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9,418 items found (0 items not approved), displaying 21 to 30.[First/Prev] 1, 2, 3, 4, 5, 6, 7, 8 [Next/Last]

Beamlines/Technical Area	Publication Details	Published
I09-Surface and Interface Structural Analysis	Chemically-resolved determination of hydrogenated graphene-substrate interaction Anders L. Jørgensen , David A. Duncan , Claus F. P. Kastorp , Line Kyhl , Zeyuan Tang , Albert Bruix , Mie Andersen , Bjork Hammer , Tien-lin Lee , Liv Hornekaer , Richard Balog Physical Chemistry Chemical Physics DOI: 10.1039/C9CP02059D Diamond Proposal Number(s): [16243] Show Abstract ▼ Abstract: Functionalization of graphene on Ir(111) is a promising route to modify graphene by chemical means in a controlled fashion at the nanoscale. Yet, the nature of such functionalized sp3 nanodots remains unknown. Density functional theory (DFT) calculations alone cannot differentiate between two plausible structures, namely true graphane and substrate stabilized graphane-like nanodots. These two structures, however, interact dramatically differently with the underlying substrate. Discriminating which type of nanodots forms on the surface is thus of paramount importance for the applications of such prepared nanostructures. By comparing X-ray standing wave measurements against theoretical model structures obtained by DFT calculations we are able to exclude the formation of true graphane nanodots and clearly show the formation graphane-like nanodots.	Jun 2019
I19-Small Molecule Single Crystal Diffraction	Self-assembly of catalytically-active supramolecular coordination compounds within metal-organic frameworks Rosa Adam , Marta Mon , Lucas H. G. Kalinke , Alejandro Vidal-moya , Antonio Fernandez , Richard E. P. Winpenny , Antonio Domenech-carbo , Antonio Leyva-perez , Donatella Armentano , Emilio Pardo , Jesus Ferrando-soria Journal Of The American Chemical Society DOI: 10.1021/jacs.9b03914 Diamond Proposal Number(s): [18768] Show Abstract ▼ Abstract: Supramolecular Coordination Compounds (SCCs) represent the power of Coordination Chemistry methodologies to self-assemble discrete architectures with targeted properties. SCCs are generally synthesised in solution, with isolat-ed fully-coordinated metal atoms as structural nodes, thus severely limited as metal-based catalysts. Metal-Organic Frameworks (MOFs) show unique features to act as chemical nanoreactors for the in-situ synthesis and stabilization of otherwise not accessible functional species. Here, we present the self-assembly of PdII SCCs within the confined space of a preformed MOF (SCCs@MOF) and its post-assembly metalation to give a PdII-AuIII supramolecular assembly, crys-tallography underpinned. These SCCs@MOF catalyse the coupling of boronic acids and/or alkynes, representative multisite metallic-catalysed reactions in which traditional SCCs tend to decompose, and retain its structural integrity as consequence of the synergetic hybridization between SCCs and MOF. These results open new avenues in both the synthesis of novel SCCs and their use on heterogeneous metal-based Supramolecular Catalysis.	Jun 2019
I05-ARPES	Emerging 2D-ferromagnetism and strong spin-orbit coupling at the surface of valence-fluctuating EuIr2Si2 Susanne Schulz , Ilya A. Nechaev , Monika Güttler , Georg Poelchen , Alexander Generalov , Steffen Danzenbächer , Alla Chikina , Silvia Seiro , Kristin Kliemt , Alexandra Yu. Vyazovskaya , Timur K. Kim , Pavel Dudin , Evgueni V. Chulkov , Clemens Laubschat , Eugene E. Krasovskii , Christoph Geibel , Cornelius Krellner , Kurt Kummer , Denis V. Vyalikh Npj Quantum Materials 4 DOI: 10.1038/s41535-019-0166-z Diamond Proposal Number(s): [18844, 17761] Open Access Show Abstract ▼ Abstract: The development of materials that are non-magnetic in the bulk but exhibit two-dimensional (2D) magnetism at the surface is at the core of spintronics applications. Here, we present the valence-fluctuating material EuIr2Si2, where in contrast to its non-magnetic bulk, the Si-terminated surface reveals controllable 2D ferromagnetism. Close to the surface the Eu ions prefer a magnetic divalent configuration and their large 4f moments order below 48 K. The emerging exchange interaction modifies the spin polarization of the 2D surface electrons originally induced by the strong Rashba effect. The temperature-dependent mixed valence of the bulk allows to tune the energy and momentum size of the projected band gaps to which the 2D electrons are confined. This gives an additional degree of freedom to handle spin-polarized electrons at the surface. Our findings disclose valence-fluctuating rare-earth based materials as a very promising basis for the development of systems with controllable 2D magnetic properties which is of interest both for fundamental science and applications.	Jun 2019
I11-High Resolution Powder Diffraction	Selective production of diethyl maleate via oxidative cleavage of lignin aromatic unit Zhenping Cai , Jinxing Long , Yingwen Li , Lin Ye , Biaolin Yin , Liam John France , Juncai Dong , Lirong Zheng , Hongyan He , Sijie Liu , Shik Chi Edman Tsang , Xuehui Li Chem DOI: 10.1016/j.chempr.2019.05.021 Show Abstract ▼ Abstract: Green production of bulk chemicals traditionally obtained from fossil resources is of great importance. One potential route toward realizing this goal is through the utilization of renewable lignin; however, current techniques generally lead to low product specificity because of the structural diversity of this recalcitrant biopolymer. Herein, we devised a new catalytic system to promote selectively oxidative lignin in air, and diethyl maleate was formed at impressively high yield of 404.8 mg g−1 and selectivity of 72.7% over the polyoxometalate ionic liquid of [BSmim]CuPW12O40. This high catalytic activity is ascribed to a five-coordinated Cu+ species, which, through the formation of end-on dioxygen species in vacant orbitals, facilitates the selective oxidation of basic lignin aromatic units (phenylpropane C9 units). Therefore, these results represent significant progress toward the realization of an industrially applicable and highly selective lignin oxidation process for the generation of value-added and bulk chemicals.	Jun 2019
I04-Macromolecular Crystallography I24-Microfocus Macromolecular Crystallography	Crystal structures of the recombinant β-factor XIIa protease with bound Thr-Arg and Pro-Arg substrate mimetics Monika Pathak , Rosa Manna , Chan Li , Bubacarr G. Kaira , Badraldin Kareem Hamad , Benny Danilo Belviso , Camila R. Bonturi , Ingrid Dreveny , Peter M. Fischer , Lodewijk V. Dekker , Maria Luiza Vilela Oliva , Jonas Emsley Acta Crystallographica Section D Structural Biology 75 DOI: 10.1107/S2059798319006910 Diamond Proposal Number(s): [19880] Open Access Show Abstract ▼ Abstract: Coagulation factor XII (FXII) is a key initiator of the contact pathway, which contributes to inflammatory pathways. FXII circulates as a zymogen, which when auto-activated forms factor XIIa (FXIIa). Here, the production of the recombinant FXIIa protease domain (βFXIIaHis) with yields of ∼1–2 mg per litre of insect-cell culture is reported. A second construct utilized an N-terminal maltose-binding protein (MBP) fusion (MBP-βFXIIaHis). Crystal structures were determined of MBP-βFXIIaHis in complex with the inhibitor D-Phe-Pro-Arg chloromethyl ketone (PPACK) and of βFXIIaHis in isolation. The βFXIIaHis structure revealed that the S2 and S1 pockets were occupied by Thr and Arg residues, respectively, from an adjacent molecule in the crystal. The Thr-Arg sequence mimics the P2–P1 FXIIa cleavage-site residues present in the natural substrates prekallikrein and FXII, and Pro-Arg (from PPACK) mimics the factor XI cleavage site. A comparison of the βFXIIaHis structure with the available crystal structure of the zymogen-like FXII protease revealed large conformational changes centred around the S1 pocket and an alternate conformation for the 99-loop, Tyr99 and the S2 pocket. Further comparison with activated protease structures of factors IXa and Xa, which also have the Tyr99 residue, reveals that a more open form of the S2 pocket only occurs in the presence of a substrate mimetic. The FXIIa inhibitors EcTI and infestin-4 have Pro-Arg and Phe-Arg P2–P1 sequences, respectively, and the interactions that these inhibitors make with βFXIIa are also described. These structural studies of βFXIIa provide insight into substrate and inhibitor recognition and establish a scaffold for the structure-guided drug design of novel antithrombotic and anti-inflammatory agents.	Jun 2019
B18-Core EXAFS	Proton chelating ligands drive improved chemical separations for rhodium Hirokazu Narita , Rebecca M. Nicolson , Ryuhei Motokawa , Fumiyuki Ito , Kazuko Morisaku , Midori Goto , Mikiya Tanaka , William T. Heller , Hideaki Shiwaku , Tsuyoshi Yaita , Ross J. Gordon , Jason B. Love , Peter A. Tasker , Emma R. Schoﬁeld , Mark R. Antonio , Carole A. Morrison Inorganic Chemistry DOI: 10.1021/acs.inorgchem.9b01136 Diamond Proposal Number(s): [15757] Show Abstract ▼ Abstract: Current methods for the extraction of rhodium carry the highest carbon footprint and worst pollution metrics of all of the elements used in modern technological applications. Improving upon existing methods is made difficult by the limited understanding of the molecular-level chemistry occurring in extraction processes, particularly in the hydrometallurgical separation step. While many of the precious metals can be separated by solvent extraction, there currently exist no commercial extractants for Rh. This is due to its complicated mixed speciation upon leaching into hydrochloric acid, which gives rise to difficulties in designing effective reagents for solvent extraction. Herein we show that the diamidoamine reagent N-n-hexylbis(N-methyl-N-n-octylethylamide)amine transports Rh(III) from aqueous HCl into an organic phase as the monoaquated dianion [RhCl5(H2O)]2– through the formation of an outer-sphere assembly; this assembly has been characterized by experimentation (slope analysis, FT-IR and NMR spectroscopy, EXAFS, SANS, and ESI-MS) and computational modeling. The paper demonstrates the importance of applying a broad range of techniques to obtain a convincing mode of action for the complex processes involved in anion recognition in the solution phase. A consistent and comprehensive understanding of how the ligand operates to achieve Rh(III) selectivity over the competitor anion Cl– has emerged. This knowledge will guide the design of extractants and thus offers promise for improving the sustainability of metal extraction from both traditional mining sources and the recycling of secondary source materials.	Jun 2019
B18-Core EXAFS	Evidence for tetranuclear bis-µ-oxo cubane species in molecular iridium-based water oxidation catalysts from XAS analysis Stuart A. Bartlett , Emma V. Sackville , Emma K. Gibson , Veronica Celorrio , Peter P. Wells , Maarten Nachtegaal , Stafford W. Sheehan , Ulrich Hintermair Chemical Communications DOI: 10.1039/C9CC02088H Diamond Proposal Number(s): [10306, 15151] Open Access Show Abstract ▼ Abstract: The structure of a highly active pyridine-alkoxide iridium water oxidation catalyst (WOC) is examined by X-ray absorption spectroscopy (XAS). A detailed comparison with IrO2 points to a rigid molecular unit of low nuclearity, with the best analysis suggesting the existence of a novel tetrameric iridium-oxo cubane as the resting state.	Jun 2019
B22-Multimode InfraRed imaging And Microspectroscopy	Elementary steps in the formation of hydrocarbons from surface methoxy groups in HZSM-5 seen by synchrotron infrared microspectroscopy Ivalina B. Minova , Santhosh K. Matam , Alex Greenaway , Richard A. Catlow , Mark D. Frogley , Gianfelice Cinque , Paul A. Wright , Russell F. Howe Acs Catalysis DOI: 10.1021/acscatal.9b01820 Diamond Proposal Number(s): [13725, 16257, 20906] Show Abstract ▼ Abstract: Synchrotron infrared microspectroscopy has identified with high temporal resolution (down to 0.25 s) the initial events occurring when methanol vapour is contacted with a crystal of zeolite HZSM-5. The first alkenes are generated directly from methoxy groups formed at the acid sites via their deprotonation. These alkenes can either desorb directly or oligomerise and cyclise to form dimethylcyclopentenyl cations. The oligomeric and dimethylcyclopentenyl cations are the first major components of the hydrocar-bon pool that precede aromatic hydrocarbons and lead to indirect alkene formation. This is the first direct observation of these events in real time.	Jun 2019
Krios I-Titan Krios I at Diamond	A novel druggable interprotomer pocket in the capsid of rhino- and enteroviruses Rana Abdelnabi , James A. Geraets , Yipeng Ma , Carmen Mirabelli , Justin W. Flatt , Ausra Domanska , Leen Delang , Dirk Jochmans , Timiri Ajay Kumar , Venkatesan Jayaprakash , Barij Nayan Sinha , Pieter Leyssen , Sarah Butcher , Johan Neyts Plos Biology DOI: 10.1371/journal.pbio.3000281 Diamond Proposal Number(s): [1973] Open Access Show Abstract ▼ Abstract: Rhino- and enteroviruses are important human pathogens, against which no antivirals are available. The best-studied inhibitors are “capsid binders” that fit in a hydrophobic pocket of the viral capsid. Employing a new class of entero-/rhinovirus inhibitors and by means of cryo–electron microscopy (EM), followed by resistance selection and reverse genetics, we discovered a hitherto unknown druggable pocket that is formed by viral proteins VP1 and VP3 and that is conserved across entero-/rhinovirus species. We propose that these inhibitors stabilize a key region of the virion, thereby preventing the conformational expansion needed for viral RNA release. A medicinal chemistry effort resulted in the identification of analogues targeting this pocket with broad-spectrum activity against Coxsackieviruses B (CVBs) and compounds with activity against enteroviruses (EV) of groups C and D, and even rhinoviruses (RV). Our findings provide novel insights in the biology of the entry of entero-/rhinoviruses and open new avenues for the design of broad-spectrum antivirals against these pathogens.	Jun 2019
I04-1-Macromolecular Crystallography (fixed wavelength) I24-Microfocus Macromolecular Crystallography	BAF complex vulnerabilities in cancer demonstrated via structure-based PROTAC design William Farnaby , Manfred Koegl , Michael J. Roy , Claire Whitworth , Emelyne Diers , Nicole Trainor , David Zollman , Steffen Steurer , Jale Karolyi-oezguer , Carina Riedmueller , Teresa Gmaschitz , Johannes Wachter , Christian Dank , Michael Galant , Bernadette Sharps , Klaus Rumpel , Elisabeth Traxler , Thomas Gerstberger , Renate Schnitzer , Oliver Petermann , Peter Greb , Harald Weinstabl , Gerd Bader , Andreas Zoephel , Alexander Weiss-puxbaum , Katharina Ehrenhöfer-wölfer , Simon Wöhrle , Guido Boehmelt , Joerg Rinnenthal , Heribert Arnhof , Nicola Wiechens , Meng-ying Wu , Tom Owen-hughes , Peter Ettmayer , Mark Pearson , Darryl B. Mcconnell , Alessio Ciulli Nature Chemical Biology DOI: 10.1038/s41589-019-0294-6 Diamond Proposal Number(s): [14980] Show Abstract ▼ Abstract: Targeting subunits of BAF/PBAF chromatin remodeling complexes has been proposed as an approach to exploit cancer vulnerabilities. Here, we develop proteolysis targeting chimera (PROTAC) degraders of the BAF ATPase subunits SMARCA2 and SMARCA4 using a bromodomain ligand and recruitment of the E3 ubiquitin ligase VHL. High-resolution ternary complex crystal structures and biophysical investigation guided rational and efficient optimization toward ACBI1, a potent and cooperative degrader of SMARCA2, SMARCA4 and PBRM1. ACBI1 induced anti-proliferative effects and cell death caused by SMARCA2 depletion in SMARCA4 mutant cancer cells, and in acute myeloid leukemia cells dependent on SMARCA4 ATPase activity. These findings exemplify a successful biophysics- and structure-based PROTAC design approach to degrade high profile drug targets, and pave the way toward new therapeutics for the treatment of tumors sensitive to the loss of BAF complex ATPases.	Jun 2019

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