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1.
J Am Chem Soc ; 141(14): 5926-5933, 2019 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-30888800

RESUMO

The oxygen evolution reaction (OER) is a key process for renewable energy storage. However, developing non-noble metal OER electrocatalysts with high activity, long durability and scalability remains a major challenge. Herein, high OER activity and stability in alkaline solution were discovered for mixed nickel/cobalt hydroxide electrocatalysts, which were derived in one-step procedure from oriented surface-mounted metal-organic framework (SURMOF) thin films that had been directly grown layer-by-layer on macro- and microelectrode substrates. The obtained mass activity of ∼2.5 mA·µg-1 at the defined overpotential of 300 mV is 1 order of magnitude higher than that of the benchmarked IrO2 electrocatalyst and at least 3.5 times higher than the mass activity of any state-of-the-art NiFe-, FeCoW-, or NiCo-based electrocatalysts reported in the literature. The excellent morphology of the SURMOF-derived ultrathin electrocatalyst coating led to a high exposure of the most active Ni- and Co-based sites.

2.
Langmuir ; 34(16): 4888-4896, 2018 04 24.
Artigo em Inglês | MEDLINE | ID: mdl-29606005

RESUMO

Silicon nanocrystals (SiNCs) are abundant and exhibit exquisitely tailorable optoelectronic properties. The incorporation of SiNCs into highly porous and lightweight substrates such as aerogels leads to hybrid materials possessing the attractive features of both materials. This study describes the covalent deposition of SiNCs on and intercalation into silica aerogels, explores the properties, and demonstrates a prototype sensing application of the composite material. SiNCs of different sizes were functionalized with triethoxyvinylsilane (TEVS) via a radical grafting approach and subsequently used for the synthesis of photoluminescent silica hybrids. The resulting SiNC-containing aerogels possess high porosities, SiNC-based size-dependent photoluminescence, transparency, and a superhydrophobic macroscopic surface. The materials were used to examine the photoluminescence response toward low concentrations of 3-nitrotoluene (270 µM), demonstrating their potential as a sensing platform for high-energy materials.

3.
Microbiologyopen ; 13(5): e70000, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39365014

RESUMO

Thermophilic cyanobacteria thrive in extreme environments, making their thermoresistant enzymes valuable for industrial applications. Common habitats include hot springs, which act as evolutionary accelerators for speciation due to geographical isolation. The family Thermosynechococcaceae comprises thermophilic cyanobacteria known for their ability to thrive in high-temperature environments. These bacteria are notable for their photosynthetic capabilities, significantly contributing to primary production in extreme habitats. Members of Thermosynechococcaceae exhibit unique adaptations that allow them to perform photosynthesis efficiently at elevated temperatures, making them subjects of interest for studies on microbial ecology, evolution, and potential biotechnological applications. In this study, the genome of a thermophilic cyanobacterium, isolated from a hot spring near Okahandja in Namibia, was sequenced using a PacBio Sequel IIe long-read platform. Cultivations were performed at elevated temperatures of 40, 50, and 55°C, followed by proteome analyses based on the annotated genome. Phylogenetic investigations, informed by the 16S rRNA gene and aligned nucleotide identity (ANI), suggest that the novel cyanobacterium is a member of the family Thermosynechococcaceae. Furthermore, the new species was assigned to a separate branch, potentially representing a novel genus. Whole-genome alignments supported this finding, revealing few conserved regions and multiple genetic rearrangement events. Additionally, 129 proteins were identified as differentially expressed in a temperature-dependent manner. The results of this study broaden our understanding of cyanobacterial adaptation to extreme environments, providing a novel high-quality genome of Thermosynechococcaceae cyanobacterium sp. Okahandja and several promising candidate proteins for expression and characterization studies.


Assuntos
Cianobactérias , Genoma Bacteriano , Fontes Termais , Filogenia , RNA Ribossômico 16S , Namíbia , Cianobactérias/genética , Cianobactérias/classificação , Cianobactérias/metabolismo , Fontes Termais/microbiologia , RNA Ribossômico 16S/genética , Proteínas de Bactérias/genética , Proteínas de Bactérias/metabolismo , Temperatura Alta , Análise de Sequência de DNA , Proteoma/análise , DNA Bacteriano/genética
4.
Chempluschem ; 88(3): e202300045, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36786339

RESUMO

Herein, this work reports fiber spinning of tailored isotactic polypropylene (iPP) by melt spinning and melt drawing, yielding an adjustable diameter of 40-400 µm. The crystallinity of all obtained fibers with a molecular weight between 330-1400 kg/mol is increased by thermal annealing and investigated via differential scanning calorimetry (DSC) as well as wide angle X-ray scattering (WAXS). The potential of ultrahigh molecular weight iPP (UHMW-iPP) fibers compared to fibers manufactured from industrially available iPP becomes evident when the mechanical performance is compared: fibers spun from UHMW-iPP (1400 kg/mol) enable a tensile strength of up to 400 MPa, whereas commercially available fibers (330 kg/mol) show a tensile strength of approximately 50 MPa. However, UHMW-iPP exhibits a short timeframe, in which extrusion is possible, thereafter extrusion rupture occurs, probably induced by an increased melt viscosity.

5.
ACS Appl Mater Interfaces ; 12(2): 2655-2661, 2020 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-31840974

RESUMO

Defect engineering is a strategy for tailoring the properties of metal-organic frameworks (MOFs). Plenty of efforts have been devoted to study the defect chemistry and structures of bulk MOFs; however, the reported example of a defect-engineered surface-mounted MOF (SURMOF) thin film is rare. In this work, defects were incorporated in SURMOF thin films by using defect-generating linkers and taking advantage of the liquid-phase stepwise epitaxial layer-by-layer growth (LBL). Two methods based on the LBL, named mixing method and alternating method, are proposed for incorporating defects in the prototypical SURMOF HKUST-1 by partially substituting the parent H3btc (benzene-1,3,5-tricarboxylic acid) linker with a set of defect-generating linkers H2ip (isophthalic acid), H2OH-ip (5-hydroxyisophthalic acid), and H2pydc (3,5-pyridinedicarboxylic acid). The crystallinity and phase purity of the obtained "defected" SURMOFs were confirmed by X-ray diffraction, infrared reflection absorption spectroscopy, and Raman spectroscopy. The incorporation of the defect-generating linkers and the types of induced defects were characterized by ultraviolet-visible spectroscopy, time-of-flight secondary ion mass spectrometry, methanol adsorption, scanning electron microscopy, and 1H nuclear magnetic resonance spectroscopy (after digestion of the samples). These two methods provide avenues for controlling the defect formation in MOF thin films.

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