Analyses of nonequilibrium transport in atmospheric-pressure direct-current argon discharge under different modes

The key plasma parameters under different discharge modes, such as heavy-particle and electron temperatures, electron number density, and nonequilibrium volume of plasmas, play important roles in various applications of gas discharge plasmas. In this study, a self-consistent two-dimensional nonequilibrium fluid model coupled with an external circuit model is established to reveal the mechanisms related to the discharge modes, including the normal glow, abnormal glow,arc, and glow-to-arc transition modes, with an atmospheric-pressure direct-current(DC) argon discharge as a model plasma system. The modeling results show that, under different discharge modes, the most significant difference between the preceding four discharge modes lies in the current and energy transfer processes on the cathode side. On one hand, the current to the cathode surface is mainly delivered by the ions coming from the plasma column under the glow discharge mode due to the low temperature of the solid cathode, whereas the thermionic and secondary electrons emitted from the hot cathode surface play a very important role under the arc mode with a higher cathode surface temperature and higher ion flux toward the cathode. On the other hand, the energy transfer channel on the cathode side changes from mainly heating the solid cathode under the glow mode to simultaneously heating both the solid cathode and plasma column under the arc mode with an increase in the discharge current. Consequently, the power density in the cathode sheath(P_c) was used as a key parameter for judging different discharge modes, and the range of(0.28–1.2) × 10^(12) W m^(-3) was determined as a critical window of P_c corresponding to the glow-to-arc-mode transition for the atmospheric-pressure DC argon discharge, which was also verified by comparison with the experimental results in this study and the data in the previous literature.

Solvent-Free Manufacturing of Lithium-Ion Battery Electrodes via Cold Plasma

Slurry casting has been used to fabricate lithium-ion battery electrodes for decades,which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering.This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials,enabling solvent-free manufacturing electrodes with any electrochemistry of choice.The cold-plasma-coating technique enables fabricating electrodes with thickness(>200 pm),high mass loading(>30 mg cm^(-2)),high peel strength,and the ability to print lithium-ion batteries in an arbitrary geometry.This crosscutting,chemistry agnostic,platform technology would increase energy density,eliminate the use of solvents,vacuum drying,and calendering processes during production,and reduce manufacturing cost for current and future cell designs.Here,lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique.It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes.Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6%over 500 cycles.For the highly conductive cathode material lithium cobalt oxide,an areal capacity of 4.2 mAh cm^(-2)at 0.2 C is attained.We anticipate that this new,highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.

Mitigation of polycyclic aromatic hydrocarbons(PAHs)in roasted beef patties by cold plasma treatment and products quality evaluation

The cold plasma(CP)technique was applied to alleviate the contamination of polycyclic aromatic hydrocarbon(PAH)in this investigation.Two different CP treatments methods were implemented in the production of beef patties,to investigate their inhibition and degradation capacity on PAHs.With 5 different cooking oils and fats addition,the inhibition mechanism of in-package cold plasma(ICP)pretreatment was explored from the aspect of raw patties fatty acids composition variation.The results of principal component analysis showed that the first two principal components accounted for more than 80%of the total variation in the original data,indicating that the content of saturated fatty acids was significantly positively correlated with the formation of PAHs.ICP pretreatment inhibited the formation of PAHs by changing the composition of fatty acids,which showed that the total amount of polyunsaturated fatty acids decreased and the total amount of monounsaturated fatty acids increased.Sensory discrimination tests demonstrated there were discernable differences between 2 CP treated samples and the controls,utilization of the ICP pretreatment in meat products processing was expected to achieve satisfying eating quality.In conclusion,CP treatment degraded PAHs through stepwise ring-opening oxidation in 2 reported pathways,the toxicity of PAHs contaminated products was alleviated after CP treatment.

All-organic modification coating prepared with large-scale atmospheric-pressure plasma for mitigating surface charge accumulation

The surface charge accumulation on polymers often leads to surface flashover.Current solutions are mainly based on the introduction of inorganic fillers.The high-cost process and low compatibility remain formidable challenges.Moreover,existing researches on all-organic insulation focus on capturing electrons,contrary to alleviating charge accumulation.Here,an all-organic modification coating was prepared on polystyrene(PS)with the large-scale atmospheric-pressure plasma,which exhibits outperformed function in mitigating surface charge accumulation.The surface charge dissipation rate and surface conductivity are promoted by about 1.37 and 9.45 times,respectively.Simulation and experimental results show that this all-organic modification coating has a smaller electron affinity potential compared with PS.The decrease of electron affinity potential may result in accelerated surface charge decay of PS,which has never been involved in previous works.Moreover,this coating also has good reliability in a repeated surface flashover.This facile and large-scale approach brings up a novel idea for surface charge regulation and the manufacture of advanced dielectric polymers.

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.

Atmospheric-Pressure DBD Cold Plasma for Preparation of High Active Au/P25 Catalysts for Low-Temperature CO Oxidation

Cold plasma generated by dielectric barrier discharge （DBD） at atmospheric pressure was adopted for preparation of commercial TiO2 Degussa P25 supported Au catalysts （Au/P25- P） with the assistance of the deposition-precipitation procedure. The influences of the plasma reduction time and calcination on the performance of the Au/P25-P catalysts were investigated. CO oxidation was performed to investigate the catalytic activity of the Au/P25 catalysts. The results show that DBD cold plasma for the fabrication of Au/P25-P catalysts is a fast process, and Au/P25-P （4 min） exhibited the highest CO oxidation activity due to the complete reduction of Au compounds and less consumption of oxygen vacancies. In order to form more oxygen vacancies active species, Au/P25-P was calcined to obtain Au/P25-PC catalysts. Interestingly, Au/P25- PC exhibited the highest activity for CO oxidation among the Au/P25 samples. The results of transmission electron microscopy （TEM） indicated that the smaller size and high distribution of Au nanoparticles are the mean reasons for a high performance of Au/P25-PC. Atmospheric- pressure DBD cold plasma was proved to be of great efficiency in preparing high performance supported Au catalysts.

Partially crystallized Pd nanoparticles decorated TiO_2 prepared by atmospheric-pressure cold plasma and its enhanced photocatalytic performance

TiO2 decorated with partially crystallized Pd nanoparticles （Pd/TiO2-P） was successfully prepared by atmospheric-pressure dielectric barrier discharge cold plasma. The XRD and XPS analyses proved that Pd ions were reduced to partially crystallized metallic Pd nanoparticles in Pd/TiO2-P. The XPS spectra also indicated that an enhanced metal-support interaction was formed due to the existence of partially crystallized Pd nanoparticles with lower coordination number in Pd/TiO2-P. Photocatalytic activity of Pd/TiO2-P was much higher than that of TiO2 samples decorated with well crystallized Pd nanoparticles.

Tuning Effect of N_2 on Atmospheric-Pressure Cold Plasma CVD of TiO_2 Photocatalytic Films

To deposit TiO2 films through plasma CVD, the partial pressure ratio of O2 to TIC14 should be greater than the stoichiometric ratio （PO2/PTiCl4 〉 1）. However, this may lead to the formation of powder instead of film on the substrate when using volume dielectric barrier discharge （volume-DBD） at atmospheric pressure. In this study, by adding N2 into the working gas Ar, TiO2 photocatalytic films were successfully fabricated in the presence of excess O2 （PO2/PTiC14 = 2.6） by using a wire-to-plate atmospheric-pressure volume-DBD. The tuning effect of N2 on the deposition of TiO2 film was studied in detail. The results showed that by increasing the N2 content, the deposition rate and particle size of the TiO2 film were reduced, and its photocatalytic activity was enhanced. The tuning mechanism of N2 is further discussed.

Synthesis of Cu-Doped Mixed-Phase TiO_2 with the Assistance of Ionic Liquid by Atmospheric-Pressure Cold Plasma

An atmospheric-pressure dielectric barrier discharge （DBD） gas-liquid cold plasma was employed to synthesize Cu-doped TiO~ nanoparticles in an aqueous solution with the assistance of [C2MIM]BF4 ionic liquid （IL） and using air as the working gas. The influences of the discharge voltage, IL and the amount of copper nitrite were investigated. X-ray diffraction, N2 adsorption-desorption measurements and UV-Vis spectroscopy were adopted to characterize the samples. The results showed that the specific surface area of TiO2 was promoted with Cu-doping （from 57.6 m^2.g^-1 to 106.2 m^2.g^-1 with 3% Cu-doping）, and the content of anatase was increased. Besides, the band gap energy of TiO~ with Cu-doping decreased according to the UV-Vis spec- troscopy test. The 3%Cu-IL-TiO2 samples showed the highest eificiency in degrading methylene blue （MB） dye solutions under simulated sunlight with an apparent rate constant of 0.0223 min-1, which was 1.2 times higher than that of non-doped samples. According to the characterization results, the reasons for the high photocatalytic activity were discussed.

Cold plasma-activated Cu-Co catalysts with CN vacancies for enhancing CO_(2)electroreduction to low-carbon alcohol

Electrocatalytic CO_(2)reduction reaction to low-carbon alcohol is a challenging task,especially high selectivity for ethanol,which is mainly limited by the regulation of reaction intermediates and subsequent C–C coupling.A Cu-Co bimetallic catalyst with CN vacancies is successfully developed by H_(2)cold plasma toward a high-efficiency CO_(2)RR into low-carbon alcohol.The Cu-Co PBA-V_(CN)(Prussian blue analogues with CN vacancies)electrocatalyst yields methanol and ethanol as major products with a total low-carbon alcohol FE of 83.8%(methanol:39.2%,ethanol:44.6%)at-0.9 V vs.RHE,excellent durability(100 h)and a small onset potential of-0.21 V.ATR-SEIRAS(attenuated total internal reflection surface enhanced infrared absorption spectroscopy)and DFT(density functional theory)reveal that the steric hindrance of V_(CN)can enhance the CO generation from*COOH,and the C–C coupling can also be increased by CO spillover on uniformly dispersed Cu atoms.This work provides a strategy for the design and preparation of electrocatalysts for CO_(2)RR into low-carbon alcohol products and highlights the impact of catalyst steric hindrance to catalytic performance.

Nitrogen cold plasma treatment stabilizes Cu^(0)/Cu^(+) electrocatalysts to enhance CO_(2) to C2 conversion

Cu-based materials are ideal catalysts for CO_(2) electrocatalytic reduction reaction(CO_(2)RR) into multicarbon products.However,such reactions require stringent conditions on local environments of catalyst surfaces,which currently are the global pressing challenges.Here,a stabilized activation of Cu^(0)/Cu^(+)-onAg interface by N_(2) cold plasma treatment was developed for improving Faradaic efficiency(FE) of CO_(2)RR into C2 products.The resultant Ag@Cu-CuN_x exhibits a C2 FE of 72% with a partial current density of-14.9 mA cm^(-2) at-1.0 V vs.RHE(reversible hydrogen electrode).Combining density functional theory(DFT) and experimental investigations,we unveiled that Cu^(0)/Cu^(+) species can be co ntrollably tu ned by the incorporation of nitrogen to form CuN_x on Ag surface,i.e.,Ag@Cu-CuN_x.This strategy enhances ^(*)CO intermediates generation and accelerates C-C coupling both thermodynamically and kinetically.The intermediates O^(*)C^(*)CO,^(*)COOH,and ^(*)CO were detected by in-situ attenuated total internal reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS).The uncovered CO_(2)RR-into-C2 products were carried out along CO_(2)→^(*)COOH→^(*)CO→O^(*)C^(*)CO→^(*)C_(2)H_(3)O→^(*)C_(2)H_(4)O→ C_(2)H_(5)OH(or ^(*)C_(2)H_(3)O→^(*)O+C_(2)H_(4)) paths over Ag@Cu-CuN_x electrocatalyst.This work provides a new approach to design Cu-based electrocatalysts with high-efficiency,mild condition,and stable CO_(2)RR to C2 products.

Surface Modification of Polypropylene Microporous Membrane by Atmospheric-pressure Plasma Induced N-vinyl-2-pyrrolidone Graft Polymerization

Membrane surfaces modified with poly（N-vinyl-2-pyrrolidone） （PNVP） can be endowed with hydrophilicity, biocompatibility and functionality. In this work, atmospheric pressure dielectric barrier discharge plasma graft polymerization of N-vinyl-2-pyrrolidone （NVP） onto polypropylene （PP） microporous membrane surface was studied. The experimental results reveal that plasma treatment conditions, such as discharge power, treatment time and adsorbed NVP amount, have remarkable effects on the grafting degree of NVP. Structural and morphological changes on the membrane surfaces were characterized by attenuated total reflection-Fourier transform infrared spectroscopy （FT-IR/ATR）, X-ray photoelectron spectroscope （XPS） and field emission scanning electron microscopy （FE-SEM）. Water contact angles of the membrane surfaces were also measured by the sessile drop method. Water contact angles on the membrane surfaces decrease with the increase of NVP grafting degree, which indicates an enhanced hydrophilicity for the modified membranes. The effects of grafting degrees on pure water fluxes were also measured. It is shown that pure water fluxes increase with grafting degree firstly and then decrease adversely. Finally, filtration of bovine serum albumin （BSA） solution and platelets adhesion of the PNVP modified membranes show good protein resistance and potential biocompatibility due to the enhancement of surface hydrophilicity.

Study of generation characteristics of glow-type atmospheric-pressure plasma jet based on DC discharge in air

In order to form an atmospheric-pressure plasma jet without airflow, a needle–ring electrode structure is proposed in this paper. When heteropolar potentials are applied to a needle and a ring, a marked electric field strength enhancement around the needle’s pointed end has been found. When the same potential is applied to both the needle and the ring, the lateral electric field strength for the needle can be weakened. By using the above two methods, an increase of the difference between the pointed end electric field strength and the lateral one is achieved and stable plasma jets are formed. A symmetrical space electric field distribution is established at the pointed end of the needles when several sets of heteropolar needle–ring electrodes are uniformly arranged, which is conducive to forming a uniform array plasma jet. Under DC discharge conditions, a safe and stable plasma jet of high density and an array plasma jet are successfully achieved.

Super-hydrophobic film deposition by an atmospheric-pressure plasma process and its anti-icing characteristics

In this work,the super-hydrophobic(SH)surface was prepared through chemical vapor deposition process by an argon atmospheric pressure plasma jet source with HMDSN(hexamethyldisilazane)as the polymerization precursor.Plasma synthesized organosilicon(SiOxCyHz)thin films with water contact angle over 160°and sliding angle below 5°,were able to be achieved.FTIR and XPS analysis indicates a large number of hydrocarbon compositions were polymerized in the thin films enduing the latter very-low surface free energy.SEM shows the SH films display micro-nanostructure and with high degree of averaged surface roughness 190 nm evaluated by AFM analysis.From experiments under controlled low-temperature and moisture conditions,the prepared SH surface exhibits good anti-icing effects.Significantly prolonging freezing time was achievable on the SH thin films for both static and sliding water droplets.This investigation demonstrates the anti-icing potentials of SH surface prepared through low-cost simple atmospheric-pressure plasma polymerization process.

Properties enhancement of antimicrobial chitosan-deposited polylactic acid films via cold plasma treatment

The present study aimed to understand the effect of dielectric barrier discharge cold plasma(DBD-CP)technology on the antimicrobial chitosan deposition and the properties enhancement of polylactic acid(PLA)films.The results indicated that DBD-CP was an effective method for improving the adhesion and surface hydrophilicity of PLA,facilitating the deposition of chitosan coating.This modification was attributed to the increased surface roughness,as well as the presence of polar functional groups observed through atomic force microscopy,surface free energy and Fourier transform infrared spectroscopy analysis.The study further revealed that both water resistance and mechanical properties were significantly improved after DBD-CP treatment,which was positively correlated with the amount of chitosan deposited on the PLA surfaces.Following comprehensive evaluation,the treatment at 75 W was determined as the optimal condition for enhancing the properties.Additionally,the modified film exhibited strong antimicrobial activity against Staphylococcus aureus.Consequently,the DBD-CP technology could be a promising tool for better utilization of PLA-based materials in the antibacterial food packaging industry.

LIF diagnostics of hydroxyl radical in a methanol containing atmospheric-pressure plasma jet

In this paper, a pulsed-dc CH;OH/Ar plasma jet generated at atmospheric pressure is studied by laser-induced fluorescence（LIF） and optical emission spectroscopy（OES）. A gas–liquid bubbler system is proposed to introduce the methanol vapor into the argon gas, and the CH3OH/Ar volume ratio is kept constant at about 0.1%. Discharge occurs in a 6-mm needle-to-ring gap in an atmospheric-pressure CH;OH/Ar mixture. The space-resolved distributions of OH LIF inside and outside the nozzle exhibit distinctly different behaviors. And, different production mechanisms of OH radicals in the needle-to-ring discharge gap and afterglow of plasma jet are discussed. Besides, the optical emission lines of carbonaceous species, such as CH, CN, and C;radicals, are identified in the CH;OH/Ar plasma jet. Finally, the influences of operating parameters（applied voltage magnitude, pulse frequency, pulsewidth） on the OH radical density are also presented and analyzed.

Local oxynitriding of AZ31 magnesium alloy by atmospheric-pressure plasma treatment at room temperature

A surface-hardening treatment for AZ31 magnesium alloy using an atmospheric-pressure plasma jet(APPJ)at room temperature was developed.Magnesium is a potential engineering material because it is lightweight;however,magnesium alloys are difficult to heat-treat because of their low flaming temperature.Magnesium alloy specimens were irradiated with a localized atmospheric-pressure plasma jet generated by dielectric-barrier discharge for 180 s in air.The APPJ excited oxygen and nitrogen molecules in the ambient air,resulting in the formation of an oxynitrided layer;oxygen and nitrogen diffusion layer,on the surface of the magnesium alloy.The hardness and elemental distribution for the treated surface were examined.The top surface of the APPJ-treated magnesium alloy achieved a maximum hardness of 108 HV,which was~1.7 times greater than that of the untreated surface.Elemental analysis using an electron-probe microanalyzer revealed strong oxygen and nitrogen signals corresponding to the hardened region of the magnesium alloy,meaning that the hardness increased as a result of the formation of the oxynitrided layer.The proposed APPJ treatment is a promising approach for locally hardening magnesium alloys without using a heat treatment.

Control of multidrug-resistant planktonic Acinetobacter baumannii:biocidal efficacy study by atmospheric-pressure air plasma

In this research,an atmospheric-pressure air plasma is used to inactivate the multidrug-resistant Acinetobacter baumannii in liquid.The efficacy of the air plasma on bacterial deactivation and the cytobiological variations after the plasma treatment are investigated.According to colony forming units,nearly all the bacteria（6-log） are inactivated after 10 min of air plasma treatment.However,7% of the bacteria enter a viable but non-culturable state detected by the resazurin based assay during the same period of plasma exposure.Meanwhile,86% of the bacteria lose their membrane integrity in the light of SYTO 9/PI staining assay.The morphological changes in the cells are examined by scanning electron microscopy and bacteria with morphological changes are rare after plasma exposure in the liquid.The concentrations of the long-living RS,such as H2O2,NO3^- and O3,in liquid induced by plasma treatment are measured,and they increase with plasma treatment time.The changes of the intracellular ROS may be related to cell death,which may be attributed to oxidative stress and other damage effects induced by RS plasma generated in liquid.The rapid and effective bacteria inactivation may stem from the RS in the liquid generated by plasma and air plasmas may become a valuable therapy in the treatment of infected wounds.

Numerical study of atmospheric-pressure argon plasma jet propagating into ambient nitrogen

A 2D axial symmetry fluid model is applied to study the features of an atmospheric-pressure argon(Ar) plasma jet propagating into ambient nitrogen(N_(2)) driven by a pulsed voltage,emphasizing the influence of gas velocity on the dynamic characteristics of the jet. The results show that the Ar jet exhibits a cylindrical-shaped channel and the jet channel gradually shrinks with the increase in propagation length. The jet propagation velocity varies with time. Inside the dielectric tube, the plasma jet accelerates propagation and reaches its maximum value near the nozzle. Exiting the tube, its velocity quickly decreases and when approaching the metal plane,the decrease in jet velocity slows down. The increase in gas speed results in the variation of jet spatial distribution. The electron density presents a solid structure at lower gas flow speeds,whereas an annular structure can be observed under the higher gas flow velocity in the ionization head. The jet length increases with the flow velocity. However, when the flow velocity exceeds a critical value, the increase in the rate of the plasma jet length slows down. In addition, the gas velocity effect on the generation and transport of the reactive particles is also studied and discussed.

Debridement Effect on Periodontal Pathogen <i>Porphyromonas gingivalis</i>Cultured on Titanium by Application of Atmospheric-Pressure Plasma

The debridement treatments of dental implants are very important in long-term maintenance after implant placement in a patient. Deposition of periodontal pathogens around the implant surface has a high risk of causing periimplantitis. The aim of this study was to evaluate the extent of elimination of Porphyromonas gingivalis, known as representative periodontopathic bacteria, from titanium, which has been the main material used for dental implants. Assuming that the debridement processing of dental implants removes periodontal bacteria, one of the methods for removing bacteria deposited on titanium is considered to be plasma irradiation. Irradiation with atmospheric-pressure plasma was carried out against periodontopathic bacteria cultured and deposited on the surface of a titanium disk. After the plasma irradiation, the reduction of the number of bacteria re-cultured for 24 hours was evaluated. The number of viable bacteria on the titanium surface was estimated by an ATP-bioluminescent assay. Viable cells after the plasma irradiation were reduced to 1.5% or less compared to the untreated group. As one of the methods of debridement in general dental treatments, atmospheric-pressure plasma has proved to be an effective method to remove adverse prognostic factors in dental patients.