RESUMO
Porous nanospheres (PNSs) have great development prospects in the electrocatalysis field because of their structural characteristics, such as a large specific surface area. However, it is still a challenge to find a simple and energy-saving method for the controllable synthesis of PNS nanocatalysts. In this paper, a one-pot CTAC-assisted strategy was developed for the successful formation of PdPtAg PNSs with high porosity at room temperature. Benefitting from the unique structures, optimized composition, acceleration of charge transfer and enhanced resistance to CO poisoning, the PdPtAg PNSs displayed considerably improved electrocatalytic performance with high mass activity and stability toward the ethylene glycol oxidation reaction (EGOR) and glycerol oxidation reaction (GOR). The EGOR and GOR mass activities of PdPtAg were 5.00 A mgmetal-1 and 3.06 A mgmetal-1, which are 6.22 and 1.91 times that of commercial Pd/C, respectively. This work is expected to offer a new path for improving catalytic performance by simple design and adjustment of morphology.
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A highly sensitive and selective detection of volatile organic compounds (VOCs) by using gas sensors based on metal oxide semiconductor (MOS) has attracted increasing interest, but still remains a challenge in gas sensitivity and selectivity. In order to improve the sensitivity and selectivity of In2O3 to triethylamine (TEA), herein, a silver (Ag)-modification strategy is proposed. Ag nanoparticles with a size around 25-30 nm were modified on pre-synthesized In2O3 PNSs via a simple room-temperature chemical reduction method by using NaBH4 as a reductant. The results of gas sensing tests indicate that after functionalization with Ag, the gas sensing performance of In2O3 PNSs for VOCs, especially for TEA, was remarkably improved. At a lower optimal working temperature (OWT) of 300 °C (bare In2O3 sensor: 320 °C), the best Ag/In2O3-2 sensor (Ag/In2O3 PNSs with an optimized Ag content of 2.90 wt%) shows a sensitivity of 116.86/ppm to 1-50 ppm TEA, about 170 times higher than that of bare In2O3 sensor (0.69/ppm). Significantly, the Ag/In2O3-2 sensor can provide a response (Ra/Rg) as high as 5697 to 50 ppm TEA, which is superior to most previous TEA sensors. Besides lower OWT and higher sensitivity, the Ag/In2O3-2 sensor also shows a remarkably improved selectivity to TEA, whose selectivity coefficient (STEA/Sethanol) is as high as 5.30, about 3.3 times higher than that of bare In2O3 (1.59). The sensitization mechanism of Ag on In2O3 is discussed in detail.
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Precise synthesis of porous materials is essential for their applications. Self-assembly is a widely used strategy for synthesizing porous materials, but quantitative control of the assembly process still remains a great challenge. Here, a quantitative coassembly approach is developed for synthesizing resin/silica composite and its derived porous spheres. The assembly behaviors of the carbon and silica precursors are regulated without surfactants and the growth kinetics of the composite spheres are quantitatively controlled. This assembly approach enables the precise control of the size and pore structures of the derived carbon spheres. These carbon spheres provide a good platform to explore the structure-performance relationships of porous materials, and demonstrate their pore structure-dependent performance in catalytic water decontamination. This work provides a simple and robust approach for precise synthesis of porous spheres and brings insights into function-oriented design of porous materials.
RESUMO
Carbon-layer-coated porous Ni-doped CoSe2 (Ni-CoSe2 /C) nanospheres have been fabricated by a facile hydrothermal method followed by a new selenization strategy. The porous structure of Ni-CoSe2 /C is formed by the aggregation of many small particles (20-40â nm), which are not tightly packed together, but are interspersed with gaps. Moreover, the surfaces of these small particles are covered with a thin carbon layer. Ni-CoSe2 /C delivers superior rate performance (314.0â mA h g-1 at 20â A g-1 ), ultra-long cycle life (316.1â mA h g-1 at 10â A g-1 after 8000â cycles), and excellent full-cell performance (208.3â mA h g-1 at 0.5â A g-1 after 70â cycles) when used as an anode material for half/full sodium-ion batteries. The Na storage mechanism and kinetics have been confirmed by ex situ X-ray diffraction analysis, assessment of capacitance performance, and a galvanostatic intermittent titration technique (GITT). GITT shows that Na+ diffusion in the electrode material is a dynamic change process, which is associated with a phase transition during charge and discharge. The excellent electrochemical performance suggests that the porous Ni-CoSe2 /C nanospheres have great potential to serve as an electrode material for sodium-ion batteries.
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Heteroatom-doped polymers or carbon nanospheres have attracted broad research interest. However, rational synthesis of these nanospheres with controllable properties is still a great challenge. Herein, we develop a template-free approach to construct cross-linked polyphosphazene nanospheres with tunable hollow structures. As comonomers, hexachlorocyclotriphosphazene provides N and P atoms, tannic acid can coordinate with metal ions, and the replaceable third comonomer can endow the materials with various properties. After carbonization, N/P-doped mesoporous carbon nanospheres were obtained with small particle size (≈50â nm) and high surface area (411.60â m2 g-1 ). Structural characterization confirmed uniform dispersion of the single atom transition metal sites (i.e., Co-N2 P2 ) with N and P dual coordination. Electrochemical measurements and theoretical simulations revealed the oxygen reduction reaction performance. This work provides a solution for fabricating diverse heteroatom-containing polymer nanospheres and their derived single metal atom doped carbon catalysts.
RESUMO
Porous carbon materials produced by biomass have been widely studied for high performance supercapacitor due to their abundance, low price, and renewable. In this paper, the series of nitrogen-doped hierarchical porous carbon nanospheres (HPCN)/polyaniline (HPCN/PANI) nanocomposites is reported, which is prepared via in-situ polymerization. A novel approach with one-step pyrolysis of wheat flour mixed with urea and ZnCl2 is proposed to prepare the HPCN with surface area of 930 m2/g. Ultrathin HPCN pyrolysised at 900°C (~3 nm in thickness) electrode displays a gravimetric capacitance of 168 F/g and remarkable cyclability with losing 5% of the maximum capacitance after 5,000 cycles. The interconnected porous texture permits depositing of well-ordered polyaniline nanorods and allows a fast absorption/desorption of electrolyte. HPCN/PANI with short diffusion pathway possesses high gravimetric capacitance of 783 F/g. It can qualify HPCN/PANI to be used as cathode in assembling asymmetric supercapacitor with HPCN as anode, and which displays an exceptional specific capacitance of 81.2 F/g. Moreover, HPCN/PANI//HPCN device presents excellent cyclability with 88.4% retention of initial capacity over 10,000 cycles. This work will provide a simple and economical protocol to prepare the sustainable biomass materials based electrodes for energy storage applications.
RESUMO
Magnetic ß-cyclodextrin (ß-CD) porous polymer nanospheres (P-MCD) was fabricated by one-pot solvent thermal method using ß-CD immobilized Fe3O4 magnetic nanoparticles with tetrafluoroterephthalonitrile as the monomer. Compared with the ß-CD polymerization method reported in the literature,_ENREF_1 the synthetic route is effective and simple, thereby overcoming the harsh conditions that require nitrogen protection and always maintain anhydrous and oxygen-free. Moreover, the immobilization of ß-CD on magnetic nanoparticles is combined with the cross-linking polymerization of the cross-linker, leading to a good synergistic effect on the removal of contaminants. Meanwhile, the dispersibility of the magnetic carrier enhances the dispersion of the ß-CD porous polymer in the aqueous phase, and improves the inclusion adsorption performance and the adsorption process. P-MCD exhibited superior adsorption capacity and fast kinetics to MB. The maximum adsorption capacity of MB for P-MCD was 305.8â¯mgâ¯g -1, which is more than ß-CD modified Fe3O4 magnetic nanoparticles (Fe3O4@ß-CD). Moreover, the material had a short equilibrium time (5â¯min) for MB, high recovery and good recyclability (the adsorption efficiency was still above 86% after five repeated uses).
Assuntos
Magnetismo , Nanosferas , Poluentes Químicos da Água/química , Purificação da Água/métodos , beta-Ciclodextrinas/química , Adsorção , Cinética , Polímeros/química , PorosidadeRESUMO
Noble metal nanostructures (NMNSs) play a crucial role in many heterogeneous catalytic reactions. Hollow and porous NMNSs possess generally prominent advantages over their solid counterparts due to their unordinary structural features. In this work, we describe a facial one-pot synthesis of hollow and porous Pd-Cu alloy nanospheres (Pd-Cu HPANSs) through a polyethylenimine (PEI)-assisted oxidation-dissolution mechanism. The strong coordination interaction between CuII and PEI facilitates the oxidation-dissolution of the Cu2O nanospheres template under air conditions, which is responsible for the generation of the Pd-Cu alloy and the convenient removal of the Cu2O nanospheres template at room temperature. Compared to the commercial Pd black, the Pd-Cu HPANSs show remarkably improved catalytic activity for the reduction of K2Cr2O7 by HCOOH at room temperature, attributing to the enhanced catalytic activity of the Pd-Cu HPANSs for the dehydrogenation decomposition of HCOOH.