Fast synthesis of gold nanoparticles by cold atmospheric pressure plasma jet in the presence of Au^(+) ions and a capping agent

Homogeneous gold nanoparticles were synthesized under atmospheric pressure using a nonthermal helium plasma jet in a single-step process.A current power supply was used to generate the plasma discharge rich in diverse reactive species.These species induce rapid chemical reactions responsible for the reduction of the gold salts upon contact with the liquid solution.In this study,spherical and monodispersed gold nanoparticles were obtained within 5 min of plasma exposure using a solution containing gold(Ⅲ)chloride hydrate(HAuCl_(4))as a precursor and polyvinylpyrrolidone(PVP)as a capping agent to inhibit agglomerations.The formation of these metal nanoparticles was initially perceptible through a visible change in the sample's color,transitioning from light yellow to a red/pink color.This was subsequently corroborated by UVvis spectroscopy,which revealed an optical absorption in the 520-550 nm range for Au NPs,corresponding to the surface plasmon resonance(SPR)band.An investigation into the impact of various parameters,including plasma discharge duration,precursor and capping agent concentrations,was carried out to optimize conditions for the formation of well-separated,spherical gold nanoparticles.Dynamic light scattering(DLS)was used to measure the size of these nanoparticles,transmission electron microscopy(TEM)was used to observe their morphology and X-ray diffraction(XRD)was also employed to determine their crystallographic structure.The results confirm that homogeneous spherical gold nanoparticles with an average diameter of 13 nm can be easily synthesized through a rapid,straightforward,and environmentally friendly approach utilizing a helium atmospheric pressure plasma.

Transition from a filamentary mode to a diffuse one with varying distance from needle to stream of an argon plasma jet

Plasma jet has extensive application potentials in various fields, which normally operates in a diffuse mode when helium is used as the working gas. However, when less expensive argon is used, the plasma jet often operates in a filamentary mode. Compared to the filamentary mode, the diffuse mode is more desirable for applications. Hence, many efforts have been exerted to accomplish the diffuse mode of the argon plasma jet. In this paper, a novel single-needle argon plasma jet is developed to obtain the diffuse mode. It is found that the plasma jet operates in the filamentary mode when the distance from the needle tip to the central line of the argon stream(d) is short. It transits to the diffuse mode with increasing d. For the diffuse mode, there is always one discharge pulse per voltage cycle, which initiates at the rising edge of the positive voltage. For comparison, the number of discharge pulse increases with an increase in the peak voltage for the filamentary mode. Fast photography reveals that the plasma plume in the filamentary mode results from a guided positive streamer,which propagates in the argon stream. However, the plume in the diffuse mode originates from a branched streamer, which propagates in the interfacial layer between the argon stream and the surrounding air. By optical emission spectroscopy,plasma parameters are investigated for the two discharge modes, which show a similar trend with increasing d. The diffuse mode has lower electron temperature, electron density, vibrational temperature, and gas temperature compared to the filamentary mode.

Different bactericidal abilities of plasma-activated saline with various reactive species prepared by surface plasma-activated air and plasma jet combinations

Plasma-activated water(PAW),as an extended form of cold atmospheric-pressure plasma,greatly expands the application of plasma-based technology.The biological effects of PAW are closely related to the aqueous reactive species,which can be regulated by the activation process.In this study,surface plasma-activated air(SAA)and a He+O_(2)plasma jet(Jet)were parallelly combined(the SAA+Jet combination)or sequentially combined(the SAA→Jet combination and the Jet→SAA combination)to prepare plasma-activated saline(PAS).The PAS activated by the combinations exhibited stronger bactericidal effects than that activated by the SAA or the Jet alone.The concentrations of H_(2)O_(2)and NO_(2)^(-)were higher in the PAS activated by the Jet→SAA combination,while ONOO^(-)concentrations were close in the three kinds of PAS and^(1)O_(2)concentrations were higher in the PAS activated by the SAA+Jet combination.The analysis of scavengers also demonstrated that H_(2)O_(2),^(1)O_(2),and ONOO^(-)in the PAS activated by the SAA+Jet combination,and^(1)O_(2)in the PAS activated by the Jet→SAA combination played critical roles in bactericidal effects.Further,the effective placement time of the three PAS varied,and the PAS activated by the Jet→SAA combination could also inactivate 2.6-log_(10)of MRSA cells after placement for more than 60 min.The regulation of reactive species in plasma-activated water via different combinations of plasma devices could improve the directional application of plasma-activated water in the biomedical field.

A large-scale cold plasma jet: generation mechanism and application effect

Atmospheric pressure cold plasma jets(APCPJs) typically exhibit a slender, conical structure,which imposes limitations on their application for surface modification due to the restricted treatment area. In this paper, we introduce a novel plasma jet morphology known as the large-scale cold plasma jet(LSCPJ), characterized by the presence of both a central conical plasma jet and a peripheral trumpet-like diffuse plasma jet. The experimental investigations have identified the factors influencing the conical and the trumpet-like diffuse plasma jet, and theoretical simulations have shed light on the role of the flow field and the electric field in shaping the formation of the LSCPJ. It is proved that, under conditions of elevated helium concentration, the distributions of impurity gas particles and the electric field jointly determine the plasma jet’s morphology. High-speed ICCD camera images confirm the dynamic behavior of plasma bullets in LSCPJ, which is consistent with the theoretical analysis. Finally, it is demonstrated that when applied to the surface treatment of silicone rubber, LSCPJ can achieve a treatment area over 28 times larger than that of APCPJ under equivalent conditions. This paper uncovers the crucial role of impurity gases and electric fields in shaping plasma jet morphology and opens up the possibility of efficiently diversifying plasma jet generation effects through external electromagnetic fields. These insights hold the promise of reducing the generation cost of plasma jets and expanding their applications across various industrial sectors.

Influence of bias voltage and oxygen addition on the discharge aspects of a diffuse argon plume in an atmospheric pressure plasma jet

A remote plasma,also referred to as a plasma plume(diffuse or filamentary),is normally formed downstream of an atmospheric pressure plasma jet.In this study,a diffuse plume is formed by increasing the bias voltage(U_(b))applied to the downstream electrode of an argon plasma jet excited by a negatively pulsed voltage.The results indicate that the plume is filamentary when U_(b)is low,which transits to the diffuse plume with increasing U_(b).The discharge initiated at the rising edge of the pulsed voltage is attributed to the diffuse plume,while that at the falling edge contributes to the filament in the plume.For the diffuse plume,the discharge intensity decreases with the increasing oxygen content(C_o).Fast photography reveals that the diffuse plume results from a negative streamer,which has a dark region near the nozzle with C_o=0%.However,the dark region is absent with C_o=0.5%.From the optical emission spectrum,the electron density,electron excitation temperature,gas temperature,and oxygen atom concentration are investigated.

Polyvinyl alcohol–potassium iodide gel probe to monitor the distribution of reactive species generation around atmospheric-pressure plasma jet

This study proposes polyvinyl alcohol–potassium iodide(PVA–KI)as a novel gel chemical probe.The probe uses the reactions among PVA,KI,water,borax,and oxidative species to visualize the distribution of reactive species.This method provides information regarding the distribution of reactive species by coloration on the gel surface.The effects of the surrounding gas phase on the distribution and diffusion of the reactive species are also investigated using the PVA–KI gel probe.Further,the relationship between the irradiation distance and reactive species diffusion is determined on the surface of the PVA–KI probe with and without plastic shielding.Adjusting the irradiation distance appropriately leads to an increase in the modified area as detected by the PVA–KI gel probe analysis.The relative concentration distributions of the reactive species are also obtained from visualized color distributions measured using a colorimeter.Furthermore,reactive species generation by long-scale line plasma is confirmed by the color reaction on the PVA–KI gel surface,with a greater area being covered by an atmospheric-pressure pulsed microwave line plasma source.

采用DC Arc Plasma JetCVD方法沉积微/纳米复合自支撑金刚石膜

在30kW级直流电弧等离子体喷射化学气相沉积(DC Arc P lasm a Jet CVD)设备上,采用Ar-H2-CH4混合气体,通过调节甲烷浓度以及控制其他沉积参数,在Mo衬底上沉积出微/纳米复合自支撑金刚石膜。实验表明,当微米金刚石膜层沉积结束后,在随后的沉积中,随着甲烷浓度的增加,金刚石膜表面的晶粒大小是逐渐减小的。当甲烷浓度达到20%以上时,金刚石膜生长面晶粒呈现菜花状的小晶团,膜体侧面已经没有了粗大的柱状晶,而是呈现出光滑的断口,对该层进行拉曼谱分析显示,位于1145 cm-1附近有一定强度的散射峰出现。这说明所沉积的晶粒全部变为纳米级尺寸。

Bacteria Inactivation Using DBD Plasma Jet in Atmospheric Pressure Argon

A coaxial dielectric barrier discharge plasma jet was designed, which can be operated in atmospheric pressure argon under an intermediate frequency sinusoidal resonant power supply, and an atmospheric pressure glow-like discharge was achieved. Two kinds of typical bacteria, i.e., the Staphylococcus aureus （S. aureus） and Escherichia coil （E. coil）, were employed to study the bacterial inactivation mechanism by means of the non-thermal plasma. The killing log value （KLV） of S. aureus reached up to 5.38 with a treatment time of 90 s and that of E. coil up to 5.36 with 60 s, respectively. According to the argon emission spectra of the plasma jet and the scanning electron microscope （SEM） images of the two bacteria before and after the plasma treatment, it is concluded that the reactive species in the argon plasma played a major role in the bacterial inactivation, while the heat, electric field and UV photons had little effect.

Two-dimensional numerical study of an atmospheric pressure helium plasma jet with dual-power electrode

In this paper, the characteristics of an atmospheric pressure helium plasma jet generated by a dual-power electrode （DPE） configuration are investigated by using a two-dimensional fluid model. The effect of a needle electrode on the discharge is studied by comparing the results of the DPE configuration with those of the single ring electrode configuration. It is found that the existence of the needle leads to the generation of a helium plasma jet with a higher propagation velocity, higher species density, and larger discharge width. Furthermore, the influences of the needle radius and needle-to-ring discharge gap on the generation of a plasma jet are also studied. The simulation results indicate that the needle electrode has an evident influence on the plasma jet characteristics.

The influence of grounded electrode positions on the evolution and characteristics of an atmospheric pressure argon plasma jet

An atmospheric pressure plasma jet（APPJ） in Ar with various grounded electrode arrangements is employed to investigate the effects of electrode arrangement on the characteristics of the APPJ.Electrical and optical methods are used to characterize the plasma properties.The discharge modes of the APPJ with respect to applied voltage are studied for grounded electrode positions of 10 mm,40 mm and 80 mm,respectively,and the main discharge and plasma parameters are investigated.It is shown that an increase in the distance between the grounded electrode and high-voltage electrode results in a change in the discharge modes and discharge parameters.The discharges transit from having two discharge modes,dielectric barrier discharge（DBD） and jet,to having three,corona,DBD and jet,with increase in the distance from the grounded to the high-voltage electrodes.The maximum length of the APPJ reaches 3.8 cm at an applied voltage of 8 kV.The discharge power and transferred charges and spectral line intensities for species in the APPJ are influenced by the positions of the grounded electrode,while there is no obvious difference in the values of the electron excited temperature（EET） for the three grounded electrode positions.

Three modes of a direct-current plasma jet operated underwater to degrade methylene blue

A direct-current air plasma jet operated underwater presents three stable modes including an intermittently-pulsed discharge, a periodically-pulsed discharge and a continuous discharge with increasing the power voltage. The three discharge modes have different appearances for the plasma plumes. Moreover, gap voltage-current characteristics indicate that the continuous discharge is in a normal glow regime. Spectral lines from reactive species（OH, N2, N2^＋, Hα,and O） have been revealed in the emission spectrum of the plasma jet operated underwater.Spectral intensities emitted from OH radical and oxygen atom increase with increasing the power voltage or the gas flow rate, indicating that reactive species are abundant. These reactive species cause the degradation of the methylene blue dye in solution. Effects of the experimental parameters such as the power voltage, the gas flow rate and the treatment time are investigated on the degradation efficiency. Results indicate that the degradation efficiency increases with increasing the power voltage, the gas flow rate or the treatment time. Compared with degradation in the intermittently-pulsed mode or the periodically-pulsed one, it is more efficient in the continuous mode, reaching 98% after 21 min treatment.

Study on an Atmospheric Pressure Plasma Jet and its Application in Etching Photo-Resistant Materials

An atmospheric pressure radio-frequency plasma jet that can eject cold plasma has been developed. In this paper, the configuration of this type of plasma jet is illustrated and its discharge characteristics curves are studied with a current and a voltage probe. A thermal couple is used to measure the temperature distribution along the axis of the jet stream. The temperature distribution curve is generated for the He/O-2 jet stream at the discharge power of 150 W. This jet can etch the photo-resistant material at an average rate of 100 nm/min on the surface of silicon wafers at a right angle.

Atmospheric Pressure Plasma Jet in Ar and O_2/Ar Mixtures:Properties and High Performance for Surface Cleaning

An atmospheric pressure plasma jet generated in Ar and O2/Ar mixtures has been investigated by specially designed equipment with double power electrodes at 20~32 kHz, and their effects on the cleaning of surfaces have been studied. Properties of the jet discharge are studied by electrical diagnostics, including the waveform of discharge voltage, discharge current and the Q-V Lissajous figures. The optical emission spectroscopy is used to measure the plasma parameters, such as the excitation temperature and the gas temperature. It is found that the consumed power and the excitation temperature increase with increase of the discharge frequency. On the other hand, at the same discharge frequency, these parameters in O2/Ar mixture plasma are found to be much larger. The effect on surface cleaning is studied from the changes in the contact angle. For Ar plasma jet, the contact angle decreases with increase of the discharge frequency. For O2/Ar mixture plasma jet, the contact angle decreases with increase of discharge frequency up to 26 kHz, however, further increase of discharge frequency does not show further decrease in the contact angle. At the same discharge frequency, the contact angle after O2/Ar mixture plasma cleaning is found to be much lower compared to the case of pure Ar. From the results of quadrupole mass-spectrum analysis, we can identify more fragment molecules of CO and H2O in the emitted gases after O2/Ar plasma jet treatment compared with Ar plasma jet treatment, which are produced by the decomposition of surface organic contaminants during the cleaning process.

The Interactions of Two Cold Atmospheric Plasma Jets

This paper presents the interactions between two cold atmospheric plasma jets. By changing the experimental conditions including the gas flow rate, the applied voltage, the power supply frequency and the inter-electrode distance d, three different interaction modes, attraction, repulsion and combination, were observed. It is shown that the interaction modes of the two jets are principally affected by the electrodes, the gas flow rate, the plasma jets and the power supply frequency.

Arc Voltage Fluctuation in DC Laminar and Turbulent Plasma Jets Generation

Arc voltage fluctuations in a direct current （DC） non-transferred arc plasma generator are experimentally studied, in generating a jet in the laminar, transitional and turbulent regimes. The study is with a view toward elucidating the mechanism of the fluctuations and their relationship with the generating parameters, arc root movement and flow regimes. Results indicate that the existence of a 300 Hz alternating current （AC） component in the power supply ripples does not cause the transition of the laminar plasma jet into a turbulent state. There exists a high frequency fluctuation at 4 kHz in the turbulent jet regime. It may be related to the rapid movement of the anode attachment point of the arc.

Bacterial-killing Effect of Atmospheric Pressure Non-equilibrium Plasma Jet and Oral Mucosa Response

Recently, plasma sterilization has attracted increasing attention in dental community ibr the atmospheric pressure non-equilibrium plasma jet （APNPs）, which is driven by a kilohertz pulsed DC power, may be applied to the dental and oral diseases. However, it is still in doubt whether APNPs can effectively kill pathogenic bacteria in the oral cavity and produce no harmful effects on normal oral tissues, especially on normal mucosa. The aim of this study was to evaluate the bacterial-killing effect of APNPs in the biofilms containing a single breed of bacteria （Porphyromonas gingivalis, Pg.）, and the pathological changes of the oral mucosa after treatment by APNPs. P.g. was incubated to form the biofilms in vitro, and the samples were divided into three groups randomly： group A （blank control）; group B in which the biofilms were treated by APNPs （the setting of the equipment： 10 kHz, 1600 ns and 8 kV）; group C in which the biofilms were exposed only to a gas jet without ignition of the plasma. Each group had three samples and each sample was processed for up to 5 min. The biofilms were then fluorescently stained, observed and photographed under a laser scanning confocal microscope. In the animal experiment, six male Japanese white rabbits were divided into two groups randomly （n=3 in each group） in terms of the different post-treatment time （1-day group and 5-day group）. The buccal mucosa of the left side and the mucosa of the ventral surface of the tongue were treated by APNPs for 10 min in the same way as the bacterial biofilm experiment in each rabbit, and the corresponding mucosa of the other sides served as normal control. The clinical manifestations of the oral mucosa were observed and recorded every day. The rabbits were sacrificed one or five day（s） after APNPs treatment. The oral mucosa were harvested and prepared to haematoxylin and eosin-stained sections. Clinical observation and histopathological scores were used to assess mucosal changes. The results showed the obvious P.g. biofilms were formed at 10 days, and most of the bacteria in groups A and C were alive under a laser scanning confocal microscope, but the bacteria in the group B were almost all dead. In animal experiment, no ulcers, anabrosis and oral mucositis were found in both the 1-day and 5-day groups. The aver- age mucous membrane irritation index was -0.83 and -0.67 in the 1-day and 5-day groups, respectively, suggesting that no intense mucosal membrane irritation responses occurred. It was concluded that APNPs could effectively kill Pg. in the biofilms and did not cause any pathological changes in the normal mucosa, suggesting that the plasma jet （APNPs） may be applied to oral diseases as a novel sterilization device in the future.

Fabricating a reactive surface on the fibroin film by a room-temperature plasma jet array for biomolecule immobilization

A simple dielectric barrier discharge（DBD） jet array was designed with a liquid electrode and helium gas.The characteristics of the jet array discharge and the preliminary polymerization with acrylic acid（AA） monomer were presented.The plasma reactor can produce a cold jet array with a gas temperature lower than 315 K,using an applied discharge power between 6 W and 30 W（V dis × I dis）.A silk fibroin film（SFF） was modified using the jet array and AA monomer,and the treated SFF samples were characterized by atomic force microscopy（AFM）,scanning electron microscopy（SEM）,Fourier transform infrared spectroscopy（FTIR）,and contact angle（CA）.The deposition rate of the poly acrylic acid（PAA） was able to reach 300 nm/min,and the surface roughness and energy increased with the AA flow rate.The FTIR results indicate that the modified SFF had more carboxyl groups（-COOH） than the original SFF.This latter characteristic allowed the modified SFF to immobilize more quantities of antimicrobial peptide（AP,LL-37） which inhibited the Escherichia coli（E.Coli） effectively.

Comparison of discharge characteristics and methylene blue degradation through a direct-current excited plasma jet with air and oxygen used as working gases

Through using a direct-current driven plasma jet operated underwater,degradation of methylene blue(MB)is investigated with air and oxygen used as working gases.With a low power voltage,a plasma plume extends from the needle electrode,which is purple in air.It turns pink after it bridges the two electrodes.During the process,oxygen plasma remains white.Discharge operates in a pulsed mode or a continuous one,which depends on the magnitude of power voltage.For the pulsed mode,oxygen discharge has a shorter plume and a higher pulse frequency than air discharge under the same power voltage.For the same current of the continuous mode,both power and gap voltages of oxygen discharge are higher than those of air discharge.Moreover,MB degradation efficiency increases with increasing power voltage or initial concentration of MB solution.Compared with air discharge,oxygen discharge has a higher degradation efficiency with the same power voltage and treatment time.The pulsed oxygen discharge with power voltage of about 6.5 k V has the highest efficiency in degrading MB dye,reaching approximately 85.8%after 10 min treatment.As a comparison,after 10 min treatment in air discharge,the highest degradation efficiency is 63.7%,which appears in the continuous mode at a power voltage of 10.6 kV.Besides,optical spectra from the discharges are also compared for the two types of working gases.

Comparison of Sterilizing Effect of Nonequilibrium Atmospheric-Pressure He/O_2 and Ar/O_2 Plasma Jets

The sterilizing effect of the non-equilibrium atmospheric pressure plasma jet by applying it to the Bacillus subtilis spores is invesigated. A stable glow discharge in argon or helium gas fed with active gas （oxygen）, was generated in the coaxial cylindrical reactor powered by the radio-frequency power supply at atmospheric pressure. The experimental results indicated that the efficiency of killing spores by making use of an Ar/O2 plasma jet was much better than with a He/O2 plasma jet. The decimal reduction value of Ar/O2 and He/O2 plasma jets under the same experimental conditions was 4.5 seconds and 125 seconds, respectively. It was found that there exists an optimum oxygen concentration for a certain input power, at which the sterilization efficiency reaches a maximum value. It is believed that the oxygen radicals are generated most efficiently under this optimum condition.

Sterilization of Staphylococcus Aureus by an Atmospheric Non-Thermal Plasma Jet

An atmospheric non-thermal plasma jet was developed for sterilizing the Staphylococcus aureus （S. aureus）. The plasma jet was generated by dielectric barrier discharge （DBD）, which was characterized by electrical and optical diagnostics. The survival curves of the bacteria showed that the plasma jet could effectively inactivate 10 6 cells of S. aureus within 120 seconds and the sterilizing efficiency depended critically on the discharge parameter of the applied voltage. It was further confirmed by scanning electron microscopy （SEM） that the cell morphology was seriously damaged by the plasma treatment. The plasma sterilization mechanism of S. aureus was attributed to the active species of OH, N 2 ＋ and O, which were generated abundantly in the plasma jet and characterized by OES. Our findings suggest a convenient and low-cost way for sterilization and inactivation of bacteria.