共查询到20条相似文献,搜索用时 15 毫秒
1.
Jian Liu Rong Chen Xun Zhu Qiang Liao Dingding Ye Biao Zhang Ming Liu Gang Chen Kun Wang 《RSC advances》2019,9(41):23560
In this study, we proposed a Pd–polyelectrolyte multilayer (PEM) hybrid film grafted on the polydopamine coated interior wall of a microreactor for nitrobenzene hydrogenation. Here, Pd nanoparticles were in situ synthesized in the PEMs consisting of poly(diallyldimethylammonium chloride) and poly(styrene sulfonate) via a two-stage ion-exchange and reduction process. The preparation process was monitored by UV-vis spectroscopy, which confirmed the formation of Pd in the PEM film. In addition, SEM and ICP-OES results indicated that the Pd content in the PEM film could be controlled by the number of the ion exchange and reduction cycles. Experimental results also showed that the prepared Pd–PEM hybrid film was active for the hydrogenation of nitrobenzene. The microreactor with the Pd–PEM hybrid film via multiple times had the increased catalyst loading, leading to a high yield of aniline and much better durability. In addition, it was also found that the NaCl concentration in the polyelectrolyte solution could affect the structure of the PEM film and therefore the Pd loading and catalytic performance.In this study, we developed a Pd–PEMs hybrid film grafted on the polydopamine coated interior wall of a microreactor for nitrobenzene hydrogenation. 相似文献
2.
X-ray powder diffraction to analyse bimetallic core–shell nanoparticles (gold and palladium; 7–8 nm)
A comparative X-ray powder diffraction study on poly(N-vinyl pyrrolidone) (PVP)-stabilized palladium and gold nanoparticles and bimetallic Pd–Au nanoparticles (both types of core–shell nanostructures) was performed. The average diameter of Au and Pd nanoparticles was 5 to 6 nm. The two types of core–shell particles had a core diameter of 5 to 6 nm and an overall diameter of 7 to 8 nm, i.e. a shell thickness of 1 to 2 nm. X-ray powder diffraction on a laboratory instrument was able to distinguish between a physical mixture of gold and palladium nanoparticles and bimetallic core–shell nanoparticles. It was also possible to separate the core from the shell in both kinds of bimetallic core–shell nanoparticles due to the different domain size and because it was known which metal was in the core and which was in the shell. The spherical particles were synthesized by reduction with glucose in aqueous media. After purification by multiple centrifugation steps, the particles were characterized with respect to their structural, colloid-chemical, and spectroscopic properties, i.e. particle size, morphology, and internal elemental distribution. Dynamic light scattering (DLS), differential centrifugal sedimentation (DCS), atomic absorption spectroscopy (AAS), ultraviolet-visible spectroscopy (UV-vis), high-angle annular dark field imaging (HAADF), and energy-dispersed X-ray spectroscopy (EDX) were applied for particle characterization.A comparative X-ray powder diffraction study on poly(N-vinyl pyrrolidone) (PVP)-stabilized palladium and gold nanoparticles and bimetallic Pd–Au nanoparticles (both types of core–shell nanostructures) was performed. 相似文献
3.
Weiping Li Tianxiang Zhou Zhilu Le Mengyin Liao Hesheng Liu Bing Na Bin Wang Haiying Zhou Heng Yan 《RSC advances》2018,8(62):35496
The thermal treatment of bimetallic nanocatalysts plays an important role in determining their catalytic performance. Here tuning the surface oxidized metal species of bimetallic Pd–Fe electrocatalysts for the formic acid (FA) oxidation reaction is reported and a correlation between the surface oxidized metal species of the Pd–Fe nanoparticles and their catalytic activities is proposed. The structural details of the Pd–Fe/C catalysts are characterized by X-ray diffraction, X-ray photoelectron spectroscopy and high-sensitivity low-energy ion scattering (HS-LEIS). Cyclic voltammetry measurements demonstrated that the mass activity of the Pd–Fe nanoparticles with a molar ratio of Pd/Fe = 1/15 is about 7.4 times higher than that of Pd/C. This enhancement could be attributed to the synergistic effect between Pd(0) and Pd oxidized species on the surface of the Pd–Fe/C treated sample and electronic effects. This finding demonstrates the importance of surface oxidized metal species at the nanoscale in harnessing the true electrocatalytic potential of bimetallic nanoparticles and opens up strategies for the development of highly active bimetallic nanoparticles for electrochemical energy conversion.The thermal treatment of bimetallic nanocatalysts plays an important role in determining their catalytic performance. 相似文献
4.
Chromium contamination in the aquatic environment is an urgent and serious issue due to its mutagenic and carcinogenic effects against living organisms. The present study demonstrates the capability of biogenic sulfur nanoparticles (SNPs) for the reduction of hexavalent chromium into a less toxic state. A green approach was adapted for the synthesis of SNPs using F. benghalensis leaf extract which acts as a reducing and capping agent. The biosynthesized SNPs were characterized by UV-Vis spectroscopy, X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), atomic force microscopy (AFM), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HR-TEM) and energy dispersive X-ray spectroscopy (EDX). TEM micrographs revealed that the zero-valent sulfur nanoparticles were in the range of 2–15 nm and the average size of 5.1 nm. The conversion rate of Cr(vi) into Cr(iii) in the presence of SNPs was 88.7% in 80 min. The optimum concentration ratio between SNPs and formic acid was 10 ppm : 480 mM.Biosynthesized sulphur nanoparticles showed high efficiency in the reduction of Cr(vi) even at a small catalyst/Cr(vi) ratio. 相似文献
5.
Pd–P@Pt–Ni core–shell nanoparticles, which consisted of a Pd–P alloy as a core and Pt–Ni thin layer as a shell, were explored as electrocatalysts for methanol oxidation reaction. The crystallographic information and the electronic properties were fully investigated by X-ray diffraction and X-ray photoelectron spectroscopy. In the methanol electrooxidation reaction, the particles showed high catalytic activity and strong resistance to the poisoning carbonaceous species in comparison with those of commercial Pt/C and the as-prepared Pt/C catalysts. The excellent durability was demonstrated by electrochemically active surface area loss and chronoamperometric measurements. These results would be due to the enhanced catalytic properties of Pt by the double synergistic effects from the core part and the nickel species in the shell part.The Pd–P@Pt–Ni core–shell nanoparticles consist of an amorphous core and a low-crystalline shell. They exhibit the excellent catalytic properties in MOR owing to the double synergistic effects from the core and the nickel species in the shell. 相似文献
6.
Cu foil is widely used in commercial lithium ion batteries as the current collector of anode materials with excellent conductivity and stability. In this research, commercial Cu foil was chosen as the current collector and substrate for the synthesis of Cu doped flake-NiO via a traditional hydrothermal method. The effect of the ratio of Cu and the calcination temperature on the electrochemical performance of NiO was investigated. The structure and phase composition of the Cu doped flake-NiO electrode were studied through X-ray diffraction (XRD), scanning electron microscopy (SEM), Energy dispersive X-ray analysis (EDAX), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and inductive coupled plasma emission spectrometry (ICP). The electrochemical properties of the Cu doped flake-NiO electrode were studied through cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and a galvanostatic charge–discharge cycling technique. According to the results, the Cu-doped NiO electrode, calcined at 400 °C with a molar ratio of Cu : Ni = 1 : 8, exhibited a high reversible charge capacity. The good cycling stability and rate performance indicate that the as-prepared electrode can be applied as a potential anode for lithium ion batteries.Cu doped flake-NiO shows excellent electrochemical performance as anode materials for lithium ion batteries. 相似文献
7.
CuO–CeO2 nanocatalysts with different amounts of Mn dopping (Mn/Cu molar ratios of 0.5 : 5, 1 : 5 and 1.5 : 5) were synthesized by flame spray pyrolysis (FSP) method and tested in the catalytic oxidation of CO. The physicochemical properties of the synthesised samples were characterized systematically, including using X-ray diffraction (XRD), Raman spectroscopy, field-emission scanning electron microscopy (FESEM), Brunauer–Emmett–Teller (BET), X-ray photoelectron spectroscopy (XPS), oxygen-temperature programmed desorption (O2-TPD), hydrogen-temperature programmed reduction (H2-TPR) and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). The results showed that the 1Mn–Cu–Ce sample (Mn/Cu molar ratio of 1 : 5) exhibited superior catalytic activity for CO oxidation, with the temperature of 90% CO oxidation at 131 °C at a high space velocity (SV = 60 000 mL g−1 h−1), which was 56 °C lower than that of the Cu–Ce sample. In addition, the 1Mn–Cu–Ce sample displays excellent stability with prolonged time on CO stream and the resistance to water vapor. The significantly enhanced activity was correlated with strong synergetic effect, leading to fine textual properties, abundant chemically adsorbed oxygen and high lattice oxygen mobility, which further induced more Cu+ species and less formation of carbon intermediates during the CO oxidation process detected by in situ DRIFTS analysis. This work will provide in-depth understanding of the synergetic effect on CO oxidation performances over Mn doped CuO–CeO2 composite catalysts through FSP method.The synergetic effect is promoted on Mn doped CuO–Ce O2 catalyst to induce less carbon intermediates to enhance CO oxidation performance. 相似文献
8.
Danqing Liu Xingxing Lv Chaoyue Zhao Jiayue Li Jinmei Huang Ling Weng Liangcan He Shaoqin Liu 《RSC advances》2022,12(46):30174
Foodborne or water-borne pathogens pose great threats to human beings and animals. There is an urgent need to detect pathogens with cheap, rapid and sensitive point-of-care diagnostic assays. Herein, we report the electrochemiluminescent (ECL) behaviors of NaBiF4 : Yb3+/Er3+ upconversion nanoparticles (UCNPs) which were synthesized via a fast and environment-friendly method at room temperature for the first time. The UCNPs together with K2S2O8 exhibit high ECL intensity and stable cathodic signals. Further, the Au nanoparticles (Au NPs) and Anti-E. coli O157 : H7 antibody were assembled on the surface of UCNPs successively to construct a novel ECL immunosensor for the detection of deadly E. coli O157 : H7. The as-prepared ECL immunosensor reveals high sensitivity to E. coli O157 : H7 in a linear range of 200–100 000 CFU mL−1, and the minimum detection limit could reach up to 138 CFU mL−1. The designed UCNP-based biosensor demonstrates high specificity, good stability and remarkable repeatability, and the strategy will provide a sensitive and selective method for rapid detection of E. coli O157 : H7 in food safety and preclinical diagnosis.The ECL behaviors of NaBiF4 : Yb3+/Er3+ UCNPs synthesized via a fast and environment-friendly method are reported for the first time. UCNPs-based ECL biosensor shows a wide detection range with low detection limit of 138 CFU mL−1 for E. coli O157 : H7. 相似文献
9.
Supported bimetallic nanoparticles are particularly attractive catalysts due to increased activity and stability compared to their monometallic counterparts. In this work, gold-based catalysts have been studied as catalysts for the selective base-free oxidation of glucose. TiO2-supported Au–Pd and Au–Cu series prepared by the sol-immobilization and precipitation-reduction methods, respectively, showed a significant synergistic effect, particularly when the theoretical weight ratio of the two metals was close to 1 : 1 (with an actual experimental bulk Au/Pd molar ratio of ca. 0.8 and ca. 0.4 for Au/Cu) in both cases. XPS analysis showed that the presence of Auδ+, Pd2+ and CuOH species played an important role in the base-free glucose oxidation.Supported bimetallic nanoparticles are particularly attractive catalysts due to increased activity and stability compared to their monometallic counterparts. 相似文献
10.
Xingyan Liu Guangmei Jiang Yuwei Tan Shuang Luo Mengmeng Xu Yiming Jia Peng Lu Youzhou He 《RSC advances》2020,10(24):14313
For the first time, highly-dispersed ruthenium precursors via a hydrogen-bond-driven melamine–cyanuric acid supramolecular complex (denoted CAM) self-assembly-assisted synthesis of uniform ruthenium nanoparticles with superior HER performance under both acidic and alkaline conditions are reported. Electrochemical tests reveal that when the current density is −10 mA cm−2, the optimal Ru/CNO electrocatalyst could express low overpotentials of −18 mV and −46 mV, low Tafel slopes of 46 mV dec−1 and 100 mV dec−1, in 0.5 M H2SO4 and 1.0 M KOH, respectively. The remarkable HER performance could be attributed to uniform ruthenium with the aid of highly dispersed ruthenium precursors (Ru–CAM) and subsequent annealing results in uniform ruthenium nanoparticles.Highly dispersed ruthenium precursors via a supramolecular self-assembly assisted synthesis of uniform ruthenium nanoparticles with excellent HER performance. 相似文献
11.
Ping Wang Hao Liu Congxin Wang Guang Lv Donge Wang Huaijun Ma Zhijian Tian 《RSC advances》2021,11(41):25364
In industrial application, molecular sieves are usually used in a certain shape. This requires the addition of binder and causes the reduction of both the molecular sieve content and catalytic performance. Herein, pseudo-boemite was mixed with deionized water at room temperature, followed by the drop-wise addition of phosphoric acid, magnesium acetate solution, hydrofluoric acid, di-n-propylamine and 1-ethyl-3-methyl imidazolium bromide with vigorous stirring. The molar ratio of Al2O3 : P2O5 : MgO : HF : DPA : [EMIm]Br : H2O in the gel was 1 : 1 : 0.03 : 0.18 : 0.4 : 1 : 45. Then the gel was dried, extruded and directly crystallized to form a shaped MgAPO-11 molecular sieve. X-ray diffraction, scanning electron microscopy, N2 adsorption, ammonia temperature programmed desorption, pyridine adsorption infrared spectroscopy and nuclear magnetic resonance spectroscopy were used to investigate the physicochemical properties of the samples. X-ray diffraction, scanning electron microscopy and N2 adsorption tests show that the shaped MgAPO-11 molecular sieve is fully crystallized and possesses hierarchical porosity. Mg is incorporated into the molecular sieve framework and the Pt catalyst supported by the obtained shaped MgAPO-11 exhibits excellent catalytic performance with n-dodecane conversion of 94% and isomer selectivity of 95% at 280 °C. Such a method for the direct synthesis of shaped molecular sieves shows potential for the green synthesis of molecular sieves in industry.Shaped MgAPO-11 with hierarchical pores can be directly synthesized via a solid transformation route. Fewer synthesis steps and superior catalytic performance make the route possess great potential in practical applications. 相似文献
12.
The Pd/CeO2 catalyst, which is highly active catalyst in automobile emission control especially for CO oxidation, often suffers from severe sintering under harsh condition, specifically hydrothermal treatment. Here, we report re-dispersion of Pd-based bimetallic (Pd–Fe, Pd–Ni, and Pd–Co) catalysts deposited on ceria by hydrothermal treatment at 750 °C using 10% H2O. The re-dispersion was confirmed by various characterization techniques of transmission electron microscopy, CO chemisorption, CO-diffuse reflectance infrared Fourier transform, CO-temperature programmed desorption, and X-ray absorption spectroscopy. The dispersion of Pd increased significantly after hydrothermal treatment, resulting in improved CO oxidation activity. The presence of secondary transition metals enhanced the CO oxidation activity further, especially hydrothermally treated Pd–Fe bimetallic catalyst showed the highest activity for CO oxidation.PdM (M: Fe, Co, Ni) catalysts deposited on ceria were hydrothermally treated, resulting in re-dispersion of the metal species. They showed enhanced activity for CO oxidation. 相似文献
13.
Masato Miyakawa Norihito Hiyoshi Hidekazu Koda Kenichi Watanabe Hideki Kunigami Hiroshi Kunigami Akira Miyazawa Masateru Nishioka 《RSC advances》2020,10(11):6571
Continuous syntheses of carbon-supported Pd@Pt core–shell nanoparticles were performed using microwave-assisted flow reaction in polyol to synthesize carbon-supported core Pd with subsequent direct coating of a Pt shell. By optimizing the amount of NaOH, almost all Pt precursors contributed to shell formation without specific chemicals.Continuous syntheses of carbon-supported Pd@Pt core–shell nanoparticles were performed using flow processes including microwave-assisted Pd core–nanoparticle formation.Continuous flow syntheses have attracted attention as a powerful method for organic, nanomaterial, and pharmaceutical syntheses because of various features that produce benefits in terms of efficiency, safety, and reduction of environmental burdens.1–7 Advances of homogeneous heating and mixing techniques in continuous flow reactors have engendered further developments for precise reaction control, which is expected to create innovative materials through combination with multiple-step flow syntheses.Microwave (MW) dielectric heating has been recognized as a promising methodology for continuous flow syntheses because rapid or selective heating raises the reaction rate and product yield.8–18 For the last two decades, most MW apparatus has been batch-type equipped with a stirring mechanism in a multi-mode cavity. Therefore, conventionally used MW-assisted flow reactors have been mainly of the modified batch-type. Results show that the electromagnetic field distribution can be spatially disordered, causing inhomogeneous heating of the reactor.19–25 Improvements of reactors suitable for flow-type work have been studied actively in recent years to improve their energy efficiency and to make irradiation of MW more homogeneous.26–37We originally designed a MW flow reactor system that forms a homogeneous heating zone through generation of a uniform electromagnetic field in a cylindrical single-mode MW cavity.26,30 The temperatures of flowing liquids in the reactor were controlled precisely via the resonance frequency auto-tracking function. Continuous flow syntheses of metal nanoparticle, metal-oxide, and binary metal core–shell systems with uniform particle size have been achieved using our MW reactor system.26,38,39 Furthermore, large-scale production necessary for industrial applications can be achieved through integration of multiple MW reactors.30Carbon-supported metal catalysts are widely used in various chemical transformations and fine organic syntheses. Particularly, binary metal systems such as Pd@Pt core–shell nanoparticles have attracted considerable interest for electro-catalysis in polymer electrolyte membrane fuel cells (PEMFC) because of their enhanced oxygen reduction activity compared to a single-use Pt catalyst. Binary metal systems also contribute to minimization of the usage of valuable Pt.40–51 Earlier studies of carbon-supported Pd@Pt syntheses involved multiple steps of batch procedures such as separation, washing and pre-treatment of core metal nanoparticles, coating procedures of metal shells, and dispersion onto carbon supports. Flow-through processes generally present advantages over batch processes in terms of simplicity and high efficiency in continuous material production.We present here a continuous synthesis of carbon-supported Pd and Pd@Pt core–shell nanoparticles as a synthesis example of a carbon-supported metal catalyst using our MW flow reactor. This system incorporates the direct transfer of a core metal dispersion into a shell formation reaction without isolation. Nanoparticle desorption is prevented by nanoparticle synthesis directly on a carbon support. The presence of protective agents that are commonly used in nanoparticle syntheses, such as poly(N-vinylpyrrolidone), can limit the chemical activity of the catalyst. Nevertheless, this system requires no protective agent. Moreover, this system is a simple polyol synthesis that uses no strong reducing agent. It therefore imposes little or no environmental burden. For this study, the particle size and distribution of metals in Pd and Pd@Pt core–shell nanoparticles were characterized using TEM, HAADF-STEM observations, and EDS elemental mapping. From electrochemical measurements, the catalytic performance of Pd@Pt core–shell nanoparticles was evaluated.A schematic view of the process for the continuous synthesis of carbon-supported Pd@Pt core–shell nanoparticles is presented in Fig. 1. Details of single-mode MW flow reactor are described in ESI.† We attempted to conduct a series of reactions coherently in a flow reaction system, i.e., MW-assisted flow reaction for the synthesis of carbon supported core Pd nanoparticles with subsequent deposition of the Pt shell. Typically, a mixture containing Na2[PdCl4] (1–4 mM) in ethylene glycol (EG), carbon support (Vulcan XC72, 0.1 wt%), and an aqueous NaOH solution were prepared. This mixture was introduced continuously into the PTFE tube reactor placed in the center of the MW cavity. Here, EG works as the reaction solvent as well as the reducing agent that converts Pd(ii) into Pd(0) nanoparticles. The MW heating temperature was set to 100 °C with the flow rate of 80 ml h−l, which corresponds to residence time of 4 s. The carbon-supported Pd nanoparticles were transferred directly to the Pt shell formation process without particle isolation. The dispersed solution was introduced into a T-type mixer and was mixed with a EG solution of H2[PtCl6]·6H2O (10 mM). The molar ratio of Pd : Pt was fixed to 1 : 1. Subsequently, after additional aqueous NaOH solution was mixed at the second T-mixer, the reaction mixture was taken out of the mixer and was let to stand at room temperature (1–72 h) for Pt shell growth.Open in a separate windowFig. 1Schematic showing continuous synthesis of carbon-supported Pd and Pd@Pt core–shell nanoparticles. The Pd nanoparticles were dispersed on the carbon support by MW heating of the EG solution. The solution was then transferred directly to Pt shell formation.Rapid formation of Pd nanoparticles with average size of 3.0 nm took place at the carbon-support surface during MW heating in the tubular reactor (Fig. 2a). Most of the Pd(ii) precursor was converted instantaneously to Pd(0) nanoparticles and was well dispersed over the carbon surface. Fig. 2b shows the time profile of the outlet temperature and applied MW power during continuous synthesis of carbon-supported Pd nanoparticles. The solution temperature rose instantaneously, reaching the setting temperature in a few seconds. This temperature was maintained with high precision (±2 °C) by the continuous supply of ca. 18 W microwave power. No appreciable deposition of metal was observed inside of the PTFE tube. It is noteworthy that Pd of 98% or more was supported on carbon by heating for 4 s at 100 °C from ICP-OES measurement. Our earlier report described continuous polyol (EG) synthesis of Pd nanoparticles as nearly completed with 6 s at 200 °C.39 The reaction temperature in polyol synthesis containing the carbon was considerably low, suggesting that selective reduction reaction occurs on the carbon surface, which is a high electron donating property.Open in a separate windowFig. 2(a) TEM image of carbon-supported Pd nanoparticles synthesized using the MW flow reactor. The average particle size was 3.0 nm. (b) The time profile of the temperature at the reactor outlet and applied microwave power during continuous synthesis of carbon-supported Pd nanoparticles. Na2[PdCl4] = 2 mM, NaOH = 10 mM.The concentrations of Na2[PdCl4] precursor and NaOH affect the Pd nanoparticle size. Results show that the Pd particle size increased as the initial concentration of Na2[PdCl4] increased (Fig. S1a and b†). Change of NaOH concentration exerted a stronger influence on the particle size. Nanoparticles of 12.3 nm were observed without addition of NaOH, whereas 2.6 nm size particles were deposited at the concentration of 20 mM (Fig. S1c and d†). The higher NaOH concentration led to instantaneous nucleation and rapid completion of reduction. The Pd nanoparticle surface is equilibrated with Pd–O− and Pd–OH depending on the NaOH concentration. The surface is more negative at high concentrations of NaOH because of the increase of the number of Pd–O−, which inhibits the mutual aggregation and further particle growth. Furthermore, to control the Pd nanoparticle morphology, we conducted synthesis by adding NaBr, which has been reported as effective for cubic Pd nanoparticle synthesis.52 However, because reduction of the Pd precursor derives from electron donation from both the polyol and the carbon support, morphological control was not achieved (Fig. S2†). That finding suggests that morphological control is difficult to achieve by adding surfactant agents to the polyol.For Pt shell formation, carbon supported Pd nanoparticles (3.0 nm average particle size) were mixed with H2[PtCl6]·6H2O solution with the molar ratio of Pd : Pt = 1 : 1. Then additional NaOH solution was mixed. As described in earlier reports,39 alkaline conditions under which base hydrolysis and reduction of [PtCl6]2− to [Pt(OH)4]2− takes place are necessary for effective Pt shell formation. It is noteworthy that the added Pt precursor was almost entirely supported on carbon within 24 h in cases where an appropriate amount of additional NaOH (5 mM) was mixed by the second T-mixer (Fig. 3a). However, for 10 mM, nucleation and growth of single Pt nanoparticles were enhanced in place of core–shell formation. Consequently, a mixture of Pd@Pt and single Pt nanoparticles was formed on the carbon support (Fig. 3b). Very fine Pt nanoparticles were observed in the supernatant solution.Open in a separate windowFig. 3(a) Time profiles of residual ratio of Pt in the mixed solutions. Horizontal axis was left standing time. Carbon-support in the mixed solution after added the Pt precursor was precipitated by centrifugation. The supernatant solution was measured by ICP-OES. Concentrations of additional NaOH were 0, 5, and 10 mM. (b) TEM image of carbon-supported Pd@Pt core–shell nanoparticles. The synthesis conditions of Pd nanoparticles were Na2[PdCl4] (2 mM) and NaOH (10 mM). The molar ratio of Na2[PdCl4] : H2[PtCl6]·6H2O was 1 : 1, and additional NaOH concentration was 10 mM. After left standing for 72 h, the mixture of Pd@Pt and single Pt nanoparticles (1–2 nm) was formed on carbon-support. Fig. 4a portrays a TEM image of carbon supported Pd@Pt core–shell nanoparticles. The average particle size of Pd@Pt core–shell nanoparticles was 3.6 nm after being left to stand for 24 h: larger than the initial Pd nanoparticles (3.0 nm). Fig. 4b shows the HAADF-STEM image of Pd@Pt core–shell nanoparticles supported on carbon. The core–shell structure of the particles can be ascertained from the contrast of the image. The Z-contrast image shows the presence of brighter shells over darker cores. Actually, the contrast is strongly dependent on the atomic number (Z) of the element.53 The Z values of Pt (Z = 78) and Pd (Z = 46) differ considerably. Therefore, the image shows the formation of Pd@Pt core–shell structure with the uniform elemental distribution. Elemental mapping images by STEM-EDS show that both Pd and Pt metals were present in all the observed nanoparticles (Fig. 4c). Based on the atomic ratio (Pd : Pt = 49 : 51), they show good agreement with the designed values. The Pt shell thickness was estimated as about 0.6 nm, which corresponds to 2–3 atomic layer thickness of Pt encapsulating the Pd core metal, indicating good agreement with Fig. 4b image. For an earlier study, uniform Pt shells were formed by dropwise injection of the Pt precursor solution because the Pt shell growth rate differs depending on the crystal plane of the Pd nanoparticle.46 For more precise control of shell thickness in our system, the Pt precursor solution should be mixed in multiple steps.Open in a separate windowFig. 4(a) TEM image and (b) HAADF-STEM image of carbon-supported Pd@Pt core–shell nanoparticles and the line profile of contrast. (c) Elemental mapping image of carbon-supported Pd@Pt core–shell nanoparticles, where Pd and Pt elements are displayed respectively as red and green. The EDS atomic ratio of Pd : Pt was 49 : 51. The synthesis conditions of Pd nanoparticles were Na2[PdCl4] (2 mM) and NaOH (10 mM). The molar ratio of Na2[PdCl4] : H2[PtCl6]·6H2O was 1 : 1. The concentration of additional NaOH were 5 mM. It was left standing for 24 h.A comparison of the catalytic performance of the carbon-supported Pd@Pt core–shell and Pt nanoparticles is shown in Fig. S3.† For this experiment, carbon-supported Pt nanoparticles with Pt 2 mM were prepared as a reference catalyst using a similar synthetic method. The initial Pt mass activities of the carbon-supported Pd@Pt and Pt nanoparticles were, respectively, 0.39 and 0.24 A mgPt−1, improving by the core–shell structure. In addition, durability tests for carbon-supported Pd@Pt nanoparticles show that the reduction rate of Pt mass activity after 5000 cycles was only 2%. The catalytic activities of carbon-supported Pd@Pt nanoparticles were superior in terms of durability, suggesting that the Pt shell was firmly formed. 相似文献
14.
Edward P. Randviir Omar Kanou Christopher M. Liauw Gary J. Miller Hayley G. Andrews Graham C. Smith 《RSC advances》2019,9(20):11239
Textile waste is on the rise due to the expanding global population and the fast fashion market. Large volumes of textile waste are increasing the need for new methods for recycling mixed fabric materials. This paper employs a hydrothermal conversion route for a polyester/cotton mix in phosphoric acid to generate carbon materials (hydrochars) for electrochemical applications. A combination of characterization techniques revealed the reaction products were largely comprised of two major components. The first is a granular material with a surface C : O ratio of 2 : 1 interspersed with phosphorous and titanium proved using energy dispersive X-ray spectroscopy, and the other is a crystalline material with a surface C : O ratio of 3 : 2 containing no phosphorous or titanium. The latter material was found via X-ray diffraction and differential scanning calorimetry to be terephthalic acid. Electrochemical experiments conducted using the hydrochar as a carbon paste electrode demonstrates an increase in current response compared to carbon reference materials. The improved current responses, intrinsically related to the surface area of the material, could be beneficial for electrochemical sensor applications, meaning that this route holds promise for the development of a cheap recycled carbon material, using straightforward methods and simple laboratory reagents.A novel method for chemically processing blended textiles is investigated, revealing a conductive carbon material as a major product. 相似文献
15.
Tatsuki Nagata Kanji Okada Ryota Kondo Takashi Toyao Ken-ichi Shimizu Takeyuki Suzuki Yasushi Obora 《RSC advances》2022,12(26):16599
N,N-Dimethylformamide-stabilized Ru nanoparticles (NPs) provide a highly efficient catalyst for the Guerbet reaction of primary alcohols. DMF-modified Ru NPs were synthesized, and characterized by transition electron microscopy, and X-ray absorption spectroscopy, X-ray photoelectronspectroscopy, and Fourier-transform infrared spectroscopy. The Ru NP catalyst was highly durable during catalytic reactions under external additive/solvent-free conditions. N,N-Dimethylformamide-stabilized Ru nanoparticles (NPs) provide a highly efficient catalyst for the Guerbet reaction of primary alcohols under solvent-free conditions and without the use of external ligands. 相似文献
16.
Zheng Li Zijian He Xiaodan Chen Yi Tang Shiwen You Yufang Chen Tao Jin 《RSC advances》2019,9(43):24659
This paper reports on the hydrophobic modification of cotton fabric grafted with 1-octadecene via an activators regenerated by electron transfer (ARGET) atom transfer radical polymerization (ATRP) mechanism. Particularly, the activation treatment of raw cotton fabric, its influence on the graft-copolymerization by the ARGET-ATRP method, along with the super-hydrophobicity and hydrophobic stability of the modified cotton fabric are discussed. Furthermore, the microstructure and elemental variation were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), and the energy dispersion spectrum (EDS) technique. The results show that chemical activation of the raw cotton fabric can significantly improve the follow-up hydrophobic modification process. Specifically, the contact angle of the hydrophobically modified cotton fabric increased to 145° after activation, and thus, this fabric presents more stable hydrophobicity (corresponding to a 5.5% contact angle attenuation) than a non-activated fabric. The hydrophobic modification reaction was carried out using a chemically optimum stoichiometric ratio of m(CuBr2) : m(C9H23N3) : m(C2H5OH) : m(C18H36) : m(C6H8O6) = 0.015 : 0.052 : 17.9 : 2.4 : 0.05, at a temperature of 30–55 °C over 8 h. Furthermore, the SEM and AFM images revealed that more copolymer micro/nano-level particles were present on the surface of the fibers of the hydrophobically modified cotton fabric, indicating that the hydrophobic property and stability of the cotton fabric increase with the grafting density on the cotton fabric.This paper reports on the hydrophobic modification of cotton fabric grafted with 1-octadecene via an electron transfer (ARGET) atom transfer radical polymerization (ATRP) mechanism. 相似文献
17.
Fereshteh Dehghani Sanij Prabhuraj Balakrishnan Huaneng Su Lindiwe Khotseng Qian Xu 《RSC advances》2021,11(62):39118
Designing advanced nanocatalysts for effectively catalyzing the oxygen reduction reaction (ORR) is of great importance for practical applications of direct methanol fuel cells (DMFCs). In this work, the reduced graphene oxide (rGO)-supported palladium–nickel (Pd–Ni/rGO) alloy modified by the novel polyoxometalate (POM) with Keggin structure (Pd–Ni/rGO-POM) is efficiently fabricated via an impregnation technique. The physical characterizations such as X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy, inductively coupled plasma optical emission spectroscopy (ICP-OES), field emission scanning electron microscopy coupled with energy dispersive X-ray spectroscopy (FESEM-EDX), and transmission electron microscopy (TEM) are utilized to confirm the structure, morphology, and chemical composition of the fabricated samples. The XRD results verify the formation of the POM-modified Pd8Ni2/rGO alloy electro-catalyst with the face-centered-cubic (fcc) structure and average crystallite size of 5.54 nm. The electro-catalytic activities of the nanocatalysts towards ORR in alkaline conditions are evaluated by cyclic voltammetry (CV), rotating disk electrode (RDE), and chronoamperometry (CA) analyses. The synthesized Pd8Ni2/rGO-POM nanomaterial shows remarkably greater ORR catalytic activity and better methanol resistance compared with the Pd8Ni2/rGO and Pd/rGO electro-catalysts. The promoted ORR activity of the Pd8Ni2/rGO-POM sample is attributed to the alloying of Pd and Ni components, the uniform scattering of Pd–Ni nanoparticles on rGO, and the alloyed catalyst being modified with POM. Moreover, these findings demonstrate that the resultant Pd8Ni2/rGO-POM material is attractive as a suitable and cost-effective cathodic catalyst for DMFCs, in which the decorated POMs play a vital role for the enhancement in the catalytic abilities of the nanocatalyst.A novel nanocatalyst, polyoxometalate-modified palladium–nickel/reduced graphene oxide (Pd8Ni2/rGO-POM), is prepared and served as an effective ORR nanomaterial in alkaline media. 相似文献
18.
Three cubic crystalline icosahedral approximants (C phase: Al72.0Pd16.4Fe11.6, P40 phase: Al72.0Pd16.4Ru11.6, P20 phase: Al70.0Pd22.3Ru7.7) exhibit high ethylene selectivity of over 90% for hydrogenating acetylene at 150 °C. Moreover, the powdered P20 also demonstrates a high catalytic performance under an industry-like ethylene feed containing 0.5% acetylene as an impurity. Overall, icosahedral approximants in the Al–Pd–(Ru, Fe) systems are promising as a novel class of alloy catalysts.The Al–Pd–(Ru, Fe) icosahedral approximants exhibited high catalytic ethylene selectivity and stability for semi-hydrogenation of acetylene. 相似文献
19.
Zhiyang Zhang Jiayi Sheng Miaomiao Zhang Xiaoyan Ma Zhirong Geng Zhilin Wang 《RSC advances》2018,8(39):22216
NaGdF4:Yb3+/Er3+ nanoparticles were synthesized via a modified hydrothermal route. The dependence of structure and morphology on the dosage of sodium polyacrylate was studied by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The as-prepared nanoparticles could be used for T2 weighted magnetic resonance imaging due to the paramagnetism of Gd3+. cis-dichlorodiamineplatinum (CDDP) could be loaded onto NaGdF4:Yb3+/Er3+ nanoparticles through binding carboxyl in the form of Pt–O bonds, and doxorubicin (DOX) could be loaded via hydrogen bonding. DOX could also be loaded onto the NaGdF4–CDDP composite in the same manner, and the loading efficiency of both drugs remained unchanged. Three as-prepared drug delivery systems were used for tumor inhibition both in vitro and in vivo, and the results indicated that NaGdF4–CDDP–DOX displayed the greatest inhibitory capacity.The drug delivery system NaGdF4–CDDP–DOX showed best tumor inhibition capacity both in vitro and in vivo. 相似文献
20.
Coal bottom ash (CBA) was modified on the basis of the engineering problems of low resource utilization of CBA and difficulty in treating HMS through alkali activation to synthesize geopolymers and solidify heavy metal-contaminated soil (HMS). The optimal values of geopolymers were selected through response surface methodology. Their mineral compositions, microstructure, and binding energy were determined through X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electron microscopy tests, respectively. The stress–strain curve, the leaching concentration and fraction of heavy metals, and the solidifying mechanism for remolded soil were determined through unconfined compressive strength, leaching toxicity, sequential chemical extraction, and infrared (IR) spectroscopy tests, respectively. Based on these experiments, the following conclusions were presented. The optimum ratios of CBA-based geopolymers were n(Si) : n(Al) = 2.666, n(Na) : n(Al) = 0.687, and n(water) : n(binder) = 2.422. The X-ray curves of the geopolymers were obvious hump-like protuberances at diffraction angles of 20–35° and had a dense amorphous structure on the surface. The maximum binding energies of Si 2p and Al 2p decreased to 101.03 and 72.89 eV, respectively. A 3D network polymerized because of strong geopolymerization. The maximum axial stress of the remolded soil was 104.91% higher than that of the undisturbed soil, and the leaching concentration decreased by more than 45.88%. The leaching toxicity met the requirements of standard GB 5085.3-2007. The proportion of the acid-extractable fraction of heavy metals in the remolded soil decreased, whereas the proportion of residual fraction increased. The stretching vibration of Si–O–Si (Al) and the bending vibration of Si–O–Si appeared in the IR spectrum. The soil particles were completely encapsulated by a hardened geopolymer structure, thereby forming a multilayer space-skeleton barrier structure that could greatly improve the mechanical properties.Coal bottom ash (CBA) was modified on the basis of the engineering problems of low resource utilization of CBA and difficulty in treating HMS through alkali activation to synthesize geopolymers and solidify heavy metal-contaminated soil (HMS). 相似文献