Krios I-Titan Krios I at Diamond
Krios II-Titan Krios II at Diamond
Krios IV-Titan Krios IV at Diamond
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Jianbing
Ma
,
Gangshun
Yi
,
Mingda
Ye
,
Craig
Macgregor-Chatwin
,
Yuewen
Sheng
,
Ying
Lu
,
Ming
Li
,
Qingrong
Li
,
Dong
Wang
,
Robert J. C.
Gilbert
,
Peijun
Zhang
Diamond Proposal Number(s):
[29812]
Open Access
Abstract: The cryo-electron microscopy (cryoEM) method has enabled high-resolution structure determination of numerous biomolecules and complexes. Nevertheless, cryoEM sample preparation of challenging proteins and complexes, especially those with low abundance or with preferential orientation, remains a major hurdle. We developed an affinity-grid method employing monodispersed single particle streptavidin on a lipid monolayer to enhance particle absorption on the grid surface and alleviate sample exposure to the air-water interface. Using this approach, we successfully enriched the Thermococcus kodakarensis mini-chromosome maintenance complex 3 (MCM3) on cryoEM grids through biotinylation and resolved its structure. We further utilized this affinity method to tether the biotin-tagged dsDNA to selectively enrich a stable MCM3-ATP-dsDNA complex for cryoEM structure determination. Intriguingly, both MCM3 apo and dsDNA bound structures exhibit left-handed open spiral conformations, distinct from other reported MCM structures. The large open gate is sufficient to accommodate a dsDNA which could potentially be melted. The value of mspSA affinity method was further demonstrated by mitigating the issue of preferential angular distribution of HIV-1 capsid protein hexamer and RNA polymerase II elongation complex from Saccharomyces cerevisiae.
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Dec 2024
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B22-Multimode InfraRed imaging And Microspectroscopy
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Diamond Proposal Number(s):
[22137, 30398]
Open Access
Abstract: Metal–organic framework (MOF) materials are attracting increasing interest in the field of electronics due to their structural diversity, intrinsic porosity, and designable host–guest interactions. Here, we report the dielectric properties of a series of robust materials, MFM-300(M) (M = Al, Sc, Cr, Fe, Ga, In), when exposed to different guest molecules. MFM-300(Fe) exhibits the most notable increase in dielectric constant to 35.3 ± 0.3 at 10 kHz upon adsorption of NH3. Structural analysis suggests that the electron delocalization induced by host–guest interactions between NH3 and the MOF host, as confirmed by neutron powder diffraction studies, leads to structural polarization, resulting in a high dielectric constant for NH3@MFM-300(Fe). This is further supported by ligand-to-metal charge-transfer transitions observed by solid-state UV/vis spectroscopy. The high detection sensitivity and stability to NH3 suggest that MFM-300(Fe) may act as a powerful dielectric-based sensor for NH3.
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Oct 2023
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B22-Multimode InfraRed imaging And Microspectroscopy
I11-High Resolution Powder Diffraction
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Jin
Chen
,
Qingqing
Mei
,
Yinlin
Chen
,
Christopher
Marsh
,
Bing
An
,
Xue
Han
,
Ian P.
Silverwood
,
Ming
Li
,
Yongqiang
Cheng
,
Meng
He
,
Xi
Chen
,
Weiyao
Li
,
Meredydd
Kippax-Jones
,
Danielle
Crawshaw
,
Mark D.
Frogley
,
Sarah J.
Day
,
Victoria
García-Sakai
,
Pascal
Manuel
,
Anibal J.
Ramirez-Cuesta
,
Sihai
Yang
,
Martin
Schroeder
Diamond Proposal Number(s):
[29649]
Open Access
Abstract: The development of materials showing rapid proton conduction with a low activation energy and stable performance over a wide temperature range is an important and challenging line of research. Here, we report confinement of sulfuric acid within porous MFM-300(Cr) to give MFM-300(Cr)·SO4(H3O)2, which exhibits a record-low activation energy of 0.04 eV, resulting in stable proton conductivity between 25 and 80 °C of >10–2 S cm–1. In situ synchrotron X-ray powder diffraction (SXPD), neutron powder diffraction (NPD), quasielastic neutron scattering (QENS), and molecular dynamics (MD) simulation reveal the pathways of proton transport and the molecular mechanism of proton diffusion within the pores. Confined sulfuric acid species together with adsorbed water molecules play a critical role in promoting the proton transfer through this robust network to afford a material in which proton conductivity is almost temperature-independent.
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Jul 2022
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I11-High Resolution Powder Diffraction
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Xi
Chen
,
Zhongyue
Zhang
,
Jin
Chen
,
Sergei
Sapchenko
,
Xue
Han
,
Ivan
Da Silva
,
Ming
Li
,
Inigo
Vitorica-Yrezabal
,
George
Whitehead
,
Chiu C.
Tang
,
Kunio
Awaga
,
Sihai
Yang
,
Martin
Schroeder
Diamond Proposal Number(s):
[22138]
Abstract: MFM-722(Pb)-DMA undergoes a single-crystal-to-single-crystal (SCSC) transformation to give MFM-722(Pb)-H2O via ligand substitution upon exposure to water vapour. In situ single crystal impedance spectroscopy reveals an increase in proton conductivity due to this structural transition, with MFM-722(Pb)-H2O showing a proton conductivity of 6.61×10-4 S cm-1 at 50 °C and 98% RH. The low activation energy (Ea = 0.21 eV) indicates that the proton conduction follows a Grotthuss mechanism.
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Nov 2020
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E01-JEM ARM 200CF
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Ruoyu
Xu
,
Jingwei
Xiang
,
Junrun
Feng
,
Xuekun
Lu
,
Zhangxiang
Hao
,
Liqun
Kang
,
Ming
Li
,
Yunsong
Wu
,
Chun
Tan
,
Yiyun
Liu
,
Guanjie
He
,
Dan J. L.
Brett
,
Paul R.
Shearing
,
Lixia
Yuan
,
Yunhui
Huang
,
Feng Ryan
Wang
Diamond Proposal Number(s):
[17559, 19318, 19246, 20643]
Abstract: The lithium-sulfur (Li-S) batteries have high theoretical energy density, exceeding that of the lithium-ion batteries. However, their practical applications are hindered by the capacity decay due to lithium polysulfide shuttle effect and sulfur volume expansion. Here, we design a S@hollow carbon with porous shell/MnOx (S@HCS/MnOx) cathode to accommodate and immobilize sulfur and polysulfides, and develop a non-destructive technique X-ray computed tomography (X-ray CT) to in situ visualize the volume expansion of Li-S cathode. The designed cathode achieves a specific capacity of ~1100 mAh g-1 at 0.2 C with a fade rate of 0.18% per cycle over 300 cycles. The X-ray CT shows that only 16% volume expansion and 70% volume fraction of solid sulfur remaining in the S@HCS/MnOx cathode, superior to the commercial cathode with 40% volume expansion and 5% volume remaining of solid sulfur particles. This is the first reported visualization evidence for the effectiveness of hollow carbon structure in accommodating cathode volume expansion and immobilizing sulfur shuttling. X-ray CT can serve as a powerful in situ tool to trace the active materials and then feedback to the structure design, which helps develop efficient and reliable energy storage systems.
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Oct 2020
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I11-High Resolution Powder Diffraction
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Xinran
Zhang
,
Ivan
Da Silva
,
Rodrigo
Fazzi
,
Alena M.
Sheveleva
,
Xue
Han
,
Ben F.
Spencer
,
Sergey A.
Sapchenko
,
Floriana
Tuna
,
Eric J. L.
Mcinnes
,
Ming
Li
,
Sihai
Yang
,
Martin
Schroder
Diamond Proposal Number(s):
[21079]
Open Access
Abstract: We report a comparative study of the binding of I2 (iodine) in a pair of redox-active metal–organic framework (MOF) materials, MFM-300(VIII) and its oxidized, deprotonated analogue, MFM-300(VIV). Adsorption of I2 in MFM-300(VIII) triggers a host-to-guest charge-transfer, accompanied by a partial (∼30%) oxidation of the VIII centers in the host framework and formation of I3– species residing in the MOF channels. Importantly, this charge-transfer induces a significant enhancement in the electrical conductivity (Δσ = 700000) of I2@MFM-300(VIII/IV) in comparison to MFM-300(VIII). In contrast, no host–guest charge-transfer or apparent change in the conductivity was observed upon adsorption of I2 in MFM-300(VIV). High-resolution synchrotron X-ray diffraction of I2@MFM-300(VIII/IV) confirms the first example of self-aggregation of adsorbed iodine species (I2 and I3–) into infinite helical chains within a MOF.
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Sep 2019
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I19-Small Molecule Single Crystal Diffraction
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Peter
Rought
,
Christopher
Marsh
,
Simona
Pili
,
Ian P.
Silverwood
,
Victoria
Garcia Sakai
,
Ming
Li
,
Martyn
Brown
,
Stephen P.
Argent
,
Inigo
Vitorica-Yrezabal
,
George
Whitehead
,
Mark R.
Warren
,
Sihai
Yang
,
Martin
Schroeder
Diamond Proposal Number(s):
[13650, 12517]
Open Access
Abstract: Three multi-carboxylic acid functionalised ligands have been designed, synthesised and utilised to synthesise the new barium-based MOFs, MFM-510, -511, and -512, which show excellent stability to water-vapour. MFM-510 and MFM-511 show moderate proton conductivities (2.1 x10-5 and 5.1 x10-5 S cm-1, respectively) at 99RH% and 298 K, attributed to the lack of free protons or hindered proton diffusion within the framework structures. In contrast, MFM-512, which incorporates a pendant carboxylic acid group directed into the pore of the framework, shows a two orders of magnitude enhancement in proton conductivity (2.9 x10-3 S cm-1). Quasi-elastic neutron scattering (QENS) suggests that the proton dynamics of MFM-512 are mediated by “free diffusion inside a sphere” confirming that incorporation of free carboxylic acid groups within the pores of MOFs is an efficient albeit a synthetically challenging strategy to improve proton conductivity.
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Nov 2018
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I11-High Resolution Powder Diffraction
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Simona
Pili
,
Peter
Rought
,
Daniil I.
Kolokolov
,
Longfei
Lin
,
Ivan
Da Silva
,
Yongqiang
Cheng
,
Christopher
Marsh
,
Ian P.
Silverwood
,
Victoria
García-Sakai
,
Ming
Li
,
Jeremy J.
Titman
,
Lyndsey
Knight
,
Luke L.
Daemen
,
Anibal J.
Ramirez-Cuesta
,
Chiu C.
Tang
,
Alexander G.
Stepanov
,
Sihai
Yang
,
Martin
Schroeder
Diamond Proposal Number(s):
[13247]
Abstract: Owing to their inherent pore structure, porous metal-organic frameworks (MOFs) can undergo post-synthetic modification, such as loading extra-framework proton carriers. However, strategies for improving the proton conductivity for non-porous MOFs are largely lacking, although increasing numbers of non-porous MOFs exhibit promising proton conductivities. Often, high humidity is required for non-porous MOFs to achieve high conductivities, but to date no clear mechanisms have been experimentally identified. Here we describe the new materials MFM-550(M), [M(HL1)], (H4L1 = biphenyl-4,4'-diphosphonic acid; M = La, Ce, Nd, Sm, Gd, Ho), MFM-550(Ba), [Ba(H2L1)], and MFM-555(M), [M(HL2)], (H4L2 = benzene-1,4-diphosphonic acid; M = La, Ce, Nd, Sm, Gd, Ho), and report enhanced proton conductivities in these non-porous materials by (i) replacing the metal ion to one with a lower oxidation state, (ii) reducing the length of the organic ligand, and (iii) introducing additional acidic protons on MOF surface. Increased framework proton density in these materials can lead to an enhancement in proton conductivity of up to four orders of magnitude. Additionally, we report a comprehensive investigation using in situ 2H NMR and neutron spectroscopy, coupled with molecular dynamic modelling, to elucidate the role of humidity in assembling interconnected networks for proton hopping. This study constructs a relationship between framework proton density and the corresponding proton conductivity in non-porous MOFs, and directly explains the role of both surface protons and external water in assembling the proton conducting pathways.
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Sep 2018
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I11-High Resolution Powder Diffraction
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Alma B.
Santibáñez-Mendieta
,
Christophe
Didier
,
Kenneth K.
Inglis
,
Alex J.
Corkett
,
Michael
Pitcher
,
Marco
Zanella
,
J. Felix
Shin
,
Luke
Daniels
,
Aydar
Rakhmatullin
,
Ming
Li
,
Matthew S.
Dyer
,
John B.
Claridge
,
Frédéric
Blanc
,
Matthew J.
Rosseinsky
Diamond Proposal Number(s):
[12336]
Open Access
Abstract: The structure and Li+ ion dynamics of a new class of ABO3 perovskite with Li on both the A- and B-sites are described. La3Li3W2O12 is synthesised by solid state reaction at 900°C and shown by powder X-ray diffraction to adopt the structure of a monoclinic double perovskite (A2)BBꞌO6, (La1.5Li0.5)WLiO6, with rock salt order of W6+ and Li+ on the B-site. High resolution powder neutron diffraction locates A-site Li in a distorted tetrahedron displaced from the conventional perovskite A-site, which differs considerably from the sites occupied by Li in the well studied La2/3-xLi3xTiO3 family. This is confirmed by the observation of a lower coordinated Li+ ion in the 6Li magic angle spinning nuclear magnetic resonance (NMR) spectra, in addition to the B-site LiO6, and supported computationally by density functional theory (DFT), which also suggests local order of A-site La3+ and Li+. DFT shows that the vacancies necessary for transport can arise from Frenkel or La excess defects, with an energetic cost of ~0.4 eV/vacancy in both cases. Ab initio molecular dynamics establishes that the Li+ ion dynamics occur by a pathway involving a series of multiple localised Li hops between two neighbouring A-sites with an overall energy barrier of ~0.25 eV, with additional possible pathways involving Li exchange between the A- and B-sites. A similar activation energy for Li+ ion mobility (~0.3 eV) was obtained from variable temperature 6Li and 7Li line narrowing and relaxometry NMR experiments, suggesting that the barrier to Li hopping between sites in La3Li3W2O12 is comparable to the best oxide Li+ ion conductors. AC impedance-derived conductivities confirm that Li+ ions are mobile but that the long-range Li+ diffusion has a higher barrier (~0.5 eV) which may be associated with blocking of transport by A-site La3+ ions.
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Sep 2016
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I11-High Resolution Powder Diffraction
I19-Small Molecule Single Crystal Diffraction
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Simona
Pili
,
Stephen
Argent
,
Christopher
Morris
,
Peter
Rought
,
Victoria
García-Sakai
,
Ian
Silverwood
,
Timothy
Easun
,
Ming
Li
,
Mark
Warren
,
Claire
Murray
,
Chiu
Tang
,
Sihai
Yang
,
Martin
Schroeder
Open Access
Abstract: Understanding the molecular mechanism of proton conduction is crucial for the design of new materials with improved conductivity. Quasi-elastic neutron scattering (QENS) has been used to probe the mechanism of proton diffusion within a new phosphonate-based metal–organic framework (MOF) material, MFM-500(Ni). QENS suggests that the proton conductivity (4.5 × 10–4 S/cm at 98% relative humidity and 25 °C) of MFM-500(Ni) is mediated by intrinsic “free diffusion inside a sphere”, representing the first example of such a mechanism observed in MOFs.
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May 2016
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