Novel organic–inorganic layer-by-layer (LbL) multilayers for visible-light phototropy, comprised of polyvinylpyrrolidone (PVP) and phosphomolybdic acid (PMoA), were fabricated via layer-by-layer (LbL) assembly with ultrasonic pretreatment. The characterizations revealed that the Keggin spatial geometry of the PMoA was still maintained in the final ultrasonic-assisted LbL thin films, which promoted halogenesis between the PVP and PMoA. Intriguingly, instead of destroying the PVP thin film, the ultrasonic pretreatment process successfully dispersed the PMoA in the PVP thin film with a median size of approximately 3.6 nm. Thanks to the dispersion of the PMoA particles, the photochromic capabilities of the ultrasonic-assisted PVP/PMoA LbL thin films gained remarkable improvement. Moreover, decreasing the size of the PMoA particles to quantum dots (10–3.4 nm) induces an up-conversion and dielectric confinement effect, which increases the intensity of the absorption peak (0.235 increased to 0.45) while narrowing the emission energy (2.51 eV narrowed to 2.23 eV). At the same time, the size reduction also extended the range of the absorption wavelength, increases the characteristic absorption intensity, and accelerates the coloration rate over the same illumination period.
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The exploration of efficient, low-cost and earth-abundant oxygen-evolution reaction (OER) electrocatalysts and the understanding of the intrinsic mechanism are important to advance the clean energy conversion technique based on electrochemical water oxidation. In this work, Fe-doping Co3N catalysts were successfully synthesized by a simple nitridation reaction of the Co3-xFexO4 precursor. This material exhibited a low overpotential of 294 mV at a current density of 10 mA cm?2, and a small Tafel slope of 49 mV dec?1 in 1 M KOH solution, superior to the performance of Co3N and IrO2. As revealed by the spectroscopic and electrochemical analyses, the enhanced OER performance mainly originates from the electronic modulation induced by the incorporation of Fe into Co3N, benefitting the formation of CoOOH as active surface species and thus facilitating the OER process. These findings also demonstrate the introduction of heterogeneous element is a simple and effective strategy to regulate the OER property of the cobalt nitrides (Co3N) catalysts. 相似文献
Hydrolytic dehydrogenation of ammonia borane (AB) driven by efficient catalysts has attracted considerable attention and is regarded as a promising strategy for hydrogen generation. Herein, RuP2 quantum dots supported on graphitic carbon nitride (g-C3N4) were successfully prepared by in-situ phosphorization, yielding a highly efficient photocatalyst toward AB hydrolysis. The catalysts were characterized by field-emission scanning electron microscopy, transmission electron microscopy, x-ray diffraction, x-ray photoelectron microscopy, inductively coupled plasma atomic emission spectroscopy, UV–visible diffuse reflectance spectroscopy and photoluminescence spectroscopy. A conventional water-displacement method was employed to record the hydrogen volume as a function of reaction time. Owing to visible-light irradiation, the initial turnover frequency of the AB hydrolysis was significantly enhanced by 110% (i.e., 134 min?1) at room temperature. Furthermore, the apparent activation energy decreased from 67.7 ± 0.9 to 47.6 ± 1.0 kJ mol?1. The photocatalytic hydrolysis mechanism and catalyst reusability were also investigated. 相似文献
Waste sugar solution (WSS), a waste by-product of manufacturing vitamin C, contains abundant waste acids and organics. In this work, a N/O-enriched copolymer was synthesized via a facile polymerization via the hydrogen bonding of O-containing functional groups and melamine and the crosslinking of aldehyde groups. Subsequently, N-doped carbon spheres were prepared by a typical carbonation/activation method. Remarkably, benefiting from an ultrahigh specific surface area (3612 m2/g) and rich heteroatom content (4.3% for N, 8.8% for O), the carbon spheres deliver a high specific capacitance of 387 F/g at 50 mA/g and 283 F/g at 5 A/g with 6 M KOH in two-electrode system. The assembled symmetric electric double-layer capacitor exhibits high energy density of 10.83 Wh/kg at 11.10 W/kg. This research provides a facile method for preparing N/O-doped carbon spheres by WSS, and confirms the excellent electrochemical performance of WSS-derived carbons in energy storage applications. 相似文献
Developing efficient oxygen evolution reaction (OER) electrocatalysts with earth-abundant elements is very important for sustainable H2 generation via electrochemical water splitting. Here we design a crystalline-amorphous Ni–Fe–Al hybrid phosphides nanosheet arrays grown on NiFe foam for efficient OER application. Dynamic surface reorganization of phosphides at anodic/cathodic polarizations is probed by in situ Raman spectroscopy. The reconstructed amorphous Ni(Fe)OOH species are determined as the active phases that facilitate the OER process. This unique electrode shows highly catalytic activity toward water oxidation, achieving the current densities of 10 and 100 mA cm?2 at 181 and 214 mV in 1 M KOH, respectively. Meanwhile, it also exhibits excellent stability at a large current density of 100 mA cm?2 for over 60 h. This work reveals the dynamic structural transformation of pre-catalyst in realistic conditions and highlights the important role of oxyhydroxides as real reactive species in OER process with high activity. 相似文献