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751 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
I18-Microfocus Spectroscopy	Adsorption of rare earth elements in regolith-hosted clay deposits Anouk M. Borst , Martin P. Smith , Adrian Finch , Guillaume Estrade , Cristina Villanova-de-benavent , Peter Nason , Eva Marquis , Nicola J. Horsburgh , Kathryn M. Goodenough , Cheng Xu , Jindřich Kynický , Kalotina Geraki Nature Communications 11 DOI: 10.1038/s41467-020-17801-5 Diamond Proposal Number(s): [14793, 15903] Open Access Show Abstract ▼ Abstract: Global resources of heavy Rare Earth Elements (REE) are dominantly sourced from Chinese regolith-hosted ion-adsorption deposits in which the REE are inferred to be weakly adsorbed onto clay minerals. Similar deposits elsewhere might provide alternative supply for these high-tech metals, but the adsorption mechanisms remain unclear and the adsorbed state of REE to clays has never been demonstrated in situ. This study compares the mineralogy and speciation of REE in economic weathering profiles from China to prospective regoliths developed on peralkaline rocks from Madagascar. We use synchrotron X-ray absorption spectroscopy to study the distribution and local bonding environment of Y and Nd, as proxies for heavy and light REE, in the deposits. Our results show that REE are truly adsorbed as easily leachable 8- to 9-coordinated outer-sphere hydrated complexes, dominantly onto kaolinite. Hence, at the atomic level, the Malagasy clays are genuine mineralogical analogues to those currently exploited in China.	Dec 2020
E02-JEM ARM 300CF	A fundamental look at electrocatalytic sulfur reduction reaction Lele Peng , Ziyang Wei , Chengzhang Wan , Jing Lin , Zhuo Chen , Dan Zhu , Daniel Baumann , Haotian Liu , Christopher S. Allen , Xiang Xu , Angus I. Kirkland , Imran Shakir , Zeyad Almutairi , Sarah Tolbert , Bruce Dunn , Yu Huang , Philippe Sautet , Xiangfeng Duan Nature Catalysis 3, 762 - 770 DOI: 10.1038/s41929-020-0498-x Diamond Proposal Number(s): [23956] Show Abstract ▼ Abstract: The fundamental kinetics of the electrocatalytic sulfur reduction reaction (SRR), a complex 16-electron conversion process in lithium–sulfur batteries, is so far insufficiently explored. Here, by directly profiling the activation energies in the multistep SRR, we reveal that the initial reduction of sulfur to the soluble polysulfides is relatively easy owing to the low activation energy, whereas the subsequent conversion of the polysulfides into the insoluble Li2S2/Li2S has a much higher activation energy, contributing to the accumulation of polysulfides and exacerbating the polysulfide shuttling effect. We use heteroatom-doped graphene as a model system to explore electrocatalytic SRR. We show that nitrogen and sulfur dual-doped graphene considerably reduces the activation energy to improve SRR kinetics. Density functional calculations confirm that the doping tunes the p-band centre of the active carbons for an optimal adsorption strength of intermediates and electroactivity. This study establishes electrocatalysis as a promising pathway to tackle the fundamental challenges facing lithium–sulfur batteries.	Sep 2020
I21-Resonant Inelastic X-ray Scattering (RIXS)	First-cycle voltage hysteresis in Li-rich 3d cathodes associated with molecular O2 trapped in the bulk Robert A. House , Gregory J. Rees , Miguel A. Pérez-osorio , John-joseph Marie , Edouard Boivin , Alex W. Robertson , Abhishek Nag , Mirian Garcia-fernandez , Kejin Zhou , Peter G. Bruce Nature Energy 137 DOI: 10.1038/s41560-020-00697-2 Diamond Proposal Number(s): [23889] Show Abstract ▼ Abstract: Li-rich cathode materials are potential candidates for next-generation Li-ion batteries. However, they exhibit a large voltage hysteresis on the first charge/discharge cycle, which involves a substantial (up to 1 V) loss of voltage and therefore energy density. For Na cathodes, for example Na0.75[Li0.25Mn0.75]O2, voltage hysteresis can be explained by the formation of molecular O2 trapped in voids within the particles. Here we show that this is also the case for Li1.2Ni0.13Co0.13Mn0.54O2. Resonant inelastic X-ray scattering and 17O magic angle spinning NMR spectroscopy show that molecular O2, rather than O22−, forms within the particles on the oxidation of O2− at 4.6 V versus Li+/Li on charge. These O2 molecules are reduced back to O2− on discharge, but at the lower voltage of 3.75 V, which explains the voltage hysteresis in Li-rich cathodes. 17O magic angle spinning NMR spectroscopy indicates a quantity of bulk O2 consistent with the O-redox charge capacity minus the small quantity of O2 loss from the surface. The implication is that O2, trapped in the bulk and lost from the surface, can explain O-redox.	Sep 2020
	Broad and strong memory CD4+ and CD8+ T cells induced by SARS-CoV-2 in UK convalescent individuals following COVID-19 Yanchun Peng , Alexander J. Mentzer , Guihai Liu , Xuan Yao , Zixi Yin , Danning Dong , Wanwisa Dejnirattisai , Timothy Rostron , Piyada Supasa , Chang Liu , César López-camacho , Jose Slon-campos , Yuguang Zhao , David I. Stuart , Guido C. Paesen , Jonathan M. Grimes , Alfred A. Antson , Oliver W. Bayfield , Dorothy E. D. P. Hawkins , De-sheng Ker , Beibei Wang , Lance Turtle , Krishanthi Subramaniam , Paul Thomson , Ping Zhang , Christina Dold , Jeremy Ratcliff , Peter Simmonds , Thushan De Silva , Paul Sopp , Dannielle Wellington , Ushani Rajapaksa , Yi-ling Chen , Mariolina Salio , Giorgio Napolitani , Wayne Paes , Persephone Borrow , Benedikt M. Kessler , Jeremy W. Fry , Nikolai F. Schwabe , Malcolm G. Semple , J. Kenneth Baillie , Shona C. Moore , Peter J. M. Openshaw , M. Azim Ansari , Susanna Dunachie , Eleanor Barnes , John Frater , Georgina Kerr , Oliver Gould , Teresa Lockett , Robert Levin , Yonghong Zhang , Ronghua Jing , Ling-pei Ho , Richard J. Cornall , Christopher P. Conlon , Paul Klenerman , Gavin R. Screaton , Juthathip Mongkolsapaya , Andrew Mcmichael , Julian C. Knight , Graham Ogg , Tao Dong Nature Immunology 7 DOI: 10.1038/s41590-020-0782-6 Open Access Show Abstract ▼ Abstract: The development of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) vaccines and therapeutics will depend on understanding viral immunity. We studied T cell memory in 42 patients following recovery from COVID-19 (28 with mild disease and 14 with severe disease) and 16 unexposed donors, using interferon-γ-based assays with peptides spanning SARS-CoV-2 except ORF1. The breadth and magnitude of T cell responses were significantly higher in severe as compared with mild cases. Total and spike-specific T cell responses correlated with spike-specific antibody responses. We identified 41 peptides containing CD4+ and/or CD8+ epitopes, including six immunodominant regions. Six optimized CD8+ epitopes were defined, with peptide–MHC pentamer-positive cells displaying the central and effector memory phenotype. In mild cases, higher proportions of SARS-CoV-2-specific CD8+ T cells were observed. The identification of T cell responses associated with milder disease will support an understanding of protective immunity and highlights the potential of including non-spike proteins within future COVID-19 vaccine design.	Sep 2020
Krios III-Titan Krios III at Diamond	Assembly intermediates of orthoreovirus captured in the cell Geoff Sutton , Dapeng Sun , Xiaofeng Fu , Abhay Kotecha , Corey W. Hecksel , Daniel K. Clare , Peijun Zhang , David I. Stuart , Mark Boyce Nature Communications 11 DOI: 10.1038/s41467-020-18243-9 Diamond Proposal Number(s): [18477] Open Access Show Abstract ▼ Abstract: Traditionally, molecular assembly pathways for viruses are inferred from high resolution structures of purified stable intermediates, low resolution images of cell sections and genetic approaches. Here, we directly visualise an unsuspected ‘single shelled’ intermediate for a mammalian orthoreovirus in cryo-preserved infected cells, by cryo-electron tomography of cellular lamellae. Particle classification and averaging yields structures to 5.6 Å resolution, sufficient to identify secondary structural elements and produce an atomic model of the intermediate, comprising 120 copies each of protein λ1 and σ2. This λ1 shell is ‘collapsed’ compared to the mature virions, with molecules pushed inwards at the icosahedral fivefolds by ~100 Å, reminiscent of the first assembly intermediate of certain prokaryotic dsRNA viruses. This supports the supposition that these viruses share a common ancestor, and suggests mechanisms for the assembly of viruses of the Reoviridae. Such methodology holds promise for dissecting the replication cycle of many viruses.	Sep 2020
	Segmented flow generator for serial crystallography at the European X-ray free electron laser Austin Echelmeier , Jorvani Cruz Villarreal , Marc Messerschmidt , Daihyun Kim , Jesse D. Coe , Darren Thifault , Sabine Botha , Ana Egatz-gomez , Sahir Gandhi , Gerrit Brehm , Chelsie E. Conrad , Debra T. Hansen , Caleb Madsen , Saša Bajt , J. Domingo Meza-aguilar , Dominik Oberthuer , Max O. Wiedorn , Holger Fleckenstein , Derek Mendez , Juraj Knoška , Jose M. Martin-garcia , Hao Hu , Stella Lisova , Aschkai Allahgoli , Yaroslav Gevorkov , Kartik Ayyer , Steve Aplin , Helen M. Ginn , Heinz Graafsma , Andrew J. Morgan , Dominic Greiffenberg , Alexander Klujev , Torsten Laurus , Jennifer Poehlsen , Ulrich Trunk , Davide Mezza , Bernd Schmitt , Manuela Kuhn , Raimund Fromme , Jolanta Sztuk-dambietz , Natascha Raab , Steffen Hauf , Alessandro Silenzi , Thomas Michelat , Chen Xu , Cyril Danilevski , Andrea Parenti , Leonce Mekinda , Britta Weinhausen , Grant Mills , Patrik Vagovic , Yoonhee Kim , Henry Kirkwood , Richard Bean , Johan Bielecki , Stephan Stern , Klaus Giewekemeyer , Adam Round , Joachim Schulz , Katerina Dörner , Thomas D. Grant , Valerio Mariani , Anton Barty , Adrian P. Mancuso , Uwe Weierstall , John C. H. Spence , Henry N. Chapman , Nadia Zatsepin , Petra Fromme , Richard A. Kirian , Alexandra Ros Nature Communications 11 DOI: 10.1038/s41467-020-18156-7 Open Access Show Abstract ▼ Abstract: Serial femtosecond crystallography (SFX) with X-ray free electron lasers (XFELs) allows structure determination of membrane proteins and time-resolved crystallography. Common liquid sample delivery continuously jets the protein crystal suspension into the path of the XFEL, wasting a vast amount of sample due to the pulsed nature of all current XFEL sources. The European XFEL (EuXFEL) delivers femtosecond (fs) X-ray pulses in trains spaced 100 ms apart whereas pulses within trains are currently separated by 889 ns. Therefore, continuous sample delivery via fast jets wastes >99% of sample. Here, we introduce a microfluidic device delivering crystal laden droplets segmented with an immiscible oil reducing sample waste and demonstrate droplet injection at the EuXFEL compatible with high pressure liquid delivery of an SFX experiment. While achieving ~60% reduction in sample waste, we determine the structure of the enzyme 3-deoxy-D-manno-octulosonate-8-phosphate synthase from microcrystals delivered in droplets revealing distinct structural features not previously reported.	Sep 2020
I03-Macromolecular Crystallography	Key role of quinone in the mechanism of respiratory complex I Javier Gutierrez-fernandez , Karol Kaszuba , Gurdeep S. Minhas , Rozbeh Baradaran , Margherita Tambalo , David T. Gallagher , Leonid A. Sazanov Nature Communications 11 DOI: 10.1038/s41467-020-17957-0 Diamond Proposal Number(s): [8547] Open Access Show Abstract ▼ Abstract: Complex I is the first and the largest enzyme of respiratory chains in bacteria and mitochondria. The mechanism which couples spatially separated transfer of electrons to proton translocation in complex I is not known. Here we report five crystal structures of T. thermophilus enzyme in complex with NADH or quinone-like compounds. We also determined cryo-EM structures of major and minor native states of the complex, differing in the position of the peripheral arm. Crystal structures show that binding of quinone-like compounds (but not of NADH) leads to a related global conformational change, accompanied by local re-arrangements propagating from the quinone site to the nearest proton channel. Normal mode and molecular dynamics analyses indicate that these are likely to represent the first steps in the proton translocation mechanism. Our results suggest that quinone binding and chemistry play a key role in the coupling mechanism of complex I.	Aug 2020
Krios III-Titan Krios III at Diamond Krios IV-Titan Krios IV at Diamond	Molecular architecture and activation of the insecticidal protein Vip3Aa from Bacillus thuringiensis Rafael Nunez-ramirez , Juanjo Huesa , Yolanda Bel , Juan Ferré , Patricia Casino , Ernesto Arias-palomo Nature Communications 11 DOI: 10.1038/s41467-020-17758-5 Diamond Proposal Number(s): [21062, 24924] Open Access Show Abstract ▼ Abstract: Bacillus thuringiensis Vip3 (Vegetative Insecticidal Protein 3) toxins are widely used in biotech crops to control Lepidopteran pests. These proteins are produced as inactive protoxins that need to be activated by midgut proteases to trigger cell death. However, little is known about their three-dimensional organization and activation mechanism at the molecular level. Here, we have determined the structures of the protoxin and the protease-activated state of Vip3Aa at 2.9 Å using cryo-electron microscopy. The reconstructions show that the protoxin assembles into a pyramid-shaped tetramer with the C-terminal domains exposed to the solvent and the N-terminal region folded into a spring-loaded apex that, after protease activation, drastically remodels into an extended needle by a mechanism akin to that of influenza haemagglutinin. These results provide the molecular basis for Vip3 activation and function, and serves as a strong foundation for the development of more efficient insecticidal proteins.	Aug 2020
I19-Small Molecule Single Crystal Diffraction	Fast spin-flip enables efficient and stable organic electroluminescence from charge-transfer states Lin-song Cui , Alexander J. Gillett , Shou-feng Zhang , Hao Ye , Yuan Liu , Xian-kai Chen , Ze-sen Lin , Emrys W. Evans , William K. Myers , Tanya K. Ronson , Hajime Nakanotani , Sebastian Reineke , Jean-luc Bredas , Chihaya Adachi , Richard H. Friend Nature Photonics 395 DOI: 10.1038/s41566-020-0668-z Diamond Proposal Number(s): [21497] Show Abstract ▼ Abstract: A spin-flip from a triplet to a singlet excited state, that is, reverse intersystem crossing (RISC), is an attractive route for improving light emission in organic light-emitting diodes, as shown by devices using thermally activated delayed fluorescence (TADF). However, device stability and efficiency roll-off remain challenging issues that originate from a slow RISC rate (kRISC). Here, we report a TADF molecule with multiple donor units that form charge-resonance-type hybrid triplet states leading to a small singlet–triplet energy splitting, large spin–orbit couplings, and a dense manifold of triplet states energetically close to the singlets. The kRISC in our TADF molecule is as fast as 1.5 × 107 s−1, a value some two orders of magnitude higher than typical TADF emitters. Organic light-emitting diodes based on this molecule exhibit good stability (estimated T90 about 600 h for 1,000 cd m−2), high maximum external quantum efficiency (>29.3%) and low efficiency roll-off (<2.3% at 1,000 cd m−2).	Aug 2020
B18-Core EXAFS	Self-supported Pt–CoO networks combining high specific activity with high surface area for oxygen reduction Gustav W. Sievers , Anders W. Jensen , Jonathan Quinson , Alessandro Zana , Francesco Bizzotto , Mehtap Oezaslan , Alexandra Dworzak , Jacob J. K. Kirkensgaard , Thomas E. L. Smitshuysen , Shima Kadkhodazadeh , Mikkel Juelsholt , Kirsten M. Ø. Jensen , Kirsten Anklam , Hao Wan , Jan Schäfer , Klára Čépe , María Escudero-escribano , Jan Rossmeisl , Antje Quade , Volker Brüser , Matthias Arenz Nature Materials 2 DOI: 10.1038/s41563-020-0775-8 Diamond Proposal Number(s): [12746] Show Abstract ▼ Abstract: Several concepts for platinum-based catalysts for the oxygen reduction reaction (ORR) are presented that exceed the US Department of Energy targets for Pt-related ORR mass activity. Most concepts achieve their high ORR activity by increasing the Pt specific activity at the expense of a lower electrochemically active surface area (ECSA). In the potential region controlled by kinetics, such a lower ECSA is counterbalanced by the high specific activity. At higher overpotentials, however, which are often applied in real systems, a low ECSA leads to limitations in the reaction rate not by kinetics, but by mass transport. Here we report on self-supported platinum–cobalt oxide networks that combine a high specific activity with a high ECSA. The high ECSA is achieved by a platinum–cobalt oxide bone nanostructure that exhibits unprecedentedly high mass activity for self-supported ORR catalysts. This concept promises a stable fuel-cell operation at high temperature, high current density and low humidification.	Aug 2020

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