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100 result(s) for "Lerch, Martin"
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Ionomer distribution control in porous carbon-supported catalyst layers for high-power and low Pt-loaded proton exchange membrane fuel cells
The reduction of Pt content in the cathode for proton exchange membrane fuel cells is highly desirable to lower their costs. However, lowering the Pt loading of the cathodic electrode leads to high voltage losses. These voltage losses are known to originate from the mass transport resistance of O 2 through the platinum–ionomer interface, the location of the Pt particle with respect to the carbon support and the supports’ structures. In this study, we present a new Pt catalyst/support design that substantially reduces local oxygen-related mass transport resistance. The use of chemically modified carbon supports with tailored porosity enabled controlled deposition of Pt nanoparticles on the outer and inner surface of the support particles. This resulted in an unprecedented uniform coverage of the ionomer over the high surface-area carbon supports, especially under dry operating conditions. Consequently, the present catalyst design exhibits previously unachieved fuel cell power densities in addition to high stability under voltage cycling. Thanks to the Coulombic interaction between the ionomer and N groups on the carbon support, homogeneous ionomer distribution and reproducibility during ink manufacturing process is ensured. Reducing Pt content in cathodes for proton exchange membrane fuel cells is crucial to lower costs but results in high voltage losses. A Pt catalyst/support design that substantially reduces local oxygen-related mass transport resistance is reported.
Perovskite BaTaO2N: From Materials Synthesis to Solar Water Splitting
Barium tantalum oxynitride (BaTaO2N), as a member of an emerging class of perovskite oxynitrides, is regarded as a promising inorganic material for solar water splitting because of its small band gap, visible light absorption, and suitable band edge potentials for overall water splitting in the absence of an external bias. However, BaTaO2N still exhibits poor water‐splitting performance that is susceptible to its synthetic history, surface states, recombination process, and instability. This review provides a comprehensive summary of previous progress, current advances, existing challenges, and future perspectives of BaTaO2N for solar water splitting. A particular emphasis is given to highlighting the principles of photoelectrochemical (PEC) water splitting, classic and emerging photocatalysts for oxygen evolution reactions, and the crystal and electronic structures, dielectric, ferroelectric, and piezoelectric properties, synthesis routes, and thin‐film fabrication of BaTaO2N. Various strategies to achieve enhanced water‐splitting performance of BaTaO2N, such as reducing the surface and bulk defect density, engineering the crystal facets, tailoring the particle morphology, size, and porosity, cation doping, creating the solid solutions, forming the heterostructures and heterojunctions, designing the photoelectrochemical cells, and loading suitable cocatalysts are discussed. Also, the avenues for further investigation and the prospects of using BaTaO2N in solar water splitting are presented. This review provides a comprehensive summary of previous progress, current advances, existing challenges, and future perspectives of BaTaO2N for solar water splitting. For enhancing the water‐splitting performance of BaTaO2N, various strategies, such as reducing the defect density, engineering the crystal facets, cation doping, forming the heterostructures/heterojunctions, designing the photoelectrochemical cells, and loading suitable cocatalysts are presented.
Better than Rician: modelling millimetre wave channels as two-wave with diffuse power
This contribution provides experimental evidence for the two-wave with diffuse power (TWDP) fading model. We have conducted two indoor millimetre wave measurement campaigns with directive horn antennas at both link ends. One horn antenna is mounted in a corner of our laboratory, while the other is steerable and scans azimuth and elevation. Our first measurement campaign is based on scalar network analysis with 7 GHz of bandwidth. Our second measurement campaign obtains magnitude and phase information; it is additionally sampled directionally at several positions in space. We apply Akaike’s information criterion to decide whether Rician fading sufficiently explains the data or the generalised TWDP fading model is necessary. Our results indicate that the TWDP fading hypothesis is favoured over Rician fading in situations where the steerable antenna is pointing towards reflecting objects or is slightly misaligned at line-of-sight. We demonstrate TWDP fading in several different domains, namely, frequency, space, and time.
Mechanochemical solid state synthesis of copper(I)/NHC complexes with K3PO4
A protocol for the mechanochemical synthesis of copper(I)/N-heterocyclic carbene complexes using cheap and readily available K3PO4 as base has been developed. This method employing a ball mill is amenable to typical simple copper(I)/NHC complexes but also to a sophisticated copper(I)/N-heterocyclic carbene complex bearing a guanidine moiety. In this way. the present approach circumvents commonly employed silver(I) complexes which are associated with significant and undesired waste formation and the excessive use of solvents. The resulting bifunctional catalyst has been shown to be active in a variety of reduction/hydrogenation transformations employing dihydrogen as terminal reducing agent.
Anharmonic Effects in Ordered Kesterite-Type Cu2ZnSnS4
We performed an in-depth investigation and analysis of the effect of temperature on the Raman-active A-modes of bulk kesterite-type Cu2ZnSnS4 within the 300–460 K temperature range. We acquired the individual contributions to each Raman mode, namely, the thermal expansion and anharmonic interactions terms responsible for the Raman shift and broadening with temperature. Our results indicate that the Raman shift with temperature is dominated by the thermal expansion term, whereas the broadening is mainly governed by three-phonon damping processes in this material. Considering relevant results from the literature, it appears that dimensionality is a key factor in regulating the dominant phonon decay mechanism.
Mayenite-Based Electride C12A7e−: A Reactivity and Stability Study
Ru supported on mayenite electride, [Ca24Al28O64]4+(e−)4 a calcium aluminum oxide denoted as C12A7e−, are described in the literature as highly active catalysts for ammonia synthesis, especially under conditions of low absolute pressure. In this study, we investigated the application of recently reported plasma arc melting synthesized C12A7e− (aluminum solid reductant) as supports of Ru/C12A7e− catalysts in ammonia synthesis up to pressures of 7.6 MPa. Together with the plasma-arc-melting-based catalyst support, we investigated a similar plasma-synthesized C12A7e− (graphite solid reductant) and a vacuum-sintering-based C12A7e−. Complementary to the catalytic tests, we applied 2H solid-state NMR spectroscopy, DRUVVis-spectroscopy, thermal analysis and PXRD to study and characterize the reactivity of different plasma-synthesized and vacuum-sintered C12A7e− towards H2/D2 and H2O. The catalysts showed an immediate deactivation at pressures > 1 MPa, which can be explained by irreversible hydride formation at higher pressures, as revealed by reactivity tests of C12A7e− towards H2/D2. The direct formation of C12A7:D from C12A7e− is proven. It can be concluded that the application of Ru/C12A7e− catalysts at the industrial scale has limited prospects due to irreversible hydride formation at relevant pressures > 1 MPa. Furthermore, we report an in-depth study relating to structural changes in the material in the presence of H2O.
Commensurate Nb2Zr5O15: Accessible Within the Field Nb2ZrxO2x+5 After All
Doped niobium zirconium oxides are applied in field‐effect transistors and as special‐purpose coatings. Whereas their material properties are sufficiently known, their crystal structures remain widely uncharacterized. Herein, we report on the comparably mild sol‐gel synthesis of Nb2Zr5O15 and the elucidation of its commensurately modulated structure via neutron diffraction. We describe the structure using the most appropriate superspace as well as the convenient supercell approach. It is part of an α‐PbO2‐homeotypic field with the formula Nb2ZrxO2x+5, which has previously been reported only for x≥5.1, and is closely related to the structure of Hf3Ta2O11. The results, supported by X‐ray diffraction and additional synthesis experiments, are contextualized within the existing literature. Via the sol‐gel route, metastable Nb−Zr−O compounds and their heavier congeners are accessible that shed light on possible structures of these commercially utilized materials. Teaching an old dog neu‐trons: The commensurately modulated Nb2Zr5O15 is not, as previously supposed, inaccessible. Synthesis is possible via a sol‐gel route under relatively mild conditions. X‐ray diffraction may be unable to elucidate its rather complex structure, but neutron diffraction sure can – with a little help from an initial model.
Perovskite BaTaO 2 N: From Materials Synthesis to Solar Water Splitting
Barium tantalum oxynitride (BaTaO 2 N), as a member of an emerging class of perovskite oxynitrides, is regarded as a promising inorganic material for solar water splitting because of its small band gap, visible light absorption, and suitable band edge potentials for overall water splitting in the absence of an external bias. However, BaTaO 2 N still exhibits poor water‐splitting performance that is susceptible to its synthetic history, surface states, recombination process, and instability. This review provides a comprehensive summary of previous progress, current advances, existing challenges, and future perspectives of BaTaO 2 N for solar water splitting. A particular emphasis is given to highlighting the principles of photoelectrochemical (PEC) water splitting, classic and emerging photocatalysts for oxygen evolution reactions, and the crystal and electronic structures, dielectric, ferroelectric, and piezoelectric properties, synthesis routes, and thin‐film fabrication of BaTaO 2 N. Various strategies to achieve enhanced water‐splitting performance of BaTaO 2 N, such as reducing the surface and bulk defect density, engineering the crystal facets, tailoring the particle morphology, size, and porosity, cation doping, creating the solid solutions, forming the heterostructures and heterojunctions, designing the photoelectrochemical cells, and loading suitable cocatalysts are discussed. Also, the avenues for further investigation and the prospects of using BaTaO 2 N in solar water splitting are presented.
Perovskite BaTaO2 N: From Materials Synthesis to Solar Water Splitting
Barium tantalum oxynitride (BaTaO2 N), as a member of an emerging class of perovskite oxynitrides, is regarded as a promising inorganic material for solar water splitting because of its small band gap, visible light absorption, and suitable band edge potentials for overall water splitting in the absence of an external bias. However, BaTaO2 N still exhibits poor water-splitting performance that is susceptible to its synthetic history, surface states, recombination process, and instability. This review provides a comprehensive summary of previous progress, current advances, existing challenges, and future perspectives of BaTaO2 N for solar water splitting. A particular emphasis is given to highlighting the principles of photoelectrochemical (PEC) water splitting, classic and emerging photocatalysts for oxygen evolution reactions, and the crystal and electronic structures, dielectric, ferroelectric, and piezoelectric properties, synthesis routes, and thin-film fabrication of BaTaO2 N. Various strategies to achieve enhanced water-splitting performance of BaTaO2 N, such as reducing the surface and bulk defect density, engineering the crystal facets, tailoring the particle morphology, size, and porosity, cation doping, creating the solid solutions, forming the heterostructures and heterojunctions, designing the photoelectrochemical cells, and loading suitable cocatalysts are discussed. Also, the avenues for further investigation and the prospects of using BaTaO2 N in solar water splitting are presented.Barium tantalum oxynitride (BaTaO2 N), as a member of an emerging class of perovskite oxynitrides, is regarded as a promising inorganic material for solar water splitting because of its small band gap, visible light absorption, and suitable band edge potentials for overall water splitting in the absence of an external bias. However, BaTaO2 N still exhibits poor water-splitting performance that is susceptible to its synthetic history, surface states, recombination process, and instability. This review provides a comprehensive summary of previous progress, current advances, existing challenges, and future perspectives of BaTaO2 N for solar water splitting. A particular emphasis is given to highlighting the principles of photoelectrochemical (PEC) water splitting, classic and emerging photocatalysts for oxygen evolution reactions, and the crystal and electronic structures, dielectric, ferroelectric, and piezoelectric properties, synthesis routes, and thin-film fabrication of BaTaO2 N. Various strategies to achieve enhanced water-splitting performance of BaTaO2 N, such as reducing the surface and bulk defect density, engineering the crystal facets, tailoring the particle morphology, size, and porosity, cation doping, creating the solid solutions, forming the heterostructures and heterojunctions, designing the photoelectrochemical cells, and loading suitable cocatalysts are discussed. Also, the avenues for further investigation and the prospects of using BaTaO2 N in solar water splitting are presented.
Structure and properties of molybdenum oxide nitrides as model systems for selective oxidation catalysts
Molybdenum oxide nitride (denoted as Mo(O,N)3) was obtained by ammonolysis of α-MoO3 with gaseous ammonia. Electronic and geometric structure, reducibility, and conductivity of Mo(O,N)3 were investigated by XRD, XAS, UV-Vis spectroscopy, and impedance measurements. Catalytic performance in selective propene oxidation was determined by online mass spectrometry und gas chromatography. Upon incorporation of nitrogen, Mo(O,N)3 maintained the characteristic layer structure of α-MoO3. XRD analysis showed an increased structural disorder in the layers while nitrogen is removed from the lattice of Mo(O,N)3 at temperatures above ~600 K. Compared to regular α-MoO3, Mo(O,N)3 exhibited a higher electronic and ionic conductivity and an onset of reduction in propene at lower temperatures. Surprisingly, α-MoO3 and Mo(O,N)3 exhibited no detectable differences in onset temperatures of propene oxidation and catalytic selectivity or activity. Apparently, the increased reducibility, oxygen mobility, and conductivity of Mo(O,N)3 compared to α-MoO3 had no effect on the catalytic behavior of the two catalysts. The results presented confirm the suitability of molybdenum oxide nitrides as model systems for studying bulk contributions to selective oxidation.