Purpose: This study examined the contribution of voice to the self via implicit associations.
Method: An implicit association test (IAT) of the voice and the self was created and presented to vocal performers and community controls. One-hundred eleven participants completed this voice-self IAT, the Vocal Congruence Scale (VCS), and the Voice Handicap Index (VHI) via an in-person, monitored, and timed Qualtrics survey.
Earth-abundant transition metal oxides are promising alternatives to precious metal oxides as electrocatalysts for the oxygen evolution reaction (OER) and are intensively investigated for alkaline water electrolysis. OER electrocatalysis, like most other catalytic reactions, is surface-initiated, and the catalyst performance is fundamentally determined by the surface properties. Most transition metal oxide catalysts show OER activities that depend on the predominantly exposed crystal facets/surface structure.
View Article and Find Full Text PDFAssessing novel electrocatalysts for the electrochemical ammonia synthesis (EAS) requires reliable quantitative trace analysis of electrochemically produced ammonia to infer activity and selectivity. This study concerns the development of an ion chromatography (IC) method for quantitative trace analysis of ammonium in 0.1 M sulfuric acid electrolyte, which is applied to EAS gas-diffusion electrode (GDE) experiments with commercial chromium nitride as electrocatalyst.
View Article and Find Full Text PDFWe have discovered the first polythioplatinate(II), [PtS(SO)] (), which was synthesized in aqueous basic medium (pH 11) by hydrothermal heating at 150 °C. Polyanion comprises a discrete, triangular assembly of three Pt ions linked by two μ-sulfido ligands, and their square-planar coordination geometry is completed by two terminal S-bound sulfito ligands. Polyanion was isolated as a hydrated sodium salt, Na[Pt(μ-S)(SO)]·22HO (), which was characterized in the solid state by single-crystal X-ray diffraction, Fourier-transform infrared spectroscopy, thermogravimetric analysis, X-ray photoelectron spectra, and elemental analysis, in solution by Pt NMR and atomic absorption spectroscopy, and in the gas phase by electrospray ionization mass spectrometry.
View Article and Find Full Text PDFThe first organofunctionalized mixed-valent polyoxo-30-molybdate wheel, [MoMoO{AsO(CH)}] (), was synthesized in aqueous, mildly acidic conditions, and upon further acidification, the neutral tetramolybdenum(V) oxo cluster [MoO{AsO(CH)}] () was obtained. Single-crystal X-ray diffraction (XRD) revealed that comprises 18 Mo and 12 Mo ions arranged in a cyclic fashion with alternating {Mo} and {Mo} groups, which are capped by 18 dimethylarsinate ligands, resulting in a novel polyoxo-30-molybdate wheel with a central cavity of ∼1.5 nm.
View Article and Find Full Text PDFThe discrete inverted-Keggin ion [MoO(OH)(4-NCH-CHAsO)] () has been prepared in an aqueous acidic (pH 0.8) medium by the reaction of MoO with the (4-triazolylphenyl)arsonic acid 4-NCH-CHAsOH under hydrothermal conditions and was isolated as a sodium salt in 21% yield. The exact same reaction in the presence of Cu ions resulted in the neutral metal-organic framework (MOF) Cu[MoO(4-NCH-CHAsO)] () in 68% yield.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2022
Metal oxide libraries for photoanodes for the oxygen evolution reaction (OER) were generated by printing a metal salt solution in an array layout, followed by calcination to yield 22 ternary metal oxide systems. The libraries included a ternary metal cation system based on CuWO with one out of eight transition or posttransition metal ions Cr, Mn, Fe, Co, Ni, Zn, Bi, and Ga in different overall atomic ratios. The photocatalyst libraries were screened by scanning photoelectrochemical microscopy for the highest anodic photocurrents.
View Article and Find Full Text PDFWe report on the synthesis and structural characterization of a giant, discrete, and neutral molecular disk, [PdO(OH){(CH)AsO}] (), comprising a 40-palladium-oxo core that is capped by 16 dimethylarsinate moieties, resulting in a palladium-oxo cluster (POC) with a diameter of ∼2 nm. , which is the largest known neutral Pd-based oxo cluster, can be isolated either as a discrete species or constituting a 3D H-bonded organic-inorganic framework (HOIF) with a 12-tungstate Keggin ion, [SiWO] or [GeWO]. H and C NMR as well as H-DOSY NMR studies indicate that is stable in aqueous solution, which is also confirmed by ESI-MS studies.
View Article and Find Full Text PDFFe-N-C materials are promising non-precious metal catalysts for the oxygen reduction reaction in fuel cells and batteries. However, during the synthesis of these materials less active Fe-containing nanoparticles are formed in many cases which lead to a decrease in electrochemical activity and stability. In this study, we reveal the significant properties of the carbon support required for the successful incorporation of Fe-N-related active sites.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2021
We report on the synthesis, structure, and physicochemical characterization of the first three examples of neutral palladium-oxo clusters (POCs). The 16-palladium(II)-oxo cluster [Pd O (OH) ((CH ) As) ] (Pd ) comprises a cyclic palladium-oxo unit capped by eight dimethylarsinate groups. The chloro-derivative [Pd Na O (OH) Cl ((CH ) As) ] (Pd Cl) was also prepared, which forms a highly stable 3D supramolecular lattice via strong intermolecular interactions.
View Article and Find Full Text PDFWe report on the synthesis and characterization of the first polyoxo-noble-metalate-containing metal-organic framework (MOF) material, wherein the preformed MIL-101 has been impregnated with the discrete, cuboid-shaped polyoxopalladate [PdSeO] (PdSe), leading to the composite PdSe@MIL-101. This material was characterized by FTIR, TGA, elemental analysis, powder-XRD, N sorption (BET), SEM-EDX, and XPS. Furthermore, the PdSe@MIL-101 composite was shown to be an effective, stable, and recyclable heterogeneous precatalyst for the Suzuki-Miyaura cross-coupling reaction at room temperature utilizing environmentally benign solvents, such as water and methanol.
View Article and Find Full Text PDFNickel-based nanostructured materials have gained widespread attention, particularly for energy-related applications. Employing chemical vapor deposition (CVD) for NiO necessitates suitable nickel precursors that are volatile and stable. Herein, we report the synthesis and characterization of a series of new nickel β-ketoiminato complexes with different aliphatic and etheric side chain substitutions, namely, bis(4-(isopropylamino)-pent-3-en-2-onato)nickel(II) ([Ni(ipki)], ), bis(4-(2-methoxyethylamino)pent-3-en-2-onato)nickel(II) ([Ni(meki)], ), bis(4-(2-ethoxyethylamino)pent-3-en-2-onato)nickel(II) ([Ni(eeki)], ), bis(4-(3-methoxy-propylamino)-pent-3-en-2-onato)nickel(II) ([Ni(mpki)], ), and bis(4-(3-ethoxypropylamino)pent-3-en-2-onato)nickel(II) ([Ni(epki)], ).
View Article and Find Full Text PDFHerein, we report a semiconductive, proton-conductive, microporous hydrogen-bonded organic framework (HOF) derived from phenylphosphonic acid and 5,10,15,20-tetrakis[p-phenylphosphonic acid] porphyrin (GTUB5). The structure of GTUB5 was characterized using single crystal X-ray diffraction. A narrow band gap of 1.
View Article and Find Full Text PDFPhys Chem Chem Phys
May 2020
Correction for 'Micro-spectroscopy of HKUST-1 metal-organic framework crystals loaded with tetracyanoquinodimethane: effects of water on host-guest chemistry and electrical conductivity' by Miguel Rivera-Torrente et al., Phys. Chem.
View Article and Find Full Text PDFPhys Chem Chem Phys
November 2019
Composite materials, consisting of a metal-organic framework (MOF) and a guest molecule, further denoted as guest@MOF composites, have gained strong interest due to the guest-induced tunability of the host properties, for example in sensing or electroconductivity applications. However, decoding the complexity of these guest@MOF composites and extracting structure-performance relationships are far from trivial and require the use of a gamut of characterization tools. In this work, we use various micro-spectroscopic tools both under static (ex situ) and dynamic (in situ) conditions to map the properties and diffusion behavior of TCNQ (7,7,8,8-tetracyanoquinodimethane) as a guest molecule in single HKUST-1 crystals as the host.
View Article and Find Full Text PDF"Chemical activation" using Brønsted acids as chemical agents is widely used to generate activated carbons for various sorption applications. Commercially relevant is especially a process using phosphoric acid as activating agent applied to abundant and inexpensive biomass such as wood or coconut shells. In this manuscript, we revisit the porogenesis mechanism based on experiments involving molecular model compounds and oxygen-free polymer precursors, as well as different molten acids as activating agents.
View Article and Find Full Text PDFWhat possible futures can be opened up by creatively reading an encyclopedic text not as a repository for information and historical facts but along two other lines instead: as an archive of concepts and of generative narrative detritus? This essay will reencounter Joseph Needham's Science and Civilisation in China (SCC) according to these two readings. Reading collaboratively, the authors proceed through the early, more general volumes of SCC. McKenzie Wark works with the main text, in connection with Needham's earlier writings, to explore conceptual tools he offered for understanding and living in our current moment.
View Article and Find Full Text PDFHere we report on the synthesis, structure, and characterization of the first example of a polyoxopalladate (POP)-based metal-organic framework (MOF). This novel class of materials comprises discrete polyoxo-13-palladate(II) nanocubes [PdO(AsO)H] decorated by four Ba ions on each of two opposite faces. These secondary building units (SBUs) are linked to each other via rigid linear organic groups, resulting in a stable 3D POP-MOF framework, which exhibits interesting sorption as well as catalytic properties.
View Article and Find Full Text PDFA series of six cobalt ketoiminates, of which one was previously reported but not explored as a chemical vapor deposition (CVD) precursor, namely, bis(4-(isopropylamino)pent-3-en-2-onato)cobalt(II) ([Co( pki)], 1), bis(4-(2-methoxyethylamino)pent-3-en-2-onato)cobalt(II) ([Co(meki)], 2), bis(4-(2-ethoxyethylamino)pent-3-en-2-onato)cobalt(II) ([Co(eeki)], 3), bis(4-(3-methoxy-propylamino)pent-3-en-2-onato)cobalt(II) ([Co(mpki)], 4), bis(4-(3-ethoxypropylamino)pent-3-en-2-onato)cobalt(II) ([Co(epki)], 5), and bis(4-(3-isopropoxypropylamino)pent-3-en-2-onato)cobalt(II) ([Co( ppki)], 6) were synthesized and thoroughly characterized. Single-crystal X-ray diffraction (XRD) studies on compounds 1-3 revealed a monomeric structure with distorted tetrahedral coordination geometry. Owing to the promising thermal properties, metalorganic CVD of CoO was performed using compound 1 as a representative example.
View Article and Find Full Text PDFThe low-temperature fabrication of flexible ZnO photo-anodes for dye-sensitized solar cells (DSSCs) by templated electrochemical deposition of films was performed in an enlarged and technical simplified deposition setup to demonstrate the feasibility of the scale-up of the deposition process. After extraction of eosin Y (EY) from the initially deposited ZnO/EY hybrid films, mesoporous ZnO films with an area of about 40 cm² were reproducibly obtained on fluorine doped tin oxide (FTO)-glass as well as flexible indium tin oxide (ITO)-polyethylenterephthalate (PET) substrates. With a film thickness of up to 9 µm and a high specific surface area of up to about 77 m²·cm the ZnO films on the flexible substrates show suitable properties for DSSCs.
View Article and Find Full Text PDFEnviron Sci Pollut Res Int
December 2018
Advanced oxidation processes using semiconducting photocatalysts for the degradation of organic pollutants are a promising approach for the remediation of pesticide-contaminated wastewater. High photodegradation efficiency and stability of the photocatalyst are of key importance for practical application of the semiconductor. In this study, mesoporous TiO/ZrO nanopowders were synthesized via two techniques; evaporation-induced self-assembly (EISA) and sol-gel using triblock copolymers Pluronic P123 and F127.
View Article and Find Full Text PDFThe new porphyrin-based tetraphosphonic acid (Ni-HTPPP) was employed in the synthesis of four isostructural MOFs of composition [M(Ni-HTPPP)(HO)], denoted CAU-29 (M = Mn, Co, Ni, Cd). Ni-CAU-29 was thoroughly characterized regarding its thermal and chemical stability as well as for proton conductivity.
View Article and Find Full Text PDFA new aluminium metal-organic framework (MOF), based on the short aliphatic linker molecule mesaconic acid (H Mes; methylfumaric acid) is reported. Al-MIL-68-Mes with composition [Al(OH)(O C-C H -CO )]⋅n H O is obtained after short reaction times of 45 minutes under mild, aqueous synthesis conditions (95 °C). It exhibits a kagome-like framework structure with large hexagonal, and small trigonal channels (diameters of ≈6 and ≈2 Å, respectively) and a specific surface area of S ≈1040 m g (V =0.
View Article and Find Full Text PDFNanosized SrSnO photocatalysts have been successfully synthesized by microwave synthesis in various ionic liquids (ILs) followed by a heat treatment process to optimize the materials' crystallinity. The influence of the ILs with various cations such as 1-butyl-3-methylimidazolium ([Cmim]), 6-bis(3-methylimidazolium-1-yl)hexane ([C(mim)]), butylpyridinium ([CPy]), and tetradecyltrihexylphosphonium ([P]) and bis(trifluoromethanesulfonyl)amide ([TfN]) as the anion on the structure, crystallization, and morphology of the products was investigated. The samples were characterized by X-ray diffraction (XRD), thermogravimetry (TG), scanning electron microscopy (SEM), surface area analysis by gas adsorption, X-ray photoelectron spectroscopy (XPS), diffuse reflectance UV-vis spectroscopy, and Raman and IR spectroscopy.
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