Irradiation Reduction Method Research Articles

Coordination engineering of defective F and N co-doped carbon dots anchored silver nanoparticles for boosting oxygen reduction reaction

The carbon-based catalysts exhibit excellent electrocatalytic and stable performance toward oxygen reduction reaction (ORR), which are expected to replace expensive and scarce Pt-based catalysts. However, how to regulate the interaction between silver and carrier carbon dots (CD) to improve electrocatalytic performance toward oxygen reduction reaction (ORR) and stability, has not been systematically studied. In this study, we in-situ synthesized fluorine and nitrogen co-doped CD anchoring Ag nanoparticles by UV irradiation reduction method. The peak potential, onset-potential and half-wave potential of F, N-CD@Ag-0.1 are 0.85 V, 1.056 V, and 0.9 V, respectively, indicating outstanding ORR performance. The current density of F, N-CD@Ag-0.1 remains 97.5 % after 50, 000 s, showing more excellent stability than Pt/C. The impressive ORR catalytic activity and stability of F, N-CD@Ag-0.1 could be attributed to the strong anchoring effect of nitrogen-doped CD on Ag. This effect leads to a significant interaction and charge transfer between Ag and CD, thereby enhancing the charge transfer process during the catalytic reaction. This project aims to design a carbon dot/silver composite catalyst with high ORR catalytic performance and favorable stability. The implementation of this project provides good theoretical guidance for the design of carbon nanomaterial-based catalytic systems.

Synthesis of an Ag@AgCl catalyst with amorphous copper as the support and its catalytic performance in the reduction of 4-nitrophenol

The support used in a composite catalyst has an important influence on the catalytic performance of the catalyst. Amorphous metals have good electron-transfer properties and the presence of defect structures on the surface will introduce additional active sites and should be excellent catalyst supports. In this study, an Ag@AgCl composite catalyst with amorphous Cu (a-Cu) as the support is prepared by a two-step precipitation method at room temperature and a light irradiation reduction method. Compared to the Ag@AgCl and a-Cu, the catalytic rate of the Ag@AgCl/a-Cu composite catalytic rate was 2.04 times and 6.69 times faster during the reduction of 4-NP in NaBH4 aqueous solution. The high-performance catalytic efficiency and reusability of Ag@AgCl/a-Cu may be attributed to the synergistic effect between Ag@AgC and amorphous metal elements. This work may provide an effective reference for the synthesis of high activity catalysts using amorphous metals as supports.

Strong Biomimetic Immobilization of Pt-Particle Catalyst on ABS Substrate Using Polydopamine and Its Application for Contact-Lens Cleaning with H2O2.

Polydopamine (PDA)—a known adhesive coating material—was used herein to strongly immobilize a Pt-particle catalyst on an acrylonitrile–butadiene–styrene copolymer (ABS) substrate. Previous studies have shown that the poor adhesion between Pt particles and ABS surfaces is a considerable problem, leading to low catalytic durability for H2O2 decomposition during contact-lens cleaning. First, the ABS substrate was coated with PDA, and the PDA film was evaluated by X-ray photoelectron spectroscopy. Second, Pt particles were immobilized on the PDA-coated ABS substrate (ABS-PDA) using the electron-beam irradiation reduction method. The Pt particles immobilized on ABS-PDA (Pt/ABS-PDA) were observed using a scanning electron microscope. The Pt-loading weight was measured by inductively coupled plasma atomic emission spectroscopy. Third, the catalytic activity of the Pt/ABS-PDA was evaluated as the residual H2O2 concentration after immersing it in a 35,000-ppm H2O2 solution (the target value was less than 100 ppm). The catalytic durability was evaluated as the residual H2O2 concentration after repeated use. The PDA coating drastically improved both the catalytic activity and durability because of the high Pt-loading weight and strong adhesion among Pt particles, PDA, and the ABS substrate. Plasma treatment prior to PDA coating further improved the catalytic durability.

Green synthesis, size control, and antibacterial activity of silver nanoparticles on chitosan films

Silver nanoparticles (AgNPs) synthesized on the surface of chitosan (CS) films using ultraviolet (UV) and natural light irradiation reduction methods were studied. Field-emission scanning electron microscopy revealed that the diameter of some AgNPs synthesized by the UV irradiation reduction method lay in the range of 5–15 nm. These AgNPs were isolated and dispersed on the surface of CS film. Meanwhile, some AgNPs aggregated to form larger cubic and irregular AgNPs with average size of 50–200 nm. Compared with those synthesized via the UV irradiation reduction method, AgNPs synthesized by the natural light irradiation reduction method were found to be much more individually isolated and uniformly dispersed on the CS film surface. The AgNPs synthesized using the natural light irradiation reduction method had spherical shape with average size of 10–30 nm. Thus, the size and morphology of AgNPs on the CS films (CS-AgNPs films) can be controlled by choosing an appropriate irradiation reduction method. The results of antibacterial testing illustrated that the CS-AgNPs films synthesized by both the ultraviolet and natural light irradiation reduction methods exhibited strong antibacterial activity against Escherichia coli.

Preparation of reduced Graphene Oxide (rGO) assisted by microwave irradiation and hydrothermal for reduction methods

Graphite is a natural carbon source that can be used for graphene synthesis because of its abundant availability and relatively low cost. In this research, Graphene Oxide (GO) and reduced Graphene Oxide (rGO) have been prepared through modified Hummers method that uses microwave irradiation and hydrothermal process as reduction methods. This research can be divided into two main steps, i.e. preparation of GO and preparation of rGO. The preparation of GO was done using modified Hummers method that refers to graphite powder oxidation for five days. Then, preparation of rGO was done using two methods, i.e. microwave irradiation for 8 minutes at 1,000 watts and hydrothermal process for 10 hours at 200°C. The characterization of the samples was observed by Fourier-Transform Infrared Spectroscopy (FTIR), X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM) and Ultraviolet-Visible Spectroscopy (UV-Vis). XRD pattern of GO sample shows a peak at 2θ = 10.63°, rGO sample from hydrothermal process at 2θ = 25.94°, and rGO sample from microwave irradiation method at 2θ = 25.94° with low intensity and at 2θ = 10.63° that indicates the presence of GO. IR spectroscopy data shows an absorption peak of aromatic C=C at 1,573 cm-1 that indicates rGO formation. SEM images of GO illustrates a structure of stacked flakes. While the morphology of rGO has a structure of stacked flakes that is more transparent than GO. According to UV-Vis spectroscopy, GO and rGO of samples show absorption peak at λmax = 225 nm and λmax = 274 nm, respectively, which indicates π→π* transition of aromatic C=C bond. Based on the results of this study, the preparation of rGO using modified Hummers that combined with hydrothermal reduction method is more effective than microwave irradiation reduction method.

γ-Ray Irradiation-Derived MnO/rGO Composites for High Performance Lithium Ion Batteries

We report a γ-ray irradiation reduction method to prepare MnO/reduced graphene oxide (rGO) nanocomposite for the anode of lithium ion batteries. γ-Ray irradiation provides a clean way to generate homogeneously dispersed MnO nanoparticles with finely tuned size on rGO surface without the use of surfactant. The MnO/rGO composite enables a fully charge/discharge in 2 min to gain a reversible specific capacity of 546 (mA·h)/g which is 45% higher than the theoretical value of commercial graphite anode.

Influence of pH on performance of sodium phosphinate for decreasing the particle size

ABSTRACTTo clarify the influence of pH on performance of sodium phosphinate (NaPH2O2) for decreasing particle size of Pt nanoparticles, carbon-supported Pt nanoparticles that contained phosphorus (P–Pt/C) were synthesised by an electron-beam irradiation reduction method (EBIRM) under four different pH conditions (pH = 3, 6, 9, and 12) and under five different NaPH2O2 concentrations (0.0, 0.5, 1.0, 3.0, and 5.0 mM). The relationship among pH, NaPH2O2 concentration, average particle size of Pt nanoparticle, and Pt loading weight was investigated in this study. The average particle size of Pt nanoparticles was in the range of 0.8–3.4 nm and lower in the order; pH12 > pH3 > pH6 > pH9; for example, under the same NaPH2O2 concentrations of 3.0 mM, the particle size of P–Pt/C prepared at pH = 12 and pH = 9 was 1.5 and 0.8 nm, respectively. In addition, Pt loading weight was also lower in the order; pH12 > pH3 > pH6 > pH9. In summary, these results indicated that the pH in the precursor solution affected the performance of NaPH2O2. These findings would be useful for controlling the particle size of monometallic Pt and Pt-based bimetallic nanoparticles supported on carbon particles for fuel cell applications.

Synthesis of carbon-supported PtRh random alloy nanoparticles using electron beam irradiation reduction method

Abstract Bimetallic nanoparticle catalysts of PtRh supported on carbon were synthesized using an electron beam irradiation reduction method. The PtRh nanoparticle catalysts were composed of particles 2–3 nm in size, which were well dispersed on the surface of the carbon support nanoparticles. Analyses of X-ray diffraction and scanning transmission electron microscopy–energy-dispersive X-ray spectroscopy revealed that the PtRh nanoparticles have a randomly alloyed structure. The lattice constant of the PtRh nanoparticles showed good correlation with Vegard's law. These results are explained by the radiochemical formation process of the PtRh nanoparticles. Catalytic activities of PtRh/C nanoparticles for ethanol oxidation reaction were found to be higher than those obtained with Pt/C.

Improving photocatalytic Rhodamine B degrading activity with Pt quantum dots on TiO2 nanotube arrays

Well-dispersed Pt quantum dots (QDs) with an average diameter of 2nm were homogeneously decorated on TiO2 nanotube arrays (TNTAs) by a modified photo irradiation–reduction method. The effect of the precursor concentration between 0.3mM and 2.0mM on the decorated Pt QD content was investigated. The synthesized nanostructures with different Pt QD contents were characterized by XRD, SEM, TEM, XPS, UV–vis and PL. The Pt QDs, acting as electron sinks, reduced the recombination of electrons and holes and extended their lifetime, leading to a greatly enhanced photocatalytic performance. In a 1.0mM concentration, the fabricated nanocomposite with excellent durability exhibited favorable photocurrent density and efficiency of degrading Rhodamine B. According to EPR analysis, the corresponding mechanism of the UV-driven photocatalytic process is proposed. Furthermore, the nanocomposite is easier to be recycled compared to the powder catalysts.

Binary and ternary palladium based electrocatalysts for alkaline direct glycerol fuel cell

Pd/C, PdAu/C 50:50, PdSn/C 50:50, PdAuSn/C 50:40:10 and PdAuSn/C 50:10:40 electrocatalysts are prepared using an electron beam irradiation reduction method and tested for glycerol electro-oxidation in alkaline medium. X-Ray diffraction (XRD), Energy dispersive X-ray analysis (EDX), Transmission electron Microscopy (TEM) and Cyclic Voltammetry (CV) are used to characterize the resulting materials. The activity for glycerol electro-oxidation is tested in alkaline medium at room temperature using Cyclic Voltammetry and Chronoamperometry (CA) and in a single alkaline direct glycerol fuel cell (ADGFC) at temperature range of 60–90 °C. EDX analysis demonstrate that Pd:Au:Sn atomic ratios are very similar to the nominal ones. X-ray diffractograms of PdAuSn/C electrocatalysts evidence the presence of Pd (fcc), Au (fcc) and SnO2 phases. TEM analysis demonstrates a good dispersion of the nanoparticles on the carbon support with some agglomerates. Cyclic Voltammetry experiments suggest that PdAuSn/C electrocatalysts demonstrate better results. In single fuel cell tests, at 85 °C, using 2.0 mol L−1 glycerol in 2.0 mol L−1 KOH solutions, the electrocatalyst PdAuSn/C 50:40:10 demonstrate highest power density (51 mW cm−2) and the 120 h durability tests demonstrate a 210 μV h−1 degradation rate.

Mass production of highly loaded and highly dispersed PtRu/C catalysts for methanol oxidation using an electron-beam irradiation reduction method

An electron-beam irradiation reduction method (EBIRM) is a technique to reduce metal ions in an aqueous solution via irradiation with a high-energy electron beam. In this study, an EBIRM is improved to develop a technique for the mass production of highly loaded and highly dispersed PtRu/C catalysts for use as direct methanol fuel cell anodes. An increase in the Pt and Ru input concentrations increased the loading weight from 9 to 37 wt%; however, the dispersibility of the PtRu nanoparticles on the carbon particles decreased. To improve the low dispersibility, sodium phosphinate was added to the precursor solution and the input amount of carbon particles was decreased. These changes resulted in not only highly loaded but also highly dispersed PtRu/C catalysts. The catalytic activity of the highly loaded and highly dispersed PtRu/C catalysts for methanol oxidation was at least 1.6 times higher than that of the lowly loaded and lowly dispersed PtRu/C catalysts in all voltage range. More than 6000 mg of highly loaded and highly dispersed PtRu/C catalysts were relatively easily obtained, and the average particle size of the PtRu nanoparticles was 1.8 nm. These results demonstrated that the improved EBIRM is effective for the mass production of carbon-supported, highly loaded, and highly dispersed metal nanoparticles.

Palladium and palladium–tin supported on multi wall carbon nanotubes or carbon for alkaline direct ethanol fuel cell

Pd and PdSn (Pd:Sn atomic ratios of 90:10), supported on Multi Wall Carbon Nanotubes (MWCNT) or Carbon (C), are prepared by an electron beam irradiation reduction method. The obtained materials are characterized by X-Ray diffraction (XRD), Energy dispersive X-ray analysis (EDX), Transmission electron Microscopy (TEM) and Cyclic Voltammetry (CV). The activity for ethanol electro-oxidation is tested in alkaline medium, at room temperature, using Cyclic Voltammetry and Chronoamperometry (CA) and in a single alkaline direct ethanol fuel cell (ADEFC), in the temperature range of 60–90 °C. CV analysis finds that Pd/MWCNT and PdSn/MWCNT presents onset potentials changing to negative values and high current values, compared to Pd/C and PdSn/C electrocatalysts. ATR-FTIR analysis, performed during the CV, identifies acetate and acetaldehyde as principal products formed during the ethanol electro-oxidation, with low conversion to CO2. In single fuel cell tests, at 85 °C, using 2.0 mol L−1 ethanol in 2.0 mol L−1 KOH solutions, the electrocatalysts supported on MWCNT, also, show higher power densities, compared to the materials supported on carbon: PdSn/MWCNT, presents the best result (36 mW cm−2). The results show that the use of MWCNT, instead of carbon, as support, plus the addition of small amounts of Sn to Pd, improves the electrocatalytic activity for Ethanol Oxidation Reaction (EOR).

Synthesis of Cu nanoparticles using gamma-ray irradiation reduction method

Nanometer size pure copper particles have been synthesized by gamma-ray irradiation reduction method. The solutions containing 0.5 mM copper acetate and 10 mM sodium dodecyl sulfate (SDS), 0 or 8.5 vol % diethylene glycol (DEG) were prepared. They were irradiated by gamma-ray from 60Co radioactive source with the dose rate of 4.70 kGy/h and the total dose of 20.0 kGy. After gamma-ray irradiation, in solution without DEG, the absorption peaks of Cu and CuO nanoparticles were observed in UV/visible (vis) spectrum. On the other hand, in solution with DEG, the production of Cu oxide nanoparticles is decreased. Consequently, Cu and Cu2O nanoparticles were generated. The mean particle sizes of generated nanoparticles without and with DEG are about 13 and 17 nm, respectively. Furthermore, by adding DEG into the solution, more monodispersed Cu nanoparticles were generated.

Effect of decrease in the size of Pt nanoparticles using sodium phosphinate on electrochemically active surface area

Carbon-supported Pt nanoparticles that contained phosphorus (P–Pt/C) were synthesized by the reduction of Pt ions in an aqueous solution via irradiation with a high-energy electron beam; this synthesis technique is referred to as the electron beam irradiation reduction method (EBIRM). To decrease the size of the Pt nanoparticles supported on the carbon particles, sodium phosphinate (NaPH2O2) was added as a phosphorus precursor to the precursor solution that contained Pt ions. The P–Pt/C samples were observed using a transmission electron microscope. The average particle size of the Pt nanoparticles decreased as the NaPH2O2 concentration in the precursor solution increased. The average particle size was in the range 0.9–3.4 nm. The electrochemically active surface areas (ECSAs) of Pt were estimated using cyclic voltammetry. In contrast to the average particle size, the ECSAs increased as the NaPH2O2 concentration was increased. The decrease in the size of the Pt nanoparticles using NaPH2O2 effectively increased the ECSA. This result indicated that the EBIRM combined with the use of NaPH2O2 to decrease the particle size is a useful and simple tool for the preparation of Pt nanoparticle catalysts with a high specific activity.

Radiolytic synthesis of carbon-supported PtRu nanoparticles using high-energy electron beam: effect of pH control on the PtRu mixing state and the methanol oxidation activity

Electrode catalysts composed of carbon-supported PtRu nanoparticles (PtRu/C) for use as a direct methanol fuel cell anode were synthesized by the reduction of precursor ions in an aqueous solution via irradiation with a high-energy electron beam. The effect of pH control in the precursor solution on the PtRu mixing state and the methanol oxidation activity was studied in order to enhance the catalytic activity for methanol oxidation. The PtRu/C structures were characterized by transmission electron microscopy, inductively coupled plasma atomic emission spectrometry, X-ray fluorescence spectrometry, and X-ray diffraction and X-ray absorption fine structure techniques. The methanol oxidation activity was evaluated by linear sweep voltammetry. The initial pH of the precursor solution has little influence on the average grain size for the metal particles (approximately 3.5 nm) on the carbon particle supports, but the dispersibility of the metal particles, PtRu mixing state, and methanol oxidation activity differed. The maintenance of a low pH in the precursor solution gave the best dispersibility of the PtRu nanoparticles supported on the surface of the carbon particles, whereas, a high pH gave the best PtRu mixing state and the highest oxidation current although a low dispersibility of the PtRu nanoparticles supported on the surface of the carbon particles was obtained. The PtRu mixing state strongly correlated with the methanol oxidation current. In addition, a high pH was more effective for PtRu mixing when using an electron beam irradiation reduction method, because the complexation reaction of the chelating agents was improved, which resulted in an enhancement of the catalytic activity for methanol oxidation.

Preparation of carbon-supported PtCo nanoparticle catalysts for the oxygen reduction reaction in polymer electrolyte fuel cells by an electron-beam irradiation reduction method

We prepared carbon-supported PtCo bimetallic nanoparticles (PtCo/C) as electrode catalysts for the oxygen reduction reaction (ORR) at the cathodes in polymer electrolyte membrane fuel cells (PEFCs) by an electron-beam irradiation reduction method (EBIRM). An EBIRM allows nanoparticles to be easily prepared by the reduction of precursor ions in an aqueous solution irradiated with a high-energy electron beam. The structures of PtCo/C were characterized by transmission electron microscopy, inductively coupled plasma atomic emission spectrometry, and the techniques of X-ray diffraction and X-ray absorption near edge structure. It found for the first time that both PtCo alloy and Co oxide were prepared simultaneously on the carbon support by an EBIRM. The catalytic activity and durability of PtCo/C were evaluated by linear-sweep voltammetry and cyclic voltammetry, respectively. The addition of Co to Pt/C not only enhanced the catalytic activity for the ORR but also improved the catalytic durability. As the Co concentration increased, both behaviors became pronounced. These improvements are explained by the effects of both PtCo alloy and Co oxide. We demonstrated that an EBIRM can not only synthesize the alloy and oxide simultaneously on the carbon support but also mass-produce the electrode catalysts for PEFC cathodes.

Catalytic Efficiency of Pt-Ru-Mo/MWNT Catalysts Prepared by γ-ray Irradiation and Chemical Reduction Method in Direct Methanol Fuel Cell

Catalytic Efficiency of Pt-Ru-Mo/MWNT Catalysts Prepared by γ-ray Irradiation and Chemical Reduction Method in Direct Methanol Fuel Cell

The Reduction and Luminescence Characteristics of Sm2+ Doped in Ba3BP3O12 Crystal

Sm2+ ions doped in Ba3BP3O12 polycrystalline samples were obtained by heating the materials in a reducing atmosphere and X-ray irradiation reduction method. The phase formations of the samples were investigated by X-ray powder diffraction measurements. The temperature-dependent emission spectra and luminescence decay curves of Sm2+ ions reduced by the two methods were investigated at various temperatures (10–300 K). The crystallographic site distributions and the thermal quenching of 5D0→7F0 luminescence transition of Sm2+ ions in the two samples have different characteristics. The photostabilities of the Sm2+ ions were evaluated with the photobleaching method by monitoring the 5D0→7F0 luminescence transition under the excitation of 488 nm of Ar+ laser. The luminescence and reduction mechanism of Sm3+→Sm2+ were discussed. The luminescence properties and stabilities of the Sm2+ ions are highly dependent on the sample preparation conditions.

Dependence of Property of Silver Nanoparticles within Dendrimer‐template on Molar Ratios of Ag+ to PAMAM Dendrimers

AbstractG5.0‐OH PAMAM dendrimers were used to prepare fluorescent silver clusters with weaker ultraviolet irradiation reduction method, in which the molar ratio of Ag+ to PAMAM dendrimers was the key factor to determine the geometry and properties of silver nanoparticles. The results showed that because of G5.0‐OH PAMAM dendrimers as strong encapsulatores, when the molar ratios of Ag+ to PAMAM dendrimers was smaller than 5, the obtained Agn clusters (n<5) had line structures and "molecular‐like" properties, which were highly fluorescent and quite stable in aqueous solution. Whereas when the molar ratios were between 5 and 8, the obtained Agn clusters were 2D structures and their fluorescence was weaker. When the molar ratio was larger than 8, the structure of silver nanoparticles was 3D and no fluorescence was observed from the obtained silver nanoparticles.

Green synthesis of silver/montmorillonite/chitosan bionanocomposites using the UV irradiation method and evaluation of antibacterial activity.

In this study, silver nanoparticles (Ag-NPs) were synthesized using a green physical synthetic route into the lamellar space of montmorillonite (MMT)/chitosan (Cts) utilizing the ultraviolet (UV) irradiation reduction method in the absence of any reducing agent or heat treatment. Cts, MMT, and AgNO3 were used as the natural polymeric stabilizer, solid support, and silver precursor, respectively. The properties of Ag/MMT/Cts bionanocomposites (BNCs) were studied as the function of UV irradiation times. UV irradiation disintegrated the Ag-NPs into smaller sizes until a relatively stable size and size distribution were achieved. Meanwhile, the crystalline structure and d-spacing of the MMT interlayer, average size and size distribution, surface morphology, elemental signal peaks, functional groups, and surface plasmon resonance of Ag/MMT/Cts BNCs were determined by powder X-ray diffraction, transmission electron microscopy, scanning electron microscopy, energy dispersive X-ray fluorescence, Fourier transform infrared, and UV-visible spectroscopy. The antibacterial activity of Ag-NPs in MMT/Cts was investigated against Gram-positive bacteria, ie, Staphylococcus aureus and methicillin-resistant S. aureus and Gram-negative bacteria (ie, Escherichia coli) by the disk diffusion method on Muller–Hinton Agar at different sizes of Ag-NPs. All of the synthesized Ag/MMT/Cts BNCs were found to have high antibacterial activity. These results show that Ag/MMT/Cts BNCs can be useful in different biologic research and biomedical applications, such as surgical devices and drug delivery vehicles.