Low-temperature chemistry in plasma-driven ammonia oxidative pyrolysis

Ammonia is gaining increasing attention as a green alternative fuel for achieving large-scale carbon emission reduction. Despite its potential technical prospects, the harsh ignition conditions and slow flame propagation speed of ammonia pose significant challenges to its application in engines. Non-equilibrium plasma has been identified as a promising method, but current research on plasma-enhanced ammonia combustion is limited and primarily focuses on ignition characteristics revealed by kinetic models. In this study, low-temperature and low-pressure chemistry in plasma-assisted ammonia oxidative pyrolysis is investigated by integrated studies of steady-state GC measurements and mathematical simulation. The detailed kinetic mechanism of NH_(3) decomposition in plasma-driven Ar/NH_(3) and Ar/NH_(3)/O_(2) mixtures has been developed. The numerical model has good agreements with the experimental measurements in NH_(3)/O_(2) consumption and N_(2)/H_(2) generation, which demonstrates the rationality of modelling. Based on the modelling results, species density profiles, path flux and sensitivity analysis for the key plasmaproduced species such as NH_(2), NH, H_(2), OH, H, O, O(^(1)D), O_(2)(a^(1)△_(g)), O_(2)(b^(1)∑_(g)^(+)), Ar^(*), H^(-), Ar^(+), NH_(3)^(+), O_(2)^(-) in the discharge and afterglow are analyzed in detail to illustrate the effectiveness of the active species on NH_(3) excitation and decomposition at low temperature and relatively higher E/N values. The results revealed that NH_(2), NH, H as well as H_(2) are primarily generated through the electron collision reactions e + NH_(3)→ e + NH_(2)+ H, e + NH_(3)→ e + NH + H_(2) and the excited-argon collision reaction Ar^(*) + NH_(3)+ H → Ar + NH_(2)+ 2H, which will then react with highly reactive oxidative species such as O_(2)^(*), O^(*), O, OH, and O_(2) to produce stable products of NOx and H_(2)O. NH_(3)→ NH is found a specific pathway for NH_(3) consumption with plasma assistance, which further highlights the enhanced kinetic effects.

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.

Sustainable ammonia synthesis:An in-depth review of non-thermal plasma technologies

Ammonia serves both as a widely used fertilizer and environmentally friendly energy source due to its high energy density,rich hydrogen content,and emissions-free combustion.Additionally,it offers convenient transportation and storage as a hydrogen carrier.The dominant method used for large-scale ammonia production is the Haber-Bosch process,which requires high temperatures and pressures and is energy-intensive.However,non-thermal plasma offers an eco-friendly alternative for ammonia synthesis,gaining significant attention.It enables ammonia production at lower temperatures and pressures using plasma technology.This review provides insights into the catalyst and reactor developments,which are pivotal for promoting ammonia efficiency and addressing existing challenges.At first,the reaction kinetics and mechanisms are introduced to gain a comprehensive understanding of the reaction pathways involved in plasma-assisted ammonia synthesis.Thereafter,the enhancement of ammonia synthesis efficiency is discussed by developing and optimizing plasma reactors and effective catalysts.The effect of other feeding sources,such as water and methane,instead of hydrogen is also presented.Finally,the challenges and possible solutions are outlined to facilitate energy-saving and enhance ammonia efficiency in the future.

Sustainable Ammonia Synthesis from Nitrogen and Water by One-Step Plasma Catalysis

Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.

Experimental Research of Inactivation Effect of Low-Temperature Plasma on Bacteria

The killing logarithms index in killing a vegetative form in an explosure of about 90s and a spore in an explosure of about 120s, by using a low-temperature plasma produced by dielectric barrier discharge （DBD）, reached 5. The speed in killing the strains tested, by using a low-temperature plasma, was the highest with E. Coli, then S. Aureus and B. Subtilis var niger spore. The results of the scanning electron microscope showed that the low-temperature plasma destroyed the outer structure of the bacteria and that the vegetative form was more susceptible to the inactivation effect of the low-temperature plasma than was the spore. This indicated that the effects of the high voltage and high velocity particle flow, in plasma, penetrating through the outer structure of the bacteria might play a dominant role during the inactivation of the bacteria.

Surface Modification of Polyvinylidene Fluoride (PVDF) Membranes by Low-Temperature Plasma with Grafting Styrene

In order to control the surface pore sizes of polyvinylidene fluoride membranes and their distribution, low temperature plasma-induced grafting modifications of PVDF were studied to prepare hydrophobe membranes. By argon （Ar） treating and subsequent grafting reaction, a hydrophobe monomer, styrene, was introduced into the PVDF membrane. Fourier transform infrared attenuated total reflection （FTIR-ATR） was utilized to characterize the chemical and physical changes in the Ar plasma modified membrane. The surface modifications of PVDF membranes were investigated by using scanning electron microscopy （SEM）, atomic force microscopy （AFM） and differential scanning calorimeter （DSC）. The water permeability and the solute rejection were measured by PVDF membrane modified in different graft conditions. Results demonstrated that the pores in the modified membranes get smaller and the distribution of pores gets narrowed with the increase in grafting reaction duration. Longer graft time caused the water flux of PVDF membrane to decrease from 578 kg/（m^2· h） to 23 kg/（m^2· h） and the solute rejection to increase from 73% to 92%.

Low-temperature Plasma Promotes Fibroblast Proliferation in Wound Healing by ROS-activated NF-κB Signaling Pathway

Low-temperature plasma(LTP)has shown great promise in wound healing,although the underlying mechanism remains poorly understood.In the present study,an argon atmospheric pressure plasma jet was employed to treat L929 murine fibroblasts cultured in vitro and skin wounds in BALB/c mice.The in vitro analysis revealed that treatment of fibroblasts with LTP for 15 s resulted in a significant increase in cell proliferation,secretion of epidermal growth factor(EGF)and transforming growth factor-β1(TGF-β1),production of intracellular reactive oxygen species(ROS),and the percentage of cells in S phase,protein expression of phosphorylated p65(P-p65)and cyclin D1,but a noted decrease in the protein expression of inhibitor kappa B(IκB).The in vivo experiments demonstrated that 30-s LTP treatment enhanced the number of fibroblasts and the ability of collagen synthesis,while 50-s treatment led to the opposite outcomes.These results suggested that LTP treatment promotes the fibroblast proliferation in wound healing by inducing the generation of ROS,upregulating the expression of P-p65,downregulating the expression of IκB,and activating the NF-κB signaling pathway and consequently altering cell cycle progression(increased DNA synthesis in S phage).

Design and characteristics investigation of a miniature low-temperature plasma spark discharge device

Atmospheric pressure low-temperature plasma is a promising tool in biomedicine applications including blood coagulation,bacterial inactivation,sterilization,and cancer treatment,due to its high chemical activity and limited thermal damage.It is of great importance to develop portable plasma sources that are safe to human touch and suitable for outdoor and household operation.In this work,a portable and rechargeable low-temperature plasma spark discharge device(130 mm×80 mm×35 mm,300 g)was designed.The discharge frequency and plume length were optimized by the selection of resistance,capacitance,electrode gap,and ground electrode aperture.Results show that the spark plasma plume is generated with a length of 12 mm and a frequency of 10 Hz at a capacitance of 0.33μF.resistance of 1 MΩ,electrode gap of 2 mm,and ground electrode aperture of 1.5 mm.Biological tests indicate that the plasma produced by this device contains abundant reactive species,which can be applied in plasma biomedicine,including daily sterilization and wound healing.

Low-Temperature Plasma Induced Grafting of 2-Methacryloyloxyethyl Phosphorylcholine onto Poly(tetrafluoroethylene) Films

Modification of poly(tetrafluoroethylene)(PTFE) films with 2-methacryloyloxyethyl phosphorylcholine(MPC) was performed by low-temperature plasma treatment and grafting polymerization.Surface properties of PTFE were characterized by attenuated total reflectance Fourier transform infrared(ATR-FTIR) spectra,X-ray photoelectron spectroscopy(XPS) ,and static contact angle.The results show that MPC has been grafted onto PTFE film surface successfully.Contact angle for the modified PTFE films in the water decreased from 108°to 58.25°,while surface energy increased from 17.52 mN/m to 45.47 mN/m.The effects of plasma treatment time,monomer concentration and grafting time on degree of grafting were determined.In the meanwhile,blood compatibility of the PTFE films was studied by checking thrombogenic time of blood plasma.

Sensitivity of two drug-resistant bacteria to low-temperature air plasma in catheterassociated urinary tract infections under different environments

The high incidence of catheter-associated urinary tract infections,which are dominated by drugresistant bacteria,has attracted an increasing number of researchers interested in solving this public health problem.The purpose of this study was to explore the killing effect of lowtemperature air plasma(LTAP)on extended-spectrum beta-lactamase-producing Escherichia coli and high level gentamycin resistance enterococci under two simulated environments in vitro.The results showed that the survival rate of these two kinds of bacteria decreased to less than20%after being treated by LTAP in different environments for 5 min.A comparison of the LTAP treatments showed that the killing efficacy of the two kinds of bacteria in the early stage(0-1 min)was up to 50%.Moreover,the results of transmission electron microscopy,reactive nitrogen species measurement,and a temperature test indicated that the bactericidal effect of the LTAP treatment on the two kinds of bacteria worked through the destruction of the ribosome and other organelles inside the bacteria,rather than the thermal effect,to achieve sterilization.

Destruction of Gaseous Styrene with a Low-Temperature Plasma Induced by a Tubular Multilayer Dielectric Barrier Discharge

The destruction of gaseous styrene was studied using a low-temperature plasma induced by tubular multilayer dielectric barrier discharge（DBD）.The results indicate that the applied voltage,gas flow rate,inlet styrene concentration and reactor configuration play important roles in styrene removal efficiency （ηstyrene） and energy yield（EY）.Values of ηstyrene and EY reached 96%and 15567 mg/kWh when the applied voltage,gas flow rate,inlet styrene concentration and layers of quartz tubes were set at 10.8 kV,5.0 m/s,229 mg/m^3 and 5 layers,respectively.A qualitative analysis of the byproducts and a detailed discussion of the reaction mechanism are also presented.The results could facilitate industrial applications of the new DBD reactor for waste gas treatment.

Remove of Phenolic Compounds in Water by Low-Temperature Plasma: A Review of Current Research

Phenolic compounds have very strong toxicity, so it has been paid sharply attention to find an effective way of controlling the wastewater containing phenolic compounds. The work on this subject done by domestic and overseas scholars is studied in this paper, and the progress of researches on low-temperature plasma treatment is summarized through the electrical discharge types, mechanism, kinetics of phenolic compounds decomposition and combination of several methods with low-temperature plasma treatment. In addition, the crucial problem and the developing tendency on low-temperature plasma treatment for phenol-bearing wastewater are briefly discussed.

Evaluation of the intraoperative trauma degree and postoperative speech function of low-temperature plasma radiofrequency surgery treatment of children with OSAHS

Objective:To evaluate the intraoperative trauma degree and postoperative speech function of low-temperature plasma radiofrequency surgery treatment of children with obstructive sleep apnea hypopnea syndrome (OSAHS).Methods: A total of 118 children with OSAHS were divided into the control group (n=59) who received general surgery and the observation group (n=59) who received the low-temperature plasma radiofrequency surgery according to the random number table. Before operation and 24 h after operation, serum levels of stress hormones, acute phase proteins and inflammatory markers of two groups of children were determined, and the speech function parameter levels were assessed.Results:Before operation, differences in serum contents of stress hormones, acute phase proteins and inflammatory factors as well as speech function parameter levels were not statistically significant between two groups of patients. 24 h after operation, serum stress hormones adrenocorticotropic hormone (ACTH), angiotensin-2 (Ang-2), norepinephrine (NE), cortisol (Cor) contents of observation group were lower than those of control group, serum acute phase proteins haptoglobin (HP), ceruloplasmin (CER), and prealbumin (PA) contents were lower than those of control group, and serum inflammatory factors interleukin-1 (IL-1), interleukin-4 (IL-4), interleukin-27 (IL-27), tumor necrosis factorα(TNF-α) contents were lower than those of control group;speech function parameters NNE and NHR levels of observation group were higher than those of control group.Conclusion:Compared with routine surgery, low-temperature plasma radiofrequency surgery treatment of children with OSAHS causes less surgical trauma and more greatly improves the postoperative speech level.

Continuous Emission Spectrum Measurement for Electron Temperature Determination in Low-Temperature Collisional Plasmas

Continuous emission spectrum measurement is applied for the inconvenient diagnos- tics of low-temperature collisional plasmas. According to the physical mechanism of continuous emission, a simplified model is presented to analyze the spectrum in low temperature plasma. The validity of this model is discussed in a wide range of discharge parameters, including electron tem- perature and ionization degree. Through the simplified model, the continuous emission spectrum in a collisional argon internal inductively coupled plasma is experimentally measured to determine the electron temperature distribution for different gas pressures and radio-frequency powers. The inverse Abel transform is also applied for a better spatially resoluted results. Meanwhile, the result of the continuous emission spectrum measurement is compared to that of the electrostatic double probes, which indicates the effectiveness of this method.

The Feasibility of Applying AC Driven Low-Temperature Plasma for Multi-Cycle Detonation Initiation

Ignition is a key system in pulse detonation engines （PDE）. As advanced ignition methods, nanosecond pulse discharge low-temperature plasma ignition is used in some combustion systems, and continuous alternating current （AC） driven low-temperature plasma using dielectric barrier discharge （DBD） is used for the combustion assistant. However, continuous AC driven plasmas cannot be used for ignition in pulse detonation engines. In this paper, experimental and numerical studies of pneumatic valve PDE using an AC driven low-temperature plasma igniter were described. The pneumatic valve was jointly designed with the low-temperature plasma igniter, and the numerical simulation of the cold-state flow field in the pneumatic valve showed that a complex flow in the discharge area, along with low speed, was beneficial for successful ignition. In the experiments ethylene was used as the fuel and air as oxidizing agent, ignition by an AC driven low-temperature plasma achieved multi-cycle intermittent detonation combustion on a PDE, the working frequency of the PDE reached 15 Hz and the peak pressure of the detonation wave was approximately 2.0 MPa. The experimental verifications of the feasibility in PDE ignition expanded the application field of AC driven low-temperature plasma.

Interaction of supersonic molecular beam with low-temperature plasma

The interaction between the supersonic molecular beam(SMB)and the low-temperature plasma is a critical issue for the diagnosis and fueling in the Tokamak device.In this work,the interaction process between the argon SMB and the argon plasma is studied by a high-speed camera based on the Linear Experimental Advanced Device(LEAD)in Southwestern Institute of Physics,China.It is found that the high-density SMB can extinct the plasma temporarily and change the distribution of the plasma density significantly,while the low-density SMB can hardly affect the distribution of plasma density.This can be used as an effective diagnostic technique to study the evolution of plasma density in the interaction between the SMB and plasma.Moreover,the related simulation based on this experiment is carried out to better understand the evolution of electron density and ion density in the interaction.The simulation results can be used to analyze and explain the experimental results well.

Plasma-assisted surface treatment for low-temperature annealed ohmic contact on AlGaN/GaN heterostructure field-effect transistors

In this study, a low-temperature annealed ohmic contact process was proposed on AlGaN/GaN heterostructure field effect transistors （HFETs） with the assistance of inductively coupled plasma （ICP） surface treatment. The effect of ICP treatment process on the 2DEG channel as well as the formation mechanism of the low annealing temperature ohmic contact was investigated. An appropriate residual AlGaN thickness and a plasma-induced damage are considered to contribute to the low-temperature annealed ohmic contact. By using a single Al layer to replace the conventional Ti/Al stacks, ohmic contact with a contact resistance of 0.35 Ω.mm was obtained when annealed at 575 ℃ for 3 min. Good ohmic contact was also obtained by annealing at 500 ℃ for 20 rain.

Application of persulfate in low-temperature atmospheric-pressure plasma jet for enhanced treatment of onychomycosis

Fungal infection of human nails,or onychomycosis,affects 10%of the world's adult population,but current therapies have various drawbacks.In this work,we employed a self-made low-temperature plasma(LTP)device,namely,an atmospheric-pressure plasma jet(APPJ)device to treat the nails infected with Trichophyton rubrum(T.rubrum)with the aid of persulfate solution.We found that persulfate solution had a promoting effect on plasma treatment of onychomycosis.With addition of sodium persulfate,the APPJ therapy could cure onychomycosis after several times of treatment.As such,this work has demonstrated a novel and effective approach which makes good use of LTP technique in the treatment of onychomycosis.

Progress of International Low-Temperature Plasma Research──Overview of the 15th International Symposium on Plasma Chemistry

International Symposium on Plasma Chemistry (ISPC) is the most influencial in- ternational symposium on science and technology research of low-temperature plasma, especially in the fields related to materials processing. People can be rightly informed of the current devel- oping trend of this field from the contents of these symposia. This paper will introduce briefly a general overview of the 15th ISPC. As viewed from the number of papers and their contents, there is still abundant research on thermal plasma, and the needs fOr micro-electronic technology and high performance films have driven forward continuous and intensive development of the research on low-pressure, non-equilibrium plasmas, while the research on normal pressure, non-equilibrium plasma has become a new highlight in this field.

Ammonia Removal from Wastewater through Combination of Absorption Process in the Membrane Contactor and Advance Oxydation Process in Hybride Plasma-Ozone Reactor

Wastewater containing high concentrations of ammonia can be harmful to aquatic life and degrade the water quality. Wastewater containing ammonia is usually removed by conventional methods such as aeration in towers, biological treatment and adsorption of the ammonium ion to the zeolite surface. However, these methods are less effective and relatively expensive. Therefore there is a need for alternative technologies that can improve the efficiency of ammonia removal from wastewater. This study aims to obtain the process of ammonia removal through a combination of absorption in the membrane contactor and the advance oxidation process in the hybrid plasma-ozone reactor. Wastewater containing ammonia used in the study was a synthetic wastewater with a concentration of about 800 ppm. In the experiment, the wastewater fi＇om the reservoir was firstly passed into the membrane contactor on the shell side, and then mixed with ozone from the ozonator befbre entering the plasma reactor, and finally was circulated back to the reservoir. Meanwhile, the absorbent solution was sent to the lumen fiber in membrane contactor. Experimental results showed that the ammonia removal efficiency increases with increasing in circulation rate and temperature of the wastewater. The highest efficiency of ammonia removal obtained from the experimental results was 77%.