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A series of seaweed-like heterogeneous Co3(PO4)2/Ni3(PO4)2/MOF-74-x electrocatalysts were synthesized via a hydrothermal method. The optimal composite exhibits excellent catalytic performance toward methanol/ethanol oxidation reactions (MOR/EOR) with peak current densities reaching 27.5 and 32.6 mA cm-2, respectively. This work heralds the advent of more efficient heterogeneous electrocatalysts for DAFCs and other energy conversion systems.
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In insects, metamorphosis is controlled by juvenile hormone (JH) and 20-hydroxyecdysone (20E). Krüppel homolog 1 (Kr-h1), a key JH-early inducible gene, is responsible for the suppression of metamorphosis and the regulation of the Broad-Complex (Br-C) gene, which is induced by 20E and functions as a "pupal specifier". In this study, we identified and characterized the expression patterns and tissue distribution of DaKr-h1 and DaBr-C at various developmental stages of Dendroctonus armandi. The expression of the two genes was induced by JH analog (JHA) methoprene and 20E, and their functions were investigated by RNA interference. DaKr-h1 and DaBr-C were predominantly expressed in the heads of larvae and were significantly downregulated during the molting stage. In contrast, the DaKr-h1 transcript level was highest in the adult anterior midgut. DaBr-C was mainly expressed in female adults, with the highest transcript levels in the ovaries. In the larval and pupal stages, both JHA and 20E significantly induced DaKr-h1, but only 20E significantly induced DaBr-C, indicating the importance of hormones in metamorphosis. DaKr-h1 knockdown in larvae upregulated DaBr-C expression, resulting in precocious metamorphosis from larvae to pupae and the formation of miniature pupae. DaKr-h1 knockdown in pupae suppressed DaBr-C expression, increased emergence, caused abnormal morphology, and caused the formation of small-winged adults. These results suggest that DaKr-h1 is required for the metamorphosis of D. armandi. Our findings provide insight into the roles of DaKr-h1 and DaBr-C in JH-induced transcriptional repression and highlight DaKr-h1 as a potential target for metamorphosis suppression in D. armandi.
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Engineering the heterogeneous interface fusing MOFs and inorganic active component is an effective strategy to improve the electrochemical performance. Herein, we report a new Ni3-based MOF (denoted as CTGU-24) with an infrequent two-fold interpenetrating 3D (3,8)-connected network constructed from Ni(II) trimer and mixed tripodal tectonics for the electrocatalytic methanol oxidation reaction (MOR). In order to improve its stability and activities, the heterogeneous hybrid CTGU-24@NiOOH has been fabricated successfully via the first preparation of the NiOOH nanosphere and then in situ formation of CTGU-24 decorated on the NiOOH surface. Moreover, the integration of CTGU-24@NiOOH and different additives [acetylene black (AB) and ketjen black (KB)], resulting in the optimized hybrid sample AB&CTGU-24@NiOOH (4:4). It attains better MOR performance with an area-specific peak current density of 34.53 mA·cm-2 than pure CTGU-24 (14.99 mA·cm-2) and improved durability in an alkali medium. The new findings indicate that the CTGU-24@NiOOH heterostructure formed in situ and the integration of moderate additives are critical to optimizing and improving electrocatalytic activity of pure MOF crystalline material.
RESUMO
Developing efficient metal-organic framework (MOF)-based electrocatalysts with improvable activity and persistence toward the methanol oxidation reaction (MOR) is attracting great research attention but still remains an enormous challenge. Herein, a facile strategy, hydrangea-shaped nickel hydroxide template-directed synthesis of the hierarchically structured Ni-MOF on the Ni(OH)2 heterocomposite (denoted as Ni-Ni) for efficient MOR, is developed. The unique hierarchical structure and synergistic effect of the heterocomposite afford more exposed active sites, a facile ion diffusion path, and improved conductivity, favorable for improving MOR catalytic performance. Remarkably, the optimized Ni-Ni-2 material delivers an excellent activity with a high peak current density (24.6 mA cm-2). Furthermore, to prove the universality of this strategy, NixCu1-x(OH)2 isometallic hydroxide was used as the precursor, and a series of MOF-74/CuxNi1-x(OH)2 (denoted as Ni-NiCu) heterogeneous materials have been prepared and could be used as an effective electrocatalyst to catalyze MOR. The results indicate that this strategy can be used in the synthesis of other new composite materials with specific hierarchical structures for a more efficient electrocatalytic system.
RESUMO
Designing novel multifunctional rare-earth metal-organic frameworks (MOFs) has attracted intensive attention. In particular, employing such materials for sensing or catalytic reactions is still very challenging. Here, a new 3D porous Eu(iii)-MOF, [Eu(cppa)(OH)]·xS (denoted as CTGU-19, S = solvent molecule, CTGU = China Three Gorges University), was synthesized by using 5-(4-carboxyphenyl)picolinic acid (H2cppa) as an organic ligand, and it shows a 3D (3,12)-connected topological net with the point symbol (420·628·818)(43)4, constructed from cubane-shaped tetranuclear europium building units. Interestingly, CTGU-19 can be used as a highly sensitive luminescent sensor to identify ornidazole (ODZ) and nitrofurantoin (NFT) at different excitation wavelengths. This result represents the first example of a lanthanide-metal-organic-framework (Eu-MOF) that can be employed as a discriminating fluorescent probe to recognize ODZ and NFT at different excitation wavelengths. Furthermore, after loading CTGU-19 with Ag and/or Au nanoparticles, the composites exhibit efficient catalytic performance for reducing 2-/3-/4-nitrophenols (2-/3-/4-NP), in which the unit mass reduction rate constants of Ag0.8Au0.2@CTGU-19 for 2-NP, 3-NP, and 4-NP reach 68.8, 53.80, and 52.34 s-1 g-1, respectively.