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  • 1.
    Abdelhamid, Hani Nasser
    et al.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). Assiut University, Egypt.
    El-Zohry, Ahmed M.
    Cong, Jiayan
    Thersleff, Thomas
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Karlsson, Martin
    Kloo, Lars
    Zou, Xiaodong
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Towards implementing hierarchical porous zeolitic imidazolate frameworks in dye-sensitized solar cells2019In: Royal Society Open Science, E-ISSN 2054-5703, Vol. 6, no 7, article id 190723Article in journal (Refereed)
    Abstract [en]

    A one-pot method for encapsulation of dye, which can be applied for dye-sensitized solar cells (DSSCs), and synthesis of hierarchical porous zeolitic imidazolate frameworks (ZIF-8), is reported. The size of the encapsulated dye tunes the mesoporosity and surface area of ZIF-8. The mesopore size, Langmuir surface area and pore volume are 15 nm, 960-1500 m(2). g(-1) and 0.36-0.61 cm(3). g(-1), respectively. After encapsulation into ZIF-8, the dyes show longer emission lifetimes (greater than 4-8-fold) as compared to the corresponding non-encapsulated dyes, due to suppression of aggregation, and torsional motions.

  • 2. Ertl, Michael
    et al.
    Ma, Zili
    Thersleff, Thomas
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Lyu, Pengbo
    Huettner, Sven
    Nachtigall, Petr
    Breu, Josef
    Slabon, Adam
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Mössbauerite as Iron-Only Layered Oxyhydroxide Catalyst for WO3 Photoanodes2019In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 58, no 15, p. 9655-9662Article in journal (Refereed)
    Abstract [en]

    Mössbauerite, a trivalent iron-only layered oxyhydroxide, has been recently identified as an electrocatalyst for water oxidation. We investigated the material as potential cocatalyst for photoelectrochemical water oxidation on semiconductor photoanodes. The band edge positions of mössbauerite were determined for the first time with a combination of Mott-Schottky analysis and UV-vis diffuse reflectance spectroscopy. The positive value of the Mott-Schottky slope and the flatband potential of 0.34 V vs reversible hydrogen electrode (RHE) identifies the material as an n-type semiconductor, but bare mössbauerite does not produce noticeable photocurrent during water oxidation. Type-II heterojunction formation by facile drop-casting with WO3 thin films yielded photoanodes with amended charge carrier separation and photocurrents up to 1.22 mA cm(-2) at 1.23 V vs RHE. Mössbauerite is capable of increasing the charge carrier separation at lower potential and improving the photocurrent during photoelectrochemical water oxidation. The rise in photocurrent of the mössbauerite-functionalized WO3 photoanode thus originates from improved charge carrier separation and augmented hole collection efficiency. Our results highlight the potential of mössbauerite as a second-phase catalyst for semiconductor electrodes.

  • 3.
    Li, Yunxiang
    et al.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Wang, Xia
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Thersleff, Thomas
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Svensson, Gunnar
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Hedin, Niklas
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Silicoaluminophosphate (SAPO)-Templated Activated Carbons2019In: Acs Omega, ISSN 2470-1343, Vol. 4, no 6, p. 9889-9895Article in journal (Refereed)
    Abstract [en]

    Microporous activated carbon was prepared by depositing and pyrolyzing propylene within the microporous voids of SAPO-37 and subsequently removing the template by a treatment with HCl and NaOH. The carbon had a high surface area and large micropore and ultramicropore volumes. The yield, crystallinity, morphology, and adsorption properties compared well with those of a structurally related zeolite-Y-templated carbon. No HF was needed to remove the SAPO-37 template in contrast to the zeolite Y template, which could be of industrial importance.

  • 4. Ma, Zili
    et al.
    Thersleff, Thomas
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Görne, Arno L.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). Aachen University, Germany.
    Cordes, Niklas
    Liu, Yanbing
    Jakobi, Simon
    Rokicinska, Anna
    Schichtl, Zebulon G.
    Coridan, Robert H.
    Kustrowski, Piotr
    Schnick, Wolfgang
    Dronskowski, Richard
    Slabon, Adam
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Quaternary Core-Shell Oxynitride Nanowire Photoanode Containing a Hole-Extraction Gradient for Photoelectrochemical Water Oxidation2019In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 11, no 21, p. 19077-19086Article in journal (Refereed)
    Abstract [en]

    A nanowire photoanode SrTaO2N, a semiconductor suitable for overall water-splitting with a band gap of 2.3 eV, was coated with functional overlayers to yield a core-shell structure while maintaining its one-dimensional morphology. The nanowires were grown hydrothermally on tantalum, and the perovskite-related oxynitride structure was obtained by nitridation. Three functional overlayers have been deposited on the nanowires to enhance the efficiency of photoelectrochemical (PEC) water oxidation. The deposition of TiOx protects the oxynitride from photocorrosion and suppresses charge-carrier recombination at the surface. Ni(OH)(x) acts a hole-storage layer and decreases the dark-current contribution. This leads to a significantly improved extraction of photogenerated holes to the electrode-electrolyte surface. The photocurrents can be increased by the deposition of a cobalt phosphate (CoPi) layer as a cocatalyst. The heterojunction nanowire photoanode generates a current density of 0.27 mA cm(-2) at 1.23 V vs the reversible hydrogen electrode (RHE) under simulated sunlight (AM 1.5G). Simultaneously, the dark-current contribution, a common problem for oxynitride photoanodes grown on metallic substrates, is almost completely minimized. This is the first report of a quaternary oxynitride nanowire photoanode in core-shell geometry containing functional overlayers for synergetic hole extraction and an electrocatalyst.

  • 5. Negi, Devendra
    et al.
    Spiegelberg, Jakob
    Muto, Shunsuke
    Thersleff, Thomas
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Ohtsuka, Masahiro
    Schönström, Linus
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Tatsumi, Kazuyoshi
    Rusz, Ján
    Proposal for Measuring Magnetism with Patterned Apertures in a Transmission Electron Microscope2019In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 122, no 3, article id 037201Article in journal (Refereed)
    Abstract [en]

    We propose a magnetic measurement method utilizing a patterned post-sample aperture in a transmission electron microscope. While utilizing electron magnetic circular dichroism, the method circumvents previous needs to shape the electron probe to an electron vortex beam or astigmatic beam. The method can be implemented in standard scanning transmission electron microscopes by replacing the spectrometer entrance aperture with a specially shaped aperture, hereafter called ventilator aperture. The proposed setup is expected to work across the whole range of beam sizes -- from wide parallel beams down to atomic resolution magnetic spectrum imaging.

  • 6. Rusz, Ján
    et al.
    Spiegelberg, Jakob
    Muto, Shunsuke
    Thersleff, Thomas
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Ohtsuka, Masahiro
    Leifer, Klaus
    Oppeneer, Peter M.
    Localization of magnetic circular dichroic spectra in transmission electron microscopy experiments with atomic plane resolution2017In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 95, no 17, article id 174412Article in journal (Refereed)
    Abstract [en]

    Inelastic electron scattering is a consequence of mostly Coulomb interaction between electrons in the sample and electron beam and, as such, it is a nonlocal event. In atomic resolution experiments, it thus opens the following question: How far is the origin of the inelastic scattering signal that is observed when the electron beam is passing nearby an atomic column or plane? We analyze computationally the delocalization of the magnetic signal in electron magnetic circular dichroism (EMCD) experiments in the so-called three-beam orientation, allowing one to image individual atomic planes. We compare the classical EMCD setup using the double-difference procedure (DD-EMCD) to a recently introduced atomic plane resolution EMCD (APR-EMCD) geometry, assuming the same probe size. We observe a strong localization of the EMCD signal to the closest atomic plane, confirming the potential of EMCD to study an evolution of magnetic properties near surfaces or interfaces with atomic plane resolution. The localization of the EMCD signal is remarkably higher than the localization of the nonmagnetic component of the inelastic scattering cross section. We also analyze double-channeling effects and find them particularly strong for the DD-EMCD method, while for APR-EMCD they appear to be minor. The DD-EMCD signal, on the other hand, appears to be more robust with respect to sample thickness than that of the APR-EMCD.

  • 7.
    Thersleff, Thomas
    et al.
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Schönström, Linus
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK). Uppsala University, Sweden.
    Tai, Cheuk-Wai
    Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
    Adam, Roman
    Bürgler, Daniel E.
    Schneider, Claus M.
    Muto, Shunsuke
    Rusz, Ján
    Single-pass STEM-EMCD on a zone axis using a patterned aperture: progress in experimental and data treatment methods2019In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 9, article id 18170Article in journal (Refereed)
    Abstract [en]

    Measuring magnetic moments in ferromagnetic materials at atomic resolution is theoretically possible using the electron magnetic circular dichroism (EMCD) technique in a (scanning) transmission electron microscope ((S)TEM). However, experimental and data processing hurdles currently hamper the realization of this goal. Experimentally, the sample must be tilted to a zone-axis orientation, yielding a complex distribution of magnetic scattering intensity, and the same sample region must be scanned multiple times with sub-atomic spatial registration necessary at each pass. Furthermore, the weak nature of the EMCD signal requires advanced data processing techniques to reliably detect and quantify the result. In this manuscript, we detail our experimental and data processing progress towards achieving single-pass zone-axis EMCD using a patterned aperture. First, we provide a comprehensive data acquisition and analysis strategy for this and other EMCD experiments that should scale down to atomic resolution experiments. Second, we demonstrate that, at low spatial resolution, promising EMCD candidate signals can be extracted, and that these are sensitive to both crystallographic orientation and momentum transfer.

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