual linear Cu-Cl-Cl bond.	Dec 2024
I19-Small Molecule Single Crystal Diffraction	A combined experimental and computational exploration of heteroleptic cis-Pd2L2L'2 coordination cages through geometric complementarity Andrew Tarzia , Wentao Shan , Victor Posligua , Cameron Cox , Louise Male , Benjamin Egleston , Rebecca Greenaway , Kim Jelfs , James E. M. Lewis Chemistry – A European Journal DOI: 10.1002/chem.202403336 Diamond Proposal Number(s): [28766] Open Access Show Abstract ▼ Abstract: Heteroleptic (mixed-ligand) coordination cages are of interest as host systems with more structurally and functionally complex cavities than homoleptic architectures. The design of heteroleptic cages, however, is far from trivial. In this work, we experimentally probed the self-assembly of Pd(II) ions with binary ligand combinations in a combinatorial fashion to search for new cis-Pd2L2L’2 heteroleptic cages. A hierarchy of computational analyses was then applied to these systems with the aim of elucidating key factors for rationalising self-assembly outcomes. Simple and inexpensive geometric analyses were shown to be effective in identifying complementary ligand pairs. Preliminary results demonstrated the viability of relatively rapid semi-empirical calculations for predicting the topology of thermodynamically favoured assemblies with rigid ligands, whilst more flexible systems proved challenging. Stemming from this, key challenges were identified for future work developing effective computational forecasting tools for self-assembled metallo-supramolecular systems.	Oct 2024
I19-Small Molecule Single Crystal Diffraction	Controlling the helical pitch of foldamers through terminal functionality: a solid state study Alexander Davis , Sena Ozturk , Colin Seaton , Louise Male , Sarah J. Pike Chemistry – A European Journal DOI: 10.1002/chem.202402892 Diamond Proposal Number(s): [28766, 36069] Open Access Show Abstract ▼ Abstract: Developing new methods to control the size and shape of the helical structures adopted by foldamers is highly important as the secondary structure displayed by these supramolecular scaffolds often dictates their activity and function. Herein, we report on a systematic study demonstrating that the helical pitch of ortho-azobenzene/2,6-pyridyldicarboamide foldamers can be readily controlled through the nature of the terminal functionality. Remarkably, simply through varying the end group of the foldamer, and without modifying any other structural features of the scaffold, the helical pitch can be over doubled in magnitude (from 3.4 Å to 7.3 Å). Additionally, crystallographic analysis of a library ten foldamers has identified general trends in the influence of a range of terminal functionalities, including carboxylbenzyl (Cbz), diphenylcarbamyl (N(Ph)2), ferrocene (Fc) and tert-butyloxycarbonyl (Boc), in controlling the folding behaviour of these supramolecular scaffolds. These studies could prove useful in the future development of functional foldamers which adopt specific sizes and shapes.	Sep 2024
	On the electrochemical growth of a crystalline p-n junction from aqueous solutions Roberto Felici , Tommaso Baroni , Francesco Carla , Nicola Cioffi , Francesco Di Benedetto , Claudio Fontanesi , Andrea Giaccherini , Walter Giurlani , Mathieu Gonidec , Alessandro Lavacchi , Enrico Berretti , Patrick Marcantelli , Giordano Montegrossi , Marco Bonechi , Rosaria Anna Picca , Lorenzo Poggini , Francesca Russo , Maria Chiara Sportelli , Luisa Torsi , Massimo Innocenti Chemistry – A European Journal DOI: 10.1002/chem.202401403 Show Abstract ▼ Abstract: Our society largely relies on inorganic semiconductor devices which are, so far, fabricated using expensive and complex processes requiring ultra-high vacuum equipment. Here we report on the possibility of growing a p-n junction taking advantage of electrochemical processes based on the use of aqueous solutions. The growth of the junction has been carried out using the Electrochemical Atomic Layer Deposition (E-ALD) technique, which allowed to sequentially deposit two different semiconductors, CdS and Cu2S, on an Ag(111) substrate, in a single procedure. The growth process was monitored in situ by Surface X-Ray Diffraction (SXRD) and resulted in the fabrication of a thin double-layer structure with a high degree of crystallographic order and a well-defined interface. The high-performance electrical characteristics of the device were analysed ex-situ and show the characteristic feature of a diode.	May 2024
I03-Macromolecular Crystallography I04-Macromolecular Crystallography	Conformational and electronic variations in 1,2- and 1,6-cyclophellitols and their impact on retaining α-glucosidase inhibition Tim P. Ofman , Jurriaan J. A. Heming , Alba Nin-Hill , Florian Küllmer , Elisha Moran , Megan Bennett , Roy Steneker , Anne-Mei Klein , Gijs Ruijgrok , Ken Kok , Zach W. B. Armstrong , Johannes M. F. G. Aerts , Gijsbert A. Van Der Marel , Carme Rovira , Gideon J. Davies , Marta Artola , Jeroen D. C. Codée , Hermen S. Overkleeft Chemistry – A European Journal DOI: 10.1002/chem.202400723 Diamond Proposal Number(s): [32736, 24948] Open Access Show Abstract ▼ Abstract: Glycoside hydrolases (glycosidases) take part in myriad biological processes and are important therapeutic targets. Competitive and mechanism-based inhibitors are useful tools to dissect their biological role and comprise a good starting point for drug discovery. The natural product, cyclophellitol, a mechanism-based, covalent and irreversible retaining β-glucosidase inhibitor has inspired the design of diverse α- and β-glycosidase inhibitor and activity-based probe scaffolds. Here, we sought to deepen our understanding of the structural and functional requirements of cyclophellitol-type compounds for effective human α-glucosidase inhibition. We synthesized a comprehensive set of α-configured 1,2- and 1,6-cyclophellitol analogues bearing a variety of electrophilic traps. The inhibitory potency of these compounds was assessed towards both lysosomal and ER retaining α-glucosidases. These studies revealed the 1,6-cyclophellitols to be the most potent retaining α-glucosidase inhibitors, with the nature of the electrophile determining inhibitory mode of action (covalent or non-covalent). DFT calculations support the ability of the 1,6-cyclophellitols, but not the 1,2-congeners, to adopt conformations that mimic either the Michaelis complex or transition state of α-glucosidases.	Apr 2024
I19-Small Molecule Single Crystal Diffraction	A study on auto-catalysis and product inhibition: a nucleophilic aromatic substitution reaction catalysed within the cavity of an octanuclear coordination cage Jack C. Dorrat , Christopher G. P. Taylor , Rosemary J. Young , Atena B. Solea , David Turner , Genevieve H. Dennison , Michael D. Ward , Kellie Tuck Chemistry – A European Journal DOI: 10.1002/chem.202400501 Diamond Proposal Number(s): [25064] Open Access Show Abstract ▼ Abstract: The ability of an octanuclear cubic coordination cage to catalyse a nucleophilic aromatic substitution reaction on a cavity-bound guest was studied with 2,4-dinitrofluorobenzene (DNFB) as the guest/substrate. It was found that DNFB undergoes a catalysed reaction with hydroxide ions within the cavity of the cubic cage (in aqueous buffer solution, pH 8.6). The rate enhancement of kcat/kuncat was determined to be 23, with cavity binding of the guest being required for catalysis to occur. The product, 2,4-dinitrophenolate (DNP), remained bound within the cavity due to electrostatic stabilisation and exerts two apparently contradictory effects: it initially auto-catalyses the reaction when present at low concentrations, but at higher concentrations inhibits catalysis when a pair of DNP guests block the cavity. When encapsulated, the UV/Vis absorption spectrum of DNP is red-shifted when compared to the spectrum of free DNP in aqueous solution. Further investigations using other aromatic guests determined that a similar red-shift on cavity binding also occurred for 4-nitrophenolate (4NP) at pH 8.6. The red-shift was used to determine the stoichiometry of guest binding of DNP and 4NP within the cage cavity, which was confirmed by structural analysis with X-ray crystallography; and also used to perform catalytic kinetic studies in the solution-state.	Mar 2024
I19-Small Molecule Single Crystal Diffraction	Structure-property relationships for potential inversion from electron acceptors based on thiophene-fused triptycene quinones, 1,4-diketones and their malononitrile adducts Stefan Warrington , Stephanie Montanaro , Mark R. J. Elsegood , Gary S. Nichol , Iain A. Wright Chemistry – A European Journal 30, e202400782 DOI: 10.1002/chem.202400782 Diamond Proposal Number(s): [30280] Open Access Show Abstract ▼ Abstract: The synthesis and properties of a series of 11,11,12,12-tetracyano-9,10-anthraquinodimethane (TCAQ) inspired electron acceptors based on thiophene-fused quinone and triptycene motifs is presented. This has yielded insights into structure-property relationships for establishing and modulating simultaneous two electron reduction processes in TCAQ analogues. These new compounds were synthesised using a Friedel-Crafts acylation between triptycene and thiophene-3,4-dicarbonyl chloride. Isomeric para-quinones featuring a [c]-fused thiophene on one side and a β,β- or α,β-fused triptycene on the other were isolated alongside a thiophene-3,4-diketone which bears two triptycene fragments. Knoevenagel condensation of these products with malononitrile produced a quinoidal bis(dicyanomethylene), an oxo-dicyanomethylene and an acyclic bis(dicyanomethylene). This series of new electron accepting molecules has been studied using X-ray crystallography and the implications of their 3D structures on NMR and UV/vis absorbance spectroscopy and cyclic voltammetry results have been ascertained with conclusions underpinned by computational methods.	Mar 2024
B18-Core EXAFS	Synthesis, characterization, and catalytic application of colloidal and supported Mn nanoparticles Johannes Zenner , Kelly Tran , Liqun Kang , Niklas Kinzel , Christophe Werlé , Serena Debeer , Alexis Bordet , Walter Leitner Chemistry – A European Journal DOI: 10.1002/chem.202304228 Diamond Proposal Number(s): [31573] Open Access Show Abstract ▼ Abstract: Colloidal and supported manganese nanoparticles were synthesized following an organometallic approach and applied in the catalytic transfer hydrogenation (CTH) of aldehydes and ketones. Reaction parameters for the preparation of colloidal nanoparticles (NPs) were optimized to yield small (2-2.5 nm) and well-dispersed NPs. Manganese NPs were further immobilized on an imidazolium-based supported ionic phase (SILP) and characterized to evaluate NP size, metal loading, and oxidation states. Oxidation of the Mn NPs by the support was observed resulting in an average formal oxidation state of +2.5. The MnOx@SILP material showed promising performance in the CTH of aldehydes and ketones using 2-propanol as a hydrogen donor, outperforming previously reported Mn NPs-based CTH catalysts in terms of metal loading-normalized turnover numbers. Interestingly, MnOx@SILP were found to lose activity upon air exposure, which correlates with an additional increase in the average oxidation state of Mn as revealed by X-ray absorption spectroscopic studies.	Feb 2024

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