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1.
Inorg Chem ; 63(5): 2388-2400, 2024 Feb 05.
Article in English | MEDLINE | ID: mdl-38242537

ABSTRACT

When electrocatalysts are prepared, modification of the morphology is a common strategy to enhance their electrocatalytic performance. In this work, we have examined and characterized nanorods (3D) and nanosheets (2D) of nickel molybdate hydrates, which previously have been treated as the same material with just a variation in morphology. We thoroughly investigated the materials and report that they contain fundamentally different compounds with different crystal structures, chemical compositions, and chemical stabilities. The 3D nanorod structure exhibits the chemical formula NiMoO4·0.6H2O and crystallizes in a triclinic system, whereas the 2D nanosheet structures can be rationalized with Ni3MoO5-0.5x(OH)x·(2.3 - 0.5x)H2O, with a mixed valence of both Ni and Mo, which enables a layered crystal structure. The difference in structure and composition is supported by X-ray photoelectron spectroscopy, ion beam analysis, thermogravimetric analysis, X-ray diffraction, electron diffraction, infrared spectroscopy, Raman spectroscopy, and magnetic measurements. The previously proposed crystal structure for the nickel molybdate hydrate nanorods from the literature needs to be reconsidered and is here refined by ab initio molecular dynamics on a quantum mechanical level using density functional theory calculations to reproduce the experimental findings. Because the material is frequently studied as an electrocatalyst or catalyst precursor and both structures can appear in the same synthesis, a clear distinction between the two compounds is necessary to assess the underlying structure-to-function relationship and targeted electrocatalytic properties.

2.
ACS Catal ; 12(11): 6506-6516, 2022 Jun 03.
Article in English | MEDLINE | ID: mdl-35692248

ABSTRACT

In an effort to support the large-scale implementation of clean hydrogen in industry and society, the electrolytic decomposition of water is considered a realistically enticing prospect, provided the guarantee of affordable and durable material components. Within alkaline systems, earth-abundant electrocatalysts could provide both these requirements. However, a continued exploration of the reactivity and the causes behind different behaviors in performance are necessary to guide optimization and design. In this paper, Ta-doped NiO thin films are prepared via DC magnetron sputtering (1-2-4 at % Ta) to demonstrate the effect of surface electronic modulation by non-3d elements on the catalysis of the oxygen evolution reaction (OER). Material properties of the catalysts are analyzed via Rutherford backscattering spectrometry, X-ray diffractometry, photoelectron spectroscopy, and Raman spectroscopy. Ta impurities are shown to be directly responsible for increasing the valence state of Ni sites and enhancing reaction kinetics, resulting in performance improvements of up to 64 mV at 10 mA cm-2 relative to pristine NiO. Particularly, we show that by applying operando Raman spectroscopy, Ta enhances the ability to create high-valence Ni in γ-NiOOH at a lower overpotential compared to the undoped sample. The lowered overpotentials of the OER can thus be attributed to the energetically less hindered advent of the creation of γ-NiOOH species on the pre-catalyst surface: a phenomenon otherwise unresolved through simple voltammetry.

3.
Sci Rep ; 10(1): 19485, 2020 Nov 10.
Article in English | MEDLINE | ID: mdl-33173113

ABSTRACT

La0.4Pr0.3Ca0.1Sr0.2MnO3 has been investigated as a potential candidate for room temperature magnetic refrigeration. Results from X-ray powder diffraction reveal an orthorhombic structure with Pnma space group. The electronic and chemical properties have been confirmed by X-ray photoelectron spectroscopy and ion-beam analysis. A second-order paramagnetic to ferromagnetic transition was observed near room temperature (289 K), with a mean-field like critical behaviour at low field and a tricritical mean-field like behaviour at high field. The field induced crossover in critical behaviour is a consequence of the system being close to a first-order magnetic transition in combination with a magnetic field induced suppression of local lattice distortions. The lattice distortions consist of interconnected and weakly distorted pairs of Mn-ions, where each pair shares an electron and a hole, dispersed by large Jahn-Teller distortions at Mn3+ lattice sites. A comparatively high value of the isothermal entropy-change (3.08 J/kg-K at 2 T) is observed and the direct measurements of the adiabatic temperature change reveal a temperature change of 1.5 K for a magnetic field change of 1.9 T.

5.
Rev Sci Instrum ; 87(10): 103303, 2016 Oct.
Article in English | MEDLINE | ID: mdl-27802744

ABSTRACT

A dedicated detector system for heavy ion elastic recoil detection analysis at the Tandem Laboratory of Uppsala University is presented. Benefits of combining a time-of-flight measurement with a segmented anode gas ionization chamber are demonstrated. The capability of ion species identification is improved with the present system, compared to that obtained when using a single solid state silicon detector for the full ion energy signal. The system enables separation of light elements, up to Neon, based on atomic number while signals from heavy elements such as molybdenum and tungsten are separated based on mass, to a sample depth on the order of 1 µm. The performance of the system is discussed and a selection of material analysis applications is given. Plasma-facing materials from fusion experiments, in particular metal mirrors, are used as a main example for the discussion. Marker experiments using nitrogen-15 or oxygen-18 are specific cases for which the described improved species separation and sensitivity are required. Resilience to radiation damage and significantly improved energy resolution for heavy elements at low energies are additional benefits of the gas ionization chamber over a solid state detector based system.

6.
BMC Surg ; 14: 23, 2014 Apr 24.
Article in English | MEDLINE | ID: mdl-24762063

ABSTRACT

BACKGROUND: Infliximab, a TNF-α inhibitor, is a potent anti-inflammatory drug in the treatment of inflammatory bowel diseases. Recent studies have investigated the effect of infliximab treatment on postoperative complications such as anastomotic leakage, however, with conflicting results and conclusions. The purpose of this study was to investigate whether a single dose infliximab has an adverse effect on the anastomotic healing process, observed as reduced anastomotic breaking strength and histopathologically verified lower grade of inflammatory response, in the small intestine of a rabbit. METHODS: Thirty New Zealand rabbits (median weight 2.5 kg) were allocated to treatment with an intravenous bolus of either 10 mg/kg infliximab (n = 15) or placebo (n = 15). One week later all rabbits underwent two separate end-to-end anastomoses in the jejunum under general anesthesia. At postoperative day three, the anastomotic breaking strength was determined and histopathological changes were examined. RESULTS: The mean value of anastomotic breaking strength in the placebo group was 1.89 ± 0.36 N and the corresponding value was 1.81 ± 0.33 N in the infliximab treated rabbits. There was no statistically significant difference between the groups (p = 0.51). The infliximab-treated rabbits had a significant lower degree of inflammatory infiltration response compared to the placebo group (p = 0.047). CONCLUSIONS: Our conclusion, limited by the small sample sizes in both groups, is that a single dose of infliximab, given one week prior to surgery, does not have an impact on the anastomotic breaking strength on the third postoperative day in the small intestine of rabbits.


Subject(s)
Anti-Inflammatory Agents/adverse effects , Antibodies, Monoclonal/adverse effects , Inflammation/etiology , Jejunum/surgery , Postoperative Complications , Tensile Strength/drug effects , Wound Healing/drug effects , Anastomosis, Surgical , Animals , Anti-Inflammatory Agents/administration & dosage , Antibodies, Monoclonal/administration & dosage , Drug Administration Schedule , Female , Inflammation/diagnosis , Infliximab , Injections, Intravenous , Jejunum/drug effects , Preoperative Period , Rabbits , Random Allocation
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