Gold/silver bimetallic nanoparticles still attract extensive interest due to their favorable properties e.g. in plasmonics or catalysis. We present here a facile and robust way for the production of clean Au/Ag binary nanoparticles (BNPs) with a total control over the composition via the spark discharge nanoparticle generation technique. With the application of pure Ag and Au electrodes, a tuning range of 55 to 90% Au content was achieved, but this can be further extended to the full 0 to 100% range by using a couple of alloyed electrodes. An added benefit of the approach is that either the concentration or the mean particle size can be kept constant at every composition by adjusting the generator parameters. Based on the systematic experimental data collected, a semi-empirical model for the prediction of the Au/Ag BNP composition was also developed. This model was used to calculate the theoretically achievable Au/Ag composition at a given spark parameter set in the parameter range most commonly used in the literature.
Spark discharge nanoparticle generation is a dynamically developing application of discharge plasmas. In the present study a spark plasma used for nanoparticle generation is characterized by means of spatially and temporally resolved optical emission spectroscopy (OES) supplemented by fast imaging. The data acquired during the generation of copper nanoparticles in argon ambient is used to describe the spatial and temporal evolution of the species in the spark gap and to derive plasma parameters such as excitation temperature and electron concentration on one hand, and the concentration of the Cu species eroded by a single spark on the other. It is shown that temporally and spatially resolved OES together with a simple equilibrium model are efficient tools to estimate the characteristics of the spark discharge plasma that typically exists in spark discharge nanoparticle generators.
A time-resolved laser induced fluorescence study on the ion velocity distribution function in a Hall thruster after a fast current disruption Phys. Plasmas 16, 043504 (2009) We present a time-resolved imaging and electrical study of an atmospheric pressure spark discharge. The conditions of the present study are those used for nanoparticle generation in spark discharge generator setups. The oscillatory bipolar spark discharge was generated between two identical Cu electrodes in different configurations (cylindrical flat-end or tipped-end geometries, electrode gap from 0.5 to 4 mm), in a controlled co-axial N 2 flow, and was supplied by a high voltage capacitor. Imaging data with nanosecond time resolution were collected using an intensified CCD camera. This data were used to study the time evolution of plasma morphology, total light emission intensity, and the rate of plasma expansion. High voltage and high current probes were employed to collect electrical data about the discharge. The electrical data recorded allowed, among others, the calculation of the equivalent resistance and inductance of the circuit, estimations for the energy dissipated in the spark gap. By combining imaging and electrical data, observations could be made about the correlation of the evolution of total emitted light and the dissipated power. It was also observed that the distribution of light emission of the plasma in the spark gap is uneven, as it exhibits a "hot spot" with an oscillating position in the axial direction, in correlation with the high voltage waveform. The initial expansion rate of the cylindrical plasma front was found to be supersonic; thus, the discharge releases a strong shockwave. Finally, the results on equivalent resistance and channel expansion are comparable to those of unipolar arcs. This shows the spark discharge has a similar behavior to the arc regime during the conductive phase and until the current oscillations stop. V C 2015 AIP Publishing LLC. [http://dx
The increased demand for high purity nanoparticles (NPs) of defined geometry necessitates the continuous development of generation routes. One of the most promising physical techniques for producing metal, semiconductor or alloy NPs in the gas phase is spark discharge NP generation. The technique has a great potential for up-scaling without altering the particles. Despite the simplicity of the setup, the formation of NPs in a spark discharge takes place via complex multi-scale processes, which greatly hinders the investigation via conventional NP measurement techniques. In the present work, time-resolved optical emission spectroscopy (OES) was used to provide information on the species present in the spark from as early as approximately 100 ns after the initiation of the discharge. We demonstrate that operando emission spectroscopy can deliver valuable insights into NP formation. The emission spectra of the spark are used to identify, among others, the main stages of material erosion and to calculate the quenching rate of the generated metal vapour. We demonstrate that the alteration of key control parameters, that are typically used to optimize NP generation, clearly affect the emission spectra. We report for Cu and Au NPs that the intensity of spectral lines emitted by metal atoms levels off when spark energy is increased above an energy threshold, suggesting that the maximum concentration of metal vapour produced in the generator is limited. This explains the size variation of the generated NPs. We report a strong correlation between the optical and particle emission of the spark discharge generator, which demonstrate the suitability of OES as a valuable characterization tool that will allow for the more deliberate optimization of spark-based NP generation.
The present review attempts to comprehensively overview the progress in the field of nanoparticle-related analytical laser and plasma spectroscopy research, focusing on the results of the past decade. The discussion...
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