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20 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2 [Next/Last]

Instruments / Technical Area	Publication Details	Published
B22-Multimode InfraRed imaging And Microspectroscopy	Observation of binding of carbon dioxide to nitro-decorated metal–organic frameworks Thien D. Duong , Sergey A. Sapchenko , Ivan Da Silva , Harry G. W. Godfrey , Yongqiang Cheng , Luke L. Daemen , Pascal Manuel , Mark D. Frogley , Gianfelice Cinque , Anibal J. Ramirez-cuesta , Sihai Yang , Martin Schroeder Chemical Science 325 DOI: 10.1039/C9SC04294F Diamond Proposal Number(s): [14938] Open Access Show Abstract ▼ Abstract: Metal–organic frameworks (MOFs) functionalised with amine, amide and hydroxyl groups show great promise for CO2 binding due to their ability to form hydrogen bonds to CO2. Herein we report the adsorption and selectivity of CO2 in four iso-reticular MOFs adopting the NbO topology. Functionalisation of the parent MOF, MFM-102, with –NO2, –NH2 and alkyl groups leads to an enhancement of CO2 adsorption of up to 36% for the NO2-decorated MOF and with raised selectivity. MFM-102-NO2 shows the highest adsorption capacity for CO2 (184 cm3 g−1 at 273 K and 1.0 bar) within this series, comparable to the best-behaving iso-reticular MOFs. At 298 K and 1.0 bar, MFM-102-NO2 shows a CO2/CH4 selectivity of 5.0. In situ inelastic neutron scattering and synchrotron FT-IR micro-spectroscopy were employed to elucidate the host–guest interaction dynamics within CO2-loaded MFM-102-NO2. Neutron powder diffraction enabled the direct observation of the preferred binding domains in MFM-102-NO2, and, to the best of our knowledge, we report the first example of CO2 binding to a –NO2 group in a porous MOF. Synergistic effects between the –NO2 group and the open metal sites lead to optimal binding of CO2 molecules within MFM-102-NO2 via hydrogen bonding to C–H groups.	May 2020
I11-High Resolution Powder Diffraction	Control of zeolite pore interior for chemoselective alkyne/olefin separations Yuchao Chai , Xue Han , Weiyao Li , Shanshan Liu , Sikai Yao , Chong Wang , Wei Shi , Ivan Da Silva , Pascal Manuel , Yongqiang Cheng , Luke D. Daemen , Anibal J. Ramirez-cuesta , Chiu C. Tang , Ling Jiang , Sihai Yang , Naijia Guan , Landong Li Science 368, 1002 - 1006 DOI: 10.1126/science.aay8447 Diamond Proposal Number(s): [23483] Open Access Show Abstract ▼ Abstract: The efficient removal of alkyne impurities for the production of polymer-grade lower olefins remains an important and challenging goal for many industries. We report a strategy to control the pore interior of faujasite (FAU) zeolites by the confinement of isolated open nickel(II) sites in their six-membered rings. Under ambient conditions, Ni@FAU showed remarkable adsorption of alkynes and efficient separations of acetylene/ethylene, propyne/propylene, and butyne/1,3-butadiene mixtures, with unprecedented dynamic separation selectivities of 100, 92, and 83, respectively. In situ neutron diffraction and inelastic neutron scattering revealed that confined nickel(II) sites enabled chemoselective and reversible binding to acetylene through the formation of metastable [Ni(II)(C2H2)3] complexes. Control of the chemistry of pore interiors of easily scalable zeolites has unlocked their potential in challenging industrial separations.	May 2020
B18-Core EXAFS I11-High Resolution Powder Diffraction	Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite Longfei Lin , Alena M. Sheveleva , Ivan Da Silva , Christopher M. A. Parlett , Zhimou Tang , Yueming Liu , Mengtian Fan , Xue Han , Joseph H. Carter , Floriana Tuna , Eric J. L. Mcinnes , Yongqiang Cheng , Luke L. Daemen , Svemir Rudic , Anibal J. Ramirez-cuesta , Chiu C. Tang , Sihai Yang Nature Materials 19, 86 - 93 DOI: 10.1038/s41563-019-0562-6 Diamond Proposal Number(s): [15151, 24726] Show Abstract ▼ Abstract: The efficient production of light olefins from renewable biomass is a vital and challenging target to achieve future sustainable chemical processes. Here we report a hetero-atomic MFI-type zeolite (NbAlS-1), over which aqueous solutions of γ-valerolactone (GVL), obtained from biomass-derived carbohydrates, can be quantitatively converted into butenes with a yield of >99% at ambient pressure under continuous flow conditions. NbAlS-1 incorporates simultaneously niobium(v) and aluminium(iii) centres into the framework and thus has a desirable distribution of Lewis and Brønsted acid sites with optimal strength. Synchrotron X-ray diffraction and absorption spectroscopy show that there is cooperativity between Nb(v) and the Brønsted acid sites on the confined adsorption of GVL, whereas the catalytic mechanism for the conversion of the confined GVL into butenes is revealed by in situ inelastic neutron scattering, coupled with modelling. This study offers a prospect for the sustainable production of butene as a platform chemical for the manufacture of renewable materials.	Dec 2019
B07-C-Versatile Soft X-ray beamline: Ambient Pressure XPS and NEXAFS B18-Core EXAFS E01-JEM ARM 200CF	Influence of synthesis conditions on the structure of nickel nanoparticles and their reactivity in selective asymmetric hydrogenation Rosa Arrigo , Simone Gallarati , Manfred E. Schuster , Jake Seymour , Diego Gianolio , Ivan Da Silva , June Callison , Haosheng Feng , John E. Proctor , Pilar Ferrer , Federica Venturini , Dave Grinter , Georg Held Chemcatchem DOI: 10.1002/cctc.201901955 Open Access Show Abstract ▼ Abstract: Unsupported and SiO 2 ‐supported Ni nanoparticles (NPs), were synthesised via hot‐injection colloidal route using oleylamine (OAm) and trioctylphosphine (TOP) as reducing and protective agents, respectively. By adopting a multi‐length scale structural characterization, it was found that by changing equivalents of OAM and TOP not only the size of the nanoparticles is affected but also the Ni electronic structure. The synthetized NPs were modified with ( R , R )‐tartaric acid (TA) and investigated in the asymmetric hydrogenation of methyl acetoacetate to chiral methyl‐3‐hydroxy butyrate. The comparative analysis of structure and catalytic performance for the synthetized catalysts has enabled us to identify a Ni metallic active surface, whereby the activity increases with the size of the metallic domains. Conversely, at the high conversion obtained for the unsupported NPs there was no impact of particle size on the selectivity. ( R )‐selectivity was very high only on catalysts containing positively charged Ni species such as over the SiO 2 ‐supported NiO NPs. This work shows that the chiral modification of metallic Ni NPs with TA is insufficient to maintain high selectivity towards the ( R )‐enantiomer at long reaction time and provide guidance for the engineering of long‐term stable enantioselective catalysts.	Dec 2019
I11-High Resolution Powder Diffraction	Iodine adsorption in a redox-active metal–organic framework: electrical conductivity induced by host−guest charge-transfer 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 Inorganic Chemistry DOI: 10.1021/acs.inorgchem.9b02176 Diamond Proposal Number(s): [21079] Show Abstract ▼ 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.	Sep 2019
I11-High Resolution Powder Diffraction	[Zr6O4(OH)4(benzene-1,4-dicarboxylato)6]n: a hexagonal polymorph of UiO-66 Maite Perfecto-irigaray , Garikoitz Beobide , Oscar Castillo , Ivan Da Silva , Daniel García-lojo , Antonio Luque , Ander Mendia , Sonia Perez-yanez Chemical Communications DOI: 10.1039/C9CC00802K Diamond Proposal Number(s): [17788] Show Abstract ▼ Abstract: Since its discovery in 2008, the paradigmatic UiO-66 has behaved as the germ that has prompted the chemistry of group-4 metal based metal-organic frameworks, all of them featured by outstanding thermal and chemical stability. Herein we present the first polymorph of UiO-66 and key conditions that led to its formation.	Apr 2019
	New strategy of controlled, stepwise release from novel MBioF and its potential application for drug delivery systems Adam Bieniek , Marek Wiśniewski , Katarzyna Roszek , Paulina Bolibok , Artur P. Terzyk , Pilar Ferrer , Ivan Da Silva Adsorption 29 DOI: 10.1007/s10450-018-00002-4 Open Access Show Abstract ▼ Abstract: Metal organic structures have gained recently an interest in many fields. Among them, metal–biomolecule framework materials with amino acids applied as organic linkers have attracted the growing attention. An application of tailored metal–biomolecule frameworks, easily decomposing in an acidic and/or reductive environment in a steerable way, is reported here. From these biocompatible, non-porous, and nanostructured drug carrier systems, the desirable portion of drug could be released depending on the portion of acid, i.e. immediately and/or in a multi-step process due to a structure decomposition. The application of naturally occurring elements as cystine ensures full biocompatibility of the obtained system as well as its degradation products. Presented materials offer potential application in drug delivery systems.	Feb 2019
	Testing the self-cleaning properties of a coordination polymer surface Artur P. Terzyk , Grzegorz S. Szymański , Emil D. Korczeniewski , Paweł Bryk , Adam Bieniek , Paulina Bolibok , Michał Chodkowski , Piotr Kowalczyk , Marek Wiśniewski , Pilar Ferrer , Ivan Da Silva Adsorption 25, 33 - 39 DOI: 10.1007/s10450-018-9987-5 Open Access Show Abstract ▼ Abstract: It is well established that self-cleaning can be related to the hydrophobic or hydrophilic nature of a surface. Using adsorption chromatography, molecular simulations and wetting dynamics measurements, the self-cleaning properties of a new, strongly water resistant and hydrophilic cystine-containing coordination polymer (CP) were tested. Adsorption isotherms of n-octane and methanol were determined in the range of 313–343 K. Next the isosteric enthalpy of adsorption and the change in adsorption entropy were calculated to explain higher adsorption of methanol than n-butane. Performed chromatographic tests, molecular dynamics simulations and wetting dynamics experiments additionally prove that the Zn(Cys)2 CP is a promising material for the application in the preperation of self-cleaning surfaces or coatings.	Jan 2019
I11-High Resolution Powder Diffraction	Exceptional adsorption and binding of sulfur dioxide in a robust zirconium-based metal–organic framework Joseph H. Carter , Xue Han , Florian Y. Moreau , Ivan Da Silva , Adam Nevin , Harry G. W. Godfrey , Chiu C. Tang , Sihai Yang , Martin Schroeder Journal Of The American Chemical Society DOI: 10.1021/jacs.8b08433 Diamond Proposal Number(s): [14341] Show Abstract ▼ Abstract: We report a record-high SO2 adsorption capacity of 12.3 mmol g–1 in a robust porous material, MFM-601, at 298 K and 1.0 bar. SO2 adsorption in MFM-601 is fully reversible and highly selective over CO2 and N2. The binding domains for adsorbed SO2 and CO2 molecules in MFM-601 have been determined by in situ synchrotron X-ray diffraction experiments, giving insights at the molecular level to the basis of the observed high selectivity.	Nov 2018
	Cystine-based MBioF for maintaining the antioxidant-oxidant balance in airways diseases Marek Wiśniewski , Adam Bieniek , Katarzyna Roszek , Joanna Czarnecka , Paulina Bolibok , Pilar Ferrer , Ivan Da Silva , Artur Piotr Terzyk Acs Medicinal Chemistry Letters DOI: 10.1021/acsmedchemlett.8b00468 Show Abstract ▼ Abstract: Reactive oxygen species, contributing to oxidant-antioxidant imbalance, initiate damage to the airways cells, inflammatory processes and further pathophysiological effects. Enhancing anti-oxidant properties is the main prophylactic and therapeutic challenge. In this work, a newly synthesized and biocompatible structure of the metal-biomolecule frameworks (MBioF) harnessing cystine as a linker and magnesium as metal nodes, is presented. This structure provides crucial sulfhydryl groups of cysteine, with antioxidant activity, released stepwise in the site of delivery. We prove that once released, the compounds of MBioF increase the intracellular level of cysteine and total antioxidative capability of airways cells. Presented MBioF structures offer new perspectives for clinical applications as therapeutics or preventives maintaining the antioxidant-oxidant balance.	Nov 2018

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