Dielectric barrier discharge plasma-assisted catalytic ammonia synthesis:synergistic effect of Ni-MOF-74 catalyst and nanosecond pulsed plasma

Ammonia is one of the most important chemical raw materials in both manufacture and life of human.Traditionally Haber-Bosch method for ammonia synthesis involves high temperature and high pressure conditions,leading to significant energy consumption and environmental pollution.Non-thermal plasma(NTP) is a promising alternative approach to ammonia synthesis at low temperature and atmospheric pressure.In this study,the synergistic effect of nanosecond pulsed dielectric barrier discharge(np-DBD) and Ni-MOF-74 catalyst was investigated in ammonia synthesis by utilizing nitrogen and hydrogen as feedstock.The results demonstrated that the plasma catalytic-synthesis process parameters play a crucial role in the synthesis process of ammonia.The highest ammonia synthesis rate of 5145.16 μmol·g^(-1)·h^(-1)with an energy efficiency of 1.27 g·kWh^(-1)was observed in the presence of the Ni-MOF-74 catalyst,which was3.7 times higher than that without Ni-MOF-74 catalyst.The synergistic effect of Ni-MOF-74catalyst and nanosecond pulsed plasma was explored by in-situ plasma discharge diagnostics.

Evaluation of genetic response of mesenchymal stem cells to nanosecond pulsed electric fields by whole transcriptome sequencing

BACKGROUND Mesenchymal stem cells(MSCs)modulated by various exogenous signals have been applied extensively in regenerative medicine research.Notably,nanosecond pulsed electric fields(nsPEFs),characterized by short duration and high strength,significantly influence cell phenotypes and regulate MSCs differentiation via multiple pathways.Consequently,we used transcriptomics to study changes in messenger RNA(mRNA),long noncoding RNA(lncRNA),microRNA(miRNA),and circular RNA expression during nsPEFs application.AIM To explore gene expression profiles and potential transcriptional regulatory mechanisms in MSCs pretreated with nsPEFs.METHODS The impact of nsPEFs on the MSCs transcriptome was investigated through whole transcriptome sequencing.MSCs were pretreated with 5-pulse nsPEFs(100 ns at 10 kV/cm,1 Hz),followed by total RNA isolation.Each transcript was normalized by fragments per kilobase per million.Fold change and difference significance were applied to screen the differentially expressed genes(DEGs).Gene Ontology and Kyoto Encyclopedia of Genes and Genomes analyses were performed to elucidate gene functions,complemented by quantitative polymerase chain reaction verification.RESULTS In total,263 DEGs were discovered,with 92 upregulated and 171 downregulated.DEGs were predominantly enriched in epithelial cell proliferation,osteoblast differentiation,mesenchymal cell differentiation,nuclear division,and wound healing.Regarding cellular components,DEGs are primarily involved in condensed chromosome,chromosomal region,actin cytoskeleton,and kinetochore.From aspect of molecular functions,DEGs are mainly involved in glycosaminoglycan binding,integrin binding,nuclear steroid receptor activity,cytoskeletal motor activity,and steroid binding.Quantitative real-time polymerase chain reaction confirmed targeted transcript regulation.CONCLUSION Our systematic investigation of the wide-ranging transcriptional pattern modulated by nsPEFs revealed the differential expression of 263 mRNAs,2 miRNAs,and 65 lncRNAs.Our study demonstrates that nsPEFs may affect stem cells through several signaling pathways,which are involved in vesicular transport,calcium ion transport,cytoskeleton,and cell differentiation.

A comparative study on the spectral characteristics of nanosecond pulsed discharges in atmospheric He and a He+2.3%H_(2)O mixture

Nanosecond pulsed discharges at atmospheric pressure in a pin-to-pin electrode configuration are well reproducible in time and space, which is beneficial to the fundamentals and applications of low-temperature plasmas. In this experiment, the discharges in helium(He) and He with 2.3%water vapor(H_(2)O) are driven by a series of 10 ns overvoltage pulses(~13 k V). Special attention is paid to the spectral characteristics obtained in the center of discharges by time-resolved optical emission spectroscopy. It is found that in helium, the emission of atomic and molecular helium during the afterglow is more intense than that in the active discharge, while in the He+2.3%H_(2)O mixture, helium emission is only observed during the discharge pulse and the molecular helium emission disappears. In addition, the emissions of OH(A-X) and Hα present similar behavior that increases sharply during the falling edge of the voltage pulse as the electrons cool down rapidly. The gas temperature is set to remain low at 540 K by fitting the OH(A-X) band. A comparative study on the emission of radiative species(He, He_(2), OH and H)is performed between these two discharge cases to derive their main production mechanisms. In both cases, the dominant primary ion is He^(+) at the onset of discharges, but their He^(+) charge transfer processes are quite different. Based on these experimental data and a qualitative discussion on the discharge kinetics, with regard to the present discharge conditions, it is shown that the electron-assisted three-body recombination processes appear to be the significant sources of radiative OH and H species in high-density plasmas.

High-quality micro-shape fabrication of monocrystalline diamond by nanosecond pulsed laser and acid cleaning

The flat plane of small surface roughness below 0.1μm average roughness was obtained for monocrystalline diamond by nanosecond pulsed laser irradiation of 1060 nm and post-process acid cleaning,at a laser fluence around the material removal threshold value.The glossy and flat plane at the bottom of the micro-groove was parallel to the top surface of the specimen,although the round beam of Gaussian mode was irradiated in the direction perpendicular to the top surface of specimen.The square beam of top-hat mode produced a shallower micro-groove with a wider,flatter bottom compared with the round beam in Gaussian mode.The creation method of the flat plane with small surface roughness was discussed in the arrangement strategy of linear micro-grooving by the square beam of top-hat mode.Normal side-by-side repetition of linear micro-grooving did not create a flat plane with constant depth.Therefore,a two-step scanning method was proposed in order to overcome the problem in the normal side-by-side repetition of liner micro-grooving.Non-removal areas were partly retained between the processing lines in the first step,and the laser scanning was conducted on the retained area in the second step.The newly proposed two-step scanning method was practical and useful to create a widely flat plane with small surface roughness,and the two-step scanning method provided superior control over the micro-groove depth.This proposed method can reduce the surface roughness in addition to the shape creation of monocrystalline diamond,and it can be used as a high-quality micro-shape fabrication method of monocrystalline diamond.

Tumor ablation with nanosecond pulsed electric fields

Liver cancer is one of the most malignant cancers. It is reported that 600 000 patients died from liver cancer every year. [1,2] Hepatocellular carcinoma (HCC) is a particular problem because symptoms are not evident until the disease has progressed and hepatitis B, which is prominent specific regions of Asia, is a common precursor of the disease. There are many liver cancer

Effects of the transverse electric field on nanosecond pulsed dielectric barrier discharge in atmospheric airflow

In this paper,an asymmetric electrode geometry(the misalignment between the ends of highvoltage and grounded electrodes)is proposed in order to investigate the effects of the transverse electric field on nanosecond pulsed dielectric barrier discharge(DBD).The results show that diffuse discharge manifests in the misaligned region and the micro-discharge channel in the aligned region moves directionally.Moreover,the diffuse discharge area increases with the decrease of the discharge gap and pulse repetition frequency,which is consistent with the variation of the moving velocity of the micro-discharge channel.When airflow is introduced into the discharge gap in the same direction as the transverse electric field,the dense filamentary discharge region at the airflow inlet of asymmetric electrode geometry is larger than that of symmetric electrode geometry.However,when the direction of the airflow is opposite to that of the transverse electric field,the dense filamentary discharge region of asymmetric electrode geometry is reduced.The above phenomena are mainly attributed to the redistribution of the space charges induced by the transverse electric field.

Spatiotemporal characteristics of nanosecond pulsed discharge in an extremely asymmetric electric field at atmospheric pressure

In this paper,high resolution temporal-spatial diagnostics are employed to research the optical characteristics of nanosecond pulsed dielectric barrier discharge in needle-plate electrode configuration.Temporal-spatial distributions of discharge images,the emission intensities of optical emission spectra,and plasma vibrational and rotational temperatures are investigated.By analyzing the evolution of vibrational and rotational temperatures in space and time dimensions,the energy distribution and energy transfer process in plasma are also discussed.It is found that a diffuse structure with high density plasma concentrated in the region near the needle tip can be presented in nanosecond pulsed discharge,and an obvious energy transfer from electronic energy to vibration energy can be observed in each discharge pulse.

The Effect of the Quartz Tube on the Appearance of Nanosecond Pulsed Discharge in Air

An experimental investigation of a nanosecond pulsed dielectric barrier discharge in atmospheric air is presented. In the setup a quartz tube was inserted between the cone and plane electrodes in the direction parallel to the electric field. It was shown that the appearance and property of the discharge were sensitive to the size and the position of the quartz tube. When the tube was placed on the grounded plane electrode, the discharge intensity was found to improve gradually with the increase in the diameter of the quartz tube. Furthermore, with an appropriate distance between the bottom edge of the quartz tube and the plane electrode, the discharge tended to exhibit better performance in generating homogeneous diffusive plasma. The possible mechanism is discussed.

Simulations and Measurement of Electron Energy and Effective Electron Temperature of Nanosecond Pulsed Argon Plasma

The behavior of argon plasma driven by nanosecond pulsed plasma in a low-pressure plasma reactor is investigated using a global model, and the results are compared with the experimental measurements. The time evolution of plasma density and the electron energy probability function are calculated by solving the energy balance and Boltzmann equations. During and shortly after the discharge pulse, the electron energy probability function can be represented by a bi-Maxwellian distribution, indicating two energy groups of electrons. According to the effective electron temperature calculation, we find that there are more high-energy electrons that play an important role in the excitation and ionization processes than low-energy electrons. The effective electron temperature is also measured via optical emission spectroscopy to evaluate the simulation model. In the comparison, the simulation results are found to be in agreement with the measure- ments. Furthermore, variations of the effective electron temperature are presented versus other discharge parameters, such as pulse width time, pulse rise time and gas pressure.

Study of the selective effect on cells induced by nanosecond pulsed electric field with the resistor-capacitor circuit model

A resistor-capacitor(RC)circuit model is proposed to study the effect of nanosecond pulsed electricfield on cells according to the structure and electrical parameters of cells.After a nanosecond step fieldhas been applied,the variation of voltages across cytomembrane and mitochondria membrane both in nor-mal and in malignant cells are studied with this model.The time for selectively targeting the mitochondriamembrane and malignant cell can be evaluated much easily with curves that show the variation of voltageacross each membrane with time.Ramp field is the typical field applied in electrobiology.The voltagesacross each membrane induced by ramp field are analyzed with this model.To selectively target the mito-chondria membrane,proper range of ramp slope is needed.It is relatively difficult to decide the range ofa slope to selectively affect the malignant cell.Under some conditions,such a range even does not exist.

Deposition of SiCxHyOz thin film on epoxy resin by nanosecond pulsed APPJ for improving the surface insulating performance

Non-thermal plasma surface modification for epoxy resin（EP）to improve the insulation properties has wide application prospects in gas insulated switchgear and gas insulatedtransmission line.In this paper,a pulsed Ar dual dielectrics atmospheric-pressure plasma jet（APPJ）was used for Si CxHyOzthin film deposition on EP samples.The film deposition was optimized by varying the treatment time while other parameters were kept at constants（treatment distance：10 mm,precursor flow rate：0.6 l min-（-1）,maximum instantaneous power：3.08 k W and single pulse energy：0.18 m J）.It was found that the maximum value of flashover voltages for negative and positive voltage were improved by 18%and 13%when the deposition time was3 min,respectively.The flashover voltage reduced as treatment time increased.Moreover,all the surface conductivity,surface charge dissipation rate and surface trap level distribution reached an optimal value when thin film deposition time was 3 min.Other measurements,such as atomic force microscopy and scanning electron microscope for EP surface morphology,Fourier transform infrared spectroscopy and x-ray photoelectron spectroscopy for EP surface compositions,optical emission spectra for APPJ deposition process were carried out to better understand the deposition processes and mechanisms.The results indicated that the original organic groups（C–H,C–C,C=O,C=C）were gradually replaced by the Si containing inorganic groups（Si–O–Si and Si–OH）.The reduction of C=O in ester group and C=C in p-substituted benzene of the EP samples might be responsible for shallowing the trap level and then enhancing the flashover voltage.However,when the plasma treatment time was longer than 3 min,the significant increase of the surface roughness might increase the trap level depth and then deteriorate the flashover performance.

Experimental and numerical investigation on the uniformity of nanosecond pulsed dielectric barrier discharge influenced by pulse parameters

Nanosecond(ns)pulsed dielectric barrier discharge(DBD)is considered as a promising method to produce controllable large-volume and high activity low-temperature plasma at atmospheric pressure,which makes it suitable for wide applications.In this work,the ns pulse power supply is used to excite Ar DBD and the influences of the pulse parameters(voltage amplitude,pulse width,pulse rise and fall times)on the DBD uniformity are investigated.The gas gap voltage(Ug)and conduct current(Ig)are separated from the measured voltage and current waveforms to analyze the influence of electrical parameters.The spectral line intensity ratio of two Ar excited species is used as an indicator of the electron temperature(Te).The time resolved discharge processes are recorded by an intensified charge-coupled device camera and a one-dimensional fluid model is employed to simulate the spatial and temporal distributions of electrons,ions,metastable argon atoms and Te.Combining the experimental and numerical results,the mechanism of the pulse parameters influencing on the discharge uniformity is discussed.It is shown that the space electric field intensity and the space particles'densities are mainly responsible for the variation of discharge uniformity.With the increase of voltage and pulse width,the electric field intensity and the density of space particles increased,which results in the discharge mode transition from non-uniform to uniform,and then non-uniform.Furthermore,the extension of pulse rise and fall times leads to the discharge transition from uniform to nonuniform.The results are helpful to reveal the mechanism of ns pulsed DBD mode transition and to realize controllable and uniform plasma sources at atmospheric pressure.

Discharge characteristics and reactive species production of unipolar and bipolar nanosecond pulsed gas–liquid discharge generated in atmospheric N2

In this paper,unipolar pulse(including positive pulse and negative pulse)and bipolar pulse voltage are employed to generate diffuse gas–liquid discharge in atmospheric N2with a rumpetshaped quartz tube.The current–voltage waveforms,optical emission spectra of excited state active species,FTIR spectra of exhaust gas components,plasma gas temperature,and aqueous H2O2,NO2-,andNO3-production are compared in three pulse modes,meanwhile,the effects of pulse peak voltage and gas flow rate on the production of reactive species are studied.The results show that two obvious discharges occur in each voltage pulse in unipolar pulse driven discharge,differently,in bipolar pulse driven discharge,only one main discharge appears in a single voltage pulse time.The intensities of active species(OH(A),and O(3p))in all three pulsed discharge increase with the rise of pulse peak voltage and have the highest value at 200 ml min-1of gas flow rate.The absorbance intensities of NO2and N2O increase with the increase of pulse peak voltage and decrease with the increase of gas flow rate.Under the same discharge conditions,the bipolar pulse driven discharge shows lower breakdown voltage,and higher intensities of excited species(N2(C),OH(A),and O(3p)),nitrogen oxides(NO2,NO,and N2O),and higher production of aqueous H2O2,NO2-,andNO3-compared with both unipolar positive and negative discharges.

Dynamics of plasma bullets by nanosecond pulsed micro-hollow cathode discharge within air

In this paper,the air plasma jet produced by micro-hollow cathode discharge(MHCD)is investigated.The discharge is powered by a positive nanosecond pulse high voltage supply.The waveforms of the discharge,the images of the jet,the evolution of the plasma bullet and the reactive species are obtained to analyze the characteristics of the MHCD plasma jet.It is found that the length of the plasma jet is almost proportional to the air flow rate of 2–6 slm.Two plasma bullets appear one after another during a single period of the voltage waveform,and both of the two plasma bullets are formed during the positive pulse voltage off.The propagation velocity of the two plasma bullets is on the order of several hundred m/s,which is approximate to that of the air flow.These results indicate that the gas flow has an important influence on the formation of this MHCD plasma jet.

Spatial characteristics of nanosecond pulsed micro-discharges in atmospheric pressure He/H2O mixture by optical emission spectroscopy

Atmospheric pressure micro-discharges in helium gas with a mixture of 0.5%water vapor between two pin electrodes are generated with nanosecond overvoltage pulses.The temporal and spatial characteristics of the discharges are investigated by means of time-resolved imaging and optical emission spectroscopy with respect to the discharge morphology,gas temperature,electron density,and excited species.The evolution of micro-discharges is captured by intensified CCD camera and electrical properties.The gas temperature is diagnosed by a two-temperature fit to the ro-vibrational OH(A^(2)Σ^(+)–X^П(2),0–0)emission band and is found to remain low at 425 K during the discharge pulses.The profile of electron density performed by the Stark broadening of Ha 656.1-nm and He I 667.8-nm lines is uniform across the discharge gap at the initial of discharge and reaches as high as 10^(23)m^(-3).The excited species of He,OH,and H show different spatio-temporal behaviors from each other by the measurement of their emission intensities,which are discussed qualitatively in regard of their plasma kinetics.

A model for Nanosecond Pulsed Dielectric Barrier Discharge(NSDBD)actuator and its investigation on the mechanisms of separation control over an airfoil

In order to simulate the flow control problem by using Nanosecond Pulsed Dielectric Barrier Discharge(NSDBD),a one-zone inhomogeneous phenomenological model is constructed based on the experimental and theoretical results.The model is coupled with the unsteady Navier-Stokes equations,which can well predict the compression-expansion wave structures and wave speed compared with experimental results and can be applied to the simulation of the flow control by using NSDBD.The model is adopted to investigate the separation control over NACA0015 airfoil using the NSDBD plasma actuator.The separation-control mechanisms are revealed that the spanwise vortices produced by the plasma actuation play the key role.Each plasma actuation can produce a spanwise vortex around the separation point near the leading edge.The spanwise vortices make the separated free-shear layer unstable and shed away,move downstream along the upper wall,control the flow near the wall,and bring outer flow with high kinetic energy into the near wall region to realize the effective separation control over the upper surface of the airfoil.

Nanosecond pulsed electric fields prime mesenchymal stem cells to peptide ghrelin and enhance chondrogenesis and osteochondral defect repair in vivo

Mesenchymal stem cells(MSCs) are important cell sources in cartilage tissue development and homeostasis,and multiple strategies have been developed to improve MSCs chondrogenic differentiation with an aim of promoting cartilage regeneration.Here we report the effects of combining nanosecond pulsed electric fields(ns PEFs) followed by treatment with ghrelin(a hormone that stimulates release of growth hormone) to regulate chondrogenesis of MSCs.ns PEFs and ghrelin were observed to separately enhance the chondrogenesis of MSCs,and the effects were significantly enhanced when the bioelectric stimulation and hormone were combined,which in turn improved osteochondral tissue repair of these cells within Sprague Dawley rats.We further found that ns PEFs can prime MSCs to be more receptive to subsequent stimuli of differentiation by upregulated Oct4/Nanog and activated JNK signaling pathway.Ghrelin initiated chondrogenic differentiation by activation of ERK1/2 signaling pathway,and RNA-seq results indicated 243 genes were regulated,and JAK-STAT signaling pathway was involved.Interestingly,the sequential order of applying these two stimuli is critical,with ns PEFs pretreatment followed by ghrelin enhanced chondrogenesis of MSCs in vitro and subsequent cartilage regeneration in vivo,but not vice versa.This synergistic prochondrogenic effects provide us new insights and strategies for future cell-based therapies.

Activation of Anti-tumor Immune Response by Ablation of HCC with Nanosecond Pulsed Electric Field

Locoregional therapy is playing an increasingly important role in the non-surgical management of hepatocellular carcinoma(HCC).The novel technique of non-thermal electric ablation by nanosecond pulsed electric field has been recognized as a potential locoregional methodology for indicated HCC.This manuscript explores the most recent studies to indicate its unique anti-tumor immune response.The possible immune mechanism,termed as nano-pulse stimulation,was also analyzed.

Immune response triggered by the ablation of hepatocellular carcinoma with nanosecond pulsed electric field

Nanosecond pulsed electric field(nsPEF)is a novel,nonthermal,and minimally invasive modality that can ablate solid tumors by inducing apoptosis.Recent animal experiments show that nsPEF can induce the immunogenic cell death of hepatocellular carcinoma(HCC)and stimulate the host’s immune response to kill residual tumor cells and decrease distant metastatic tumors.nsPEF-induced immunity is of great clinical importance because the nonthermal ablation may enhance the immune memory,which can prevent HCC recurrence and metastasis.This review summarized the most advanced research on the effect of nsPEF.The possible mechanisms of how locoregional nsPEF ablation enhances the systemic anticancer immune responses were illustrated.nsPEF stimulates the host immune system to boost stimulation and prevail suppression.Also,nsPEF increases the dendritic cell loading and inhibits the regulatory responses,thereby improving immune stimulation and limiting immunosuppression in HCC-bearing hosts.Therefore,nsPEF has excellent potential for HCC treatment.

A study of pulsed high voltage driven hollow-cathode electron beam sources through synchronous optical trigger

In this study,a pulsed,high voltage driven hollow-cathode electron beam sources through an optical trigger is designed with characteristics of simple structure,low cost,and easy triggering.To validate the new design,the characteristics of hollow-cathode discharge and electron beam characterization under pulsed high voltage drive are studied experimentally and discussed by discharge characteristics and analyses of waveform details,respectively.The validation experiments indicate that the pulsed high voltage supply significantly improves the frequency and stability of the discharge,which provides a new solution for the realization of a high-frequency,high-energy electron beam source.The peak current amplitude in the high-energy electron beam increases from 6.2 A to 79.6 A,which indicates the pulsed power mode significantly improves the electron beam performance.Besides,increasing the capacitance significantly affects the highcurrent,lower-energy electron beam more than the high-energy electron beam.