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Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable energy conversion. In this regard, meticulous design of active sites and probing their catalytic mechanism on both cathode and anode with different reaction environment at molecular-scale are vitally necessary. Herein, a coordination environment inheriting strategy is presented for designing low-coordination Ni2+ octahedra (L-Ni-8) atomic interface at a high concentration (4.6 at.%). Advanced spectroscopic techniques and theoretical calculations reveal that the self-matching electron delocalization and localization state at L-Ni-8 atomic interface enable an ideal reaction environment at both cathode and anode. To improve the efficiency of using the self-modification reaction environment at L-Ni-8, all of the structural features, including high atom economy, mass transfer, and electron transfer, are integrated together from atomic-scale to macro-scale. At high current density of 500 mA/cm2, the samples synthesized at gram-scale can deliver low hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) overpotentials of 262 and 348 mV, respectively.
相似文献Carbon-carbon (C-C) coupling reactions represent one of the most powerful tools for the synthesis of complex natural products, bioactive molecules developed as drugs and agrochemicals. In this work, a multifunctional nanoreactor for C-C coupling reaction was successfully fabricated via encapsulating the core-shell Cu@Ni nanocubes into ZIF-8 (Cu@Ni@ZIF-8). In this nanoreactor, Ni shell of the core-shell Cu@Ni nanocubes was the catalytical active center, and Cu core was in situ heating source for the catalyst by absorbing the visible light. Moreover, benefiting from the plasmonic resonance effect between Cu@Ni nanocubes encapsulated in ZIF-8, the absorption range of nanoreactor was widened and the utilization rate of visible light was enhanced. Most importantly, the microporous structure of ZIF-8 provided shape-selective of reactant. This composite was used for the highly shape-selective and stable photocatalysed C-C coupling reaction of boric acid under visible light irradiation. After five cycles, the nanoreactor still remained high catalytical activity. This Cu@Ni@ZIF-8 nanoreactor opens a way for photocatalytic C-C coupling reactions with shape-selectivity.
相似文献Different synthesis routes for carbon nitride materials (CN) and the resulting products were compared to study the photocatalytic activity (pollutant degradation) in dependence on structure and properties. The CN materials were synthesized by thermal decomposition of dicyandiamide in air and under argon as well as in sealed ampoules with or without the use of a salt melt. The as-prepared materials were characterized by IR spectroscopy, nitrogen adsorption measurement, solid-state NMR spectroscopy, diffuse reflectance UV–Vis spectroscopy, elemental analysis and powder X-ray diffraction (PXRD). The surface polarity of the CN materials was estimated by adsorption of the dicyano-bis(1,10-phenanthroline)-iron(II) complex, which allows an evaluation of the degree of condensation. The CN materials were tested with regard to the photocatalytic degradation of rhodamine B (RhB). It is shown that the photocatalytic activity increases with higher surface polarity. Promising CN materials with high RhB degradation of 85% within 25 min and high surface polarity of 0.89 were selected for an immobilization approach to obtain coatings on a silicone substrate using a high-volume low-pressure (HVLP) spray coating technique. To study the photocatalytic activity of the catalyst coatings, the degradation rates of an aqueous RhB solution and solutions of organic pollutants such as triclosan and ethinyl estradiol were examined. Pollutants are decomposed with up to 63% of the initial concentration. Xenon lamps and different LEDs were used as light sources for comparison. Particularly high degradation efficiencies were obtained using LEDs, and the degradation rates are increased by adjusting the emission spectrum of the lamp to the pollutant and absorption edge of the catalyst, which results in a 40 times higher degradation efficiencies of LEDs compared to a Xe lamp.
Graphical abstract 相似文献In this paper, a novel compact semi-circular slot (SCS) 2 × 2 MIMO antenna is presented for 5G NR sub-6 GHz applications with high isolation. The proposed antenna consists of a semi-circular slot in ground plane, U-shaped stub, and 50-ohm microstrip feed line. The novelty of this paper are the Semi-Circular Slot acts a radiator, the port isolation is enhanced using a simple conductor strip as a neutralization line, very compact in size, low ECC, and good impedance matching. The overall size of the proposed SCS MIMO antenna is 16 mm x 21 mm, and FR4 substrate is used with thickness of 1.6 mm. The two SCS antenna elements are separated by edge-to-edge distance of 1mm (\(=0.019\lambda _{0}\)). The proposed compact MIMO antenna design is simulated using Ansys HFSS. To validate SCS MIMO antenna, a prototype was fabricated and tested. The measured results are attained at 5.5 GHz with isolation greater than 25dB, impedance bandwidth (S11\(<-10\) dB) covers from 5.10 GHz to 5.80 GHz with return loss of ? 39.5 dB. The MIMO antenna parameters, ECC, CCL, TARC, and MEG are studied, and the values are obtained within acceptable limits. The measured and simulated antenna results are almost similar. This compact MIMO antenna is suitable for 5G communications in sub-6 GHz wifi-5 band applications.
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