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11 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	A multimodal study on the unique sensing behavior of a guest@metal-organic framework material for the detection of volatile acetone Annika F. Moeslein , Mario Gutierrez , Kirill Titov , Lorenzo Donà , Bartolomeo Civalleri , Mark D. Frogley , Gianfelice Cinque , Svemir Rudic , Jin-Chong Tan Advanced Materials Interfaces 112 DOI: 10.1002/admi.202201401 Diamond Proposal Number(s): [14902, 25407] Open Access Show Abstract ▼ Abstract: Owing to their unique functionalities and tailorable properties that are unattainable in conventional materials, metal-organic frameworks (MOFs) have emerged as candidate materials for next-generation chemical sensors and optoelectronics. For instance, the ZnQ@OX-1 composite material, comprising a light-emitting guest encapsulated in the pores of the OX-1 framework, affords excellent sensing performance: a visible color change upon exposure to volatile acetone. In this work, a multimodal study on the exceptional vapochromism of this composite material using high-resolution spectroscopy techniques based on inelastic neutron scattering and synchrotron radiation is presented, supported by density functional theory calculations. While FTIR spectroscopy in the far-IR and mid-IR regions reveals the underlying interactions between ZnQ, OX-1, and acetone, the limit of detection at 50 ppm is determined through in situ gas dosing experiments using fluorescence spectroscopy. In addition, in situ gas dosing on the single crystal level is achieved with near-field infrared nanospectroscopy.	Dec 2022
	Cryogenic temperature growth of Sn thin films on ferromagnetic Co(0001) Leszek Gladczuk , Lukasz Gladczuk , Piotr Dłuzewski , Pavlo Aleshkevych , Artem Lynnyk , Gerrit Van Der Laan , Thorsten Hesjedal Advanced Materials Interfaces 464 DOI: 10.1002/admi.202201452 Open Access Show Abstract ▼ Abstract: Topological electronic materials hold great promise for revolutionizing spintronics, owing to their topological protected, spin-polarized conduction edge or surface state. One of the key bottlenecks for the practical use of common binary and ternary topological insulator materials is the large defect concentration that leads to a high background carrier concentration. Elemental tin in its α-phase is a room temperature topological semimetal, which is intrinsically less prone to defect-related shortcomings. Recently, the growth of ultrathin α-Sn films on ferromagnetic Co surfaces has been achieved; however, thicker films are needed to reach the 3D topological Dirac semimetallic state. Here, the growth of α-Sn films on Co at cryogenic temperatures was explored. Very low-temperature growth holds the promise of suppressing undesired phases, alloying across the interfaces, as well as the formation of Sn pillars or hillocks. Nevertheless, the critical Sn layer thickness of ≈3 atomic layers, above which the film partially transforms into the undesired b-phase, remains the same as for room-temperature growth. From ferromagnetic resonance studies, and supported by electron microscopy, it can be concluded that for cryogenic Sn layer growth, the interface between Sn and Co remains sharp and the magnetic properties of the Co layer stay intact.	Oct 2022
I11-High Resolution Powder Diffraction	Enhanced long-term cathode stability by tuning interfacial nanocomposite for intermediate temperature solid oxide fuel cells Dingyue Hu , Karl Dawson , Marco Zanella , Troy D. Manning , Luke M. Daniels , Nigel D. Browning , B. Layla Mehdi , Yaobin Xu , Houari Amari , J. Felix Shin , Michael J. Pitcher , Ruiyong Chen , Hongjun Niu , Bowen Liu , Matthew Bilton , Junyoung Kim , John B. Claridge , Matthew J. Rosseinsky Advanced Materials Interfaces 3 DOI: 10.1002/admi.202102131 Diamond Proposal Number(s): [23666] Open Access Show Abstract ▼ Abstract: Performance durability is one of the essential requirements for solid oxide fuel cell materials operating in the intermediate temperature range (500–700 °C). The trade-off between desirable catalytic activity and long-term stability challenges the development and commercialization of electrode materials. Here an oxygen cathode material, Ba0.5Sr0.5(Co0.7Fe0.3)0.69−xMgxW0.31O3−δ (BSCFW-xMg), that exhibits excellent electrocatalytic performance through the addition of an optimized amount of Mg to the self-assembled nanocomposite Ba0.5Sr0.5(Co0.7Fe0.3)0.69W0.31O3−δ (BSCFW) by simple solid-state reaction is reported. Distinct from the bulk and surface approaches to introduce vacancies and defects in materials design, here the Mg2+ ions concentrate at the single perovskite/double perovskite interface of BSCFW with dislocations and Mg2+-rich nanolayers, resulting in stressed and compositionally inhomogeneous interface regions. The interfacial chemistry within these nanocomposites provides an additional degree of freedom to enable performance optimization over single phase materials and promotes the durability of alkaline-earth based fuel cell materials.	Mar 2022
I07-Surface & interface diffraction	Thickness-dependent energy-level alignment at the organic–organic interface induced by templated gap states Jan Hagenlocher , Katharina Broch , Matthias Zwadlo , Daniel Lepple , Jonathan Rawle , Francesco Carla , Satoshi Kera , Frank Schreiber , Alexander Hinderhofer Advanced Materials Interfaces 133 DOI: 10.1002/admi.202101382 Diamond Proposal Number(s): [18570] Open Access Show Abstract ▼ Abstract: Planar organic heterostructures are widely explored and employed in photovoltaic cells, light-emitting diodes, and bilayer field-effect transistors. An important role for device performance plays the energy level alignment at the inorganic–organic and organic–organic interfaces. In this work, incremental ultraviolet photoelectron spectroscopy measurements and real-time X-ray scattering experiments are used to thoroughly investigate the thickness-dependent electronic and structural properties of a perfluoropentacene (PFP)-on-[6]phenacene heterostructure. For both materials an incremental increase of the material work function (positive interface dipole) is found. For [6]phenacene, this can be assigned to a thickness-dependent change of molecular arrangement evident from a change of the unit cell volume and a consequential alteration of the ionization energy. In the case of PFP the interface dipole stems from charge transfer from the substrate into unoccupied molecular orbitals resulting in an electrostatic potential on the surface. The magnitude of this potential can be correlated with an increased gap state density resulting from templated structural defects mediated by the bottom layer.	Dec 2021
I09-Surface and Interface Structural Analysis	A halogen-free and flame-retardant sodium electrolyte compatible with hard carbon anodes Lars Olow Simon Colbin , Ronnie Mogensen , Alexander Buckel , Yong‐lei Wang , Andrew J. Naylor , Jolla Kullgren , Reza Younesi Advanced Materials Interfaces DOI: 10.1002/admi.202101135 Diamond Proposal Number(s): [26551] Open Access Show Abstract ▼ Abstract: For sodium-ion batteries, two pressing issues concerning electrolytes are flammability and compatibility with hard carbon anode materials. Non-flammable electrolytes that are sufficiently stable against hard carbon have—to the authors’ knowledge—previously only been obtained by either the use of high salt concentrations or additives. Herein, the authors present a simple, fluorine-free, and flame-retardant electrolyte which is compatible with hard carbon: 0.38 m sodium bis(oxalato)borate (NaBOB) in triethyl phosphate (TEP). A variety of techniques are employed to characterize the physical properties of the electrolyte, and to evaluate the electrochemical performance in full-cell sodium-ion batteries. The results reveal that the conductivity is sufficient for battery operation, no significant self-discharge occurs, and a satisfactory passivation is enabled by the electrolyte. In fact, a mean discharge capacity of 107 ± 4 mAh g−1 is achieved at the 1005th cycle, using Prussian white cathodes and hard carbon anodes. Hence, the studied electrolyte is a promising candidate for use in sodium-ion batteries.	Oct 2021
I19-Small Molecule Single Crystal Diffraction	Synthesis and enhanced capture properties of a new BioMOF@SWCNT-BP: Recovery of the endangered rare-earth elements from aqueous systems Antonio Tursi , Teresa F. Mastropietro , Rosaria Bruno , Mariafrancesca Baratta , Jesus Ferrando-Soria , Alexander I. Mashin , Fiore P. Nicoletta , Emilio Pardo , Giovanni De Filpo , Donatella Armentano Advanced Materials Interfaces 8 DOI: 10.1002/admi.202100730 Diamond Proposal Number(s): [18768, 22411] Open Access Show Abstract ▼ Abstract: Human society is facing—among other environmental threats—an enormous challenge due to human activities. The extensive use of high-tech devices and electronics equipment in the daily life makes, among others, rare-earth elements (REEs) recovery from secondary sources highly required. Here, a novel bioMOF-based single-walled carbon nanotube buckypaper (SWCNTBP) is presented as a new and efficient composite material (BioMOF@SWCNT-BP). The flexible and highly crystalline metal–organic framework (MOF), prepared from the natural amino acid L-threonine, has been homogeneously dispersed within the tangled net of a self-standing SWCNT-BP for lanthanides recovery from water. This MOF-carbon-based membrane exhibits high efficiency, either in static or dynamic regimes, in the recovery of lanthanides from aqueous streams outperforming the state-of-the-art. The capture performances of BPs are successfully improved after incorporation of such MOF featuring hexagonal functional channels decorated with the threonine amino acid residues, pointing toward the accessible void spaces, which boosts the capture properties of the final membrane, providing the adaptable functional environment to interact with lanthanides. This material's preparation presents also a potential for large-scale applications with a potential benefit on natural aquatic ecosystems as well. It is highly demanded because REEs from non-recycled waste materials are potential pollutants for surface waters.	Aug 2021
B22-Multimode InfraRed imaging And Microspectroscopy	Guest‐tunable dielectric sensing using a single crystal of HKUST‐1 Arun S. Babal , Abhijeet K. Chaudhari , Hamish H.-M. Yeung , Jin-Chong Tan Advanced Materials Interfaces 7 DOI: 10.1002/admi.202000408 Open Access Show Abstract ▼ Abstract: There is rising interest on low‐k dielectric materials based on porous metal–organic frameworks (MOFs) for improved electrical insulation in microelectronics. Herein, the concept of MOF dielectric sensor built from a single crystal of HKUST‐1 is demonstrated. Guest encapsulation effects of polar and non‐polar molecules are studied, by monitoring the transient dielectric response and AC conductivity of the crystal exposed to different vapors (water, iodine, methanol, and ethanol). The dielectric properties are measured along the <100> crystal direction in the frequency range of 100 Hz to 2 MHz. The dielectric data show the efficacy of MOF dielectric sensor for discriminating the guest analytes. The time‐dependent transient response reveals dynamics of the molecular inclusion and exclusion processes in the nanoscale pores. Since dielectric response is ubiquitous to all MOF materials (unlike DC conductivity and fluorescence), the results demonstrate the potential of dielectric MOF sensors compared to resistive sensors and luminescence‐based approaches.	Jul 2020
I09-Surface and Interface Structural Analysis	Understanding the roles of tris(trimethylsilyl) phosphite (TMSPi) in LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811)/silicon–graphite (Si–Gr) lithium‐ion batteries Haidong Liu , Andrew Naylor , Ashok Sreekumar Menon , William R. Brant , Kristina Edström , Reza Younesi Advanced Materials Interfaces 8 DOI: 10.1002/admi.202000277 Diamond Proposal Number(s): [23159] Open Access Show Abstract ▼ Abstract: The coupling of nickel‐rich LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes with high‐capacity silicon–graphite (Si–Gr) anodes is one promising route to further increase the energy density of lithium‐ion batteries. Practically, however, the cycle life of such cells is seriously hindered due to continuous electrolyte degradation on the surfaces of both electrodes. In this study, tris(trimethylsilyl) phosphite (TMSPi) is introduced as an electrolyte additive to improve the electrochemical performance of the NMC811/Si–Gr full cells through formation of protective surface layers at the electrode/electrolyte interfaces. This is thought to prevent the surface fluorination of the active materials and enhance interfacial stability. Notably, TMSPi is shown to significantly reduce the overpotential and operando X‐ray diffraction (XRD) confirms that an irreversible “two‐phase” transition reaction caused by the formed adventitious Li2CO3 layer on the surface of NMC811 can transfer to a solid‐solution reaction mechanism with TMSPi‐added electrolyte. Moreover, influences of TMSPi on the cathode electrolyte interphase (CEI) on the NMC811 and solid electrolyte interphase (SEI) on the Si–Gr are systematically investigated by electron microscopy and synchrotron‐based X‐ray photoelectron spectroscopy which allows for the nondestructive depth‐profiling analysis of chemical compositions and oxidation states close to the electrode surfaces.	Jun 2020
B18-Core EXAFS	Revealing strain effects on the chemical composition of perovskite oxide thin films surface, bulk, and interfaces Celeste A. M. Van Den Bosch , Andrea Cavallaro , Roberto Moreno , Giannantonio Cibin , Gwilherm Kerherve , José M. Caicedo , Thomas K. Lippert , Max Doebeli , José Santiso , Stephen J. Skinner , Ainara Aguadero Advanced Materials Interfaces 247 DOI: 10.1002/admi.201901440 Diamond Proposal Number(s): [13530, 16839] Show Abstract ▼ Abstract: Understanding the effects of lattice strain on oxygen surface and diffusion kinetics in oxides is a controversial subject that is critical for developing efficient energy storage and conversion materials. In this work, high‐quality epitaxial thin films of the model perovskite La0.5Sr0.5Mn0.5Co0.5O3−δ (LSMC), under compressive or tensile strain, are characterized with a combination of in situ and ex situ bulk and surface‐sensitive techniques. The results demonstrate a nonlinear correlation of mechanical and chemical properties as a function of the operation conditions. It is observed that the effect of strain on reducibility is dependent on the “effective strain” induced on the chemical bonds. In‐plain strain, and in particular the relative BO length bond, is the key factor controlling which of the B‐site cation can be reduced preferentially. Furthermore, the need to use a set of complimentary techniques to isolate different chemically induced strain effects is proven. With this, it is confirmed that tensile strain favors the stabilization of a more reduced lattice, accompanied by greater segregation of strontium secondary phases and a decrease of oxygen exchange kinetics on LSMC thin films.	Dec 2019
I13-2-Diamond Manchester Imaging	Thermoresponsive wrinkles on hydrogels for soft actuators Yasuaki Tokudome , Hiroki Kuniwaki , Kazumasa Suzuki , Davide Carboni , Gowsihan Poologasundarampillai , Masahide Takahashi Advanced Materials Interfaces 3 DOI: 10.1002/admi.201500802 Diamond Proposal Number(s): [11225] Open Access Show Abstract ▼ Abstract: Adaptive surface wrinkles are demonstrated to exhibit a peristaltic motion and a size-selective transportation of micro-objects under thermal stimulus. The bilayered materials made of thermoresponsive poly(N-iso-propylacrylamide) and hybrid silica form responsive wrinkles of submillimeter dimensions with temperature variation. This hydrogel-based actuation works in a near-physiological environment, which meets the critical requirement for artificial alternatives in bioapplications.	Jun 2016

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