the anode, required the large overpotential (η) to overcome the sluggish kinetically and hindered practical utilization of water splitting technology. [7][8][9] Efficient catalysts should be designed and synthesized to decrease the overpotential and accelerate the kinetically for the OER. Although state-of-the-art precious metalbased materials (e.g., RuO 2 or IrO 2 ) are the benchmark catalysts for OER, they are very costly due to their limited resources on earth. [10,11] Huge efforts have therefore been devoted to fabricate efficient and alternative electrocatalysts.Over the last few decades, extensive attentions have been paid to earth-abundant and cost-efficient (3d) transition metal-based alternatives. [1,7,9,12] Apart from the well-developed metal oxides and (oxy)hydroxides catalysts, [2,13]
We report metallurgy on the nanoscale to generate metal nanoparticles and their simultaneous patterning in a single step. This is achieved by the self-reduction of porous metal–organic framework crystals using nanosecond pulsed laser irradiation. Metal nanoparticles of Fe, Co, Ni, Cu, Zn, Cd, In, Bi, and Pb with uniform sizes (controllable between 3 to 200 nm) and gaps (as narrow as 2 nm) are produced by nine different metal–organic frameworks, where atomically dispersed non-noble metal ions are reduced and gathered across the pores. The instant light absorption and cooling at local positions by a laser allows for precise and efficient patterning of metal nanoparticles. This new method is suitable for device fabrication at a speed of 15 mm2 s–1 on glass, consuming only 1.5 W of power. A large variety of metal nanoparticle three-dimensional architectures are demonstrated, among which one architecture exhibits an enhanced plasmonic effect homogeneously across the entire pattern for the detection of molecules at an extremely low concentration (10–12 M). These architectures are extremely stable under air and humidity during production, use, and storage, without altering the oxidation state, for 6 months.
In this study, we report a novel and efficient fluorescence probe synthesized by Tris(hydroxymethyl)aminomethane-derived carbon dots (CDs)-modified hexagonal cobalt oxyhydroxide(CoOOH) nanoflakes (Tris-derived CDs-CoOOH) for monitoring of cerebral ascorbic acid (AA) in brain microdialysate. The as-prepared Tris-derived CDs with the fluorescence quantum yield of 7.3% are prepared by a one-step pyrolysis strategy of the sole precursor and used as the signal output. After being hybridized with CoOOH nanoflakes to form Tris-derived CDs-CoOOH, the luminescence of the Tris-derived CDs can be efficiently quenched by CoOOH via fluorescence resonance energy transfer (FRET). Due to the specific redox reaction between the enediol group of AA and hexagonal CoOOH nanoflakes, AA can reduce the hexagonal CoOOH nanoflakes in the Tris-derived CDs-CoOOH and lead to collapse of the hybrized structure, then the release of Tris-derived CDs, and thus finally the fluorescence recovery. Moreover, cobalt ions (II), generated by CoOOH nanoflakes oxidizing AA, almost have no obvious interference on the fluorescence probe, i.e., Tris-derived CDs, which could be ascribed to the surface of Tris-derived CDs containing a few strong chelation groups such as amino/carboxyl/thiol groups, instead of plenty of -OH groups with weak chelation with Co(2+). On the basis of this feature, the Tris-derived CDs-CoOOH fluorescent probe demonstrates a linear range from 100 nM to 20 μM with the detection limit of ∼50 nM, i.e., with an improved sensitivity toward AA detection. Compared with other turn-on fluorescent methods using convenient fluorophore-nitroxide fluorescent probes for detection of AA, the method demonstrated here possesses a facial synthesis route, lower limit of detection, and wider linear range, which validates sensing of AA in the cerebral systems during the calm/ischemia process. This study provides a fluorescence assay for the simple yet facial detection of AA in the cerebral systems and assists in the understanding of the biological processes in the physiological and pathological study.
With flaky BaFe12O19 nanoparticles (BF NPs, 10-20 nm in thickness) as polymerization seeds, electromagnetic functionalized and microstructured quasi-spherical PPY/BF (PPY: polypyrrole) organic-inorganic composites were prepared by a conventional in situ chemical oxidative polymerization. X-ray diffraction and Fourier transform infrared analyses interpreted that there was no obvious chemical interaction between BF NPs and PPY in the composites but that BF NPs only served as the nucleation sites for the polymerization of pyrrole. As compared to pure BF NPs, PPY/BF composites showed distinct increases in electrical conductivities and decreases in magnetization and thus improved the matched characteristic impedance of the free space, leading to a substantial enhancement of reflection loss at 2-18 GHz. For the first time, multi-layered and single-layered films formed at different places on the reaction flask were studied by scanning electron microscopy and energy dispersive X-ray analysis, indicating that the films composed of quasi-spherical microstructures can be very different in morphology but surprisingly contain no BF NPs.
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