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 nont...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.展开更多
C1 chemistrymainly involves the catalytic transformation of C1molecules(i.e.,CO,CO2,CH4 and CH3OH),which usually encounters thermodynamic and/or kinetic limitations.To address these limitations,non-thermal plasma(NTP)...C1 chemistrymainly involves the catalytic transformation of C1molecules(i.e.,CO,CO2,CH4 and CH3OH),which usually encounters thermodynamic and/or kinetic limitations.To address these limitations,non-thermal plasma(NTP)activated heterogeneous catalysis offers a number of advantages,such as relatively mild reaction conditions and energy efficiency,in comparison to the conventional thermal catalysis.This review presents the state-of-the-art for the application of NTP-catalysis towards C1 chemistry,including the CO2 hydrogenation,reforming of CH4 and CH3OH,and water-gas shift(WGS)reaction.In the hybrid NTP-catalyst system,the plasma-catalyst interactions aremultifaceted.Accordingly,this reviewalso includes a brief discussion on the fundamental research into themechanisms of NTP activated catalytic C1 chemistry,such as the advanced characterisation methods(e.g.,in situ diffuse reflectance infrared Fourier transform spectroscopy,DRIFTS),temperatureprogrammed plasma surface reaction(TPPSR),kinetic studies.Finally,prospects for the future research on the development of tailor-made catalysts for NTP-catalysis systems(which will enable the further understanding of its mechanism)and the translation of the hybrid technique to practical applications of catalytic C1 chemistry are discussed.展开更多
Plasma-catalytic dry reforming of CH_(4)(DRM) is promising to convert the greenhouse gasses CH_(4) and CO_(2) into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock f...Plasma-catalytic dry reforming of CH_(4)(DRM) is promising to convert the greenhouse gasses CH_(4) and CO_(2) into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products,because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex,as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, high-lighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems.Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures,at which vibrational excitation can enhance the surface reactions.展开更多
This study investigates the dry reformation of methane(DRM)over Ni/Al_(2)O_(3)catalysts in a dielectric barrier discharge(DBD)non-thermal plasma reactor.A novel hybrid machine learning(ML)model is developed to optimiz...This study investigates the dry reformation of methane(DRM)over Ni/Al_(2)O_(3)catalysts in a dielectric barrier discharge(DBD)non-thermal plasma reactor.A novel hybrid machine learning(ML)model is developed to optimize the plasma-catalytic DRM reaction with limited experimental data.To address the non-linear and complex nature of the plasma-catalytic DRM process,the hybrid ML model integrates three well-established algorithms:regression trees,support vector regression,and artificial neural networks.A genetic algorithm(GA)is then used to optimize the hyperparameters of each algorithm within the hybrid ML model.The ML model achieved excellent agreement with the experimental data,demonstrating its efficacy in accurately predicting and optimizing the DRM process.The model was subsequently used to investigate the impact of various operating parameters on the plasma-catalytic DRM performance.We found that the optimal discharge power(20 W),CO_(2)/CH_(4)molar ratio(1.5),and Ni loading(7.8 wt%)resulted in the maximum energy yield at a total flow rate of∼51 mL/min.Furthermore,we investigated the relative significance of each operating parameter on the performance of the plasma-catalytic DRM process.The results show that the total flow rate had the greatest influence on the conversion,with a significance exceeding 35%for each output,while the Ni loading had the least impact on the overall reaction performance.This hybrid model demonstrates a remarkable ability to extract valuable insights from limited datasets,enabling the development and optimization of more efficient and selective plasma-catalytic chemical processes.展开更多
Diesel particulate matter(DPM)and hydrocarbons(HCs)emitted from diesel engines have a negative affect on air quality and human health.Catalysts for oxidative removal of DPM and HCs are currently used universally but t...Diesel particulate matter(DPM)and hydrocarbons(HCs)emitted from diesel engines have a negative affect on air quality and human health.Catalysts for oxidative removal of DPM and HCs are currently used universally but their low removal efficiency at low temperatures is a problem.In this study,Cu-doped CeO_(2) loaded on Al_(2)O_(3) coupled with plasma was used to enhance low-temperature oxidation of DPM and HCs.Removals of DPM and HCs at 200℃ using the catalyst were as high as 90%with plasma but below 30%without plasma.Operando plasma diffuse reflectance infrared Fourier transform spectroscopy coupled with mass spectrometry was conducted to reveal the functional mechanism of the oxygen species in the DPM oxidation process.It was found that Cu-CeO_(2) can promote the formation of adsorbed oxygen(M^(+)-O_(2)^(-))and terminal oxygen(M=O),which can react with DPM to form carbonates that are easily converted to gaseous CO_(2).Our results provide a practical plasma catalysis technology to obtain simultaneous removals of DPM and HCs at low temperatures.M+O-2Diesel particulate matter(DPM)and hydrocarbons(HCs)emitted from diesel engines have a negative affect on air quality and human health.Catalysts for oxidative removal of DPM and HCs are currently used universally but their low removal efficiency at low temperatures is a problem.In this study,Cu-doped CeO_(2) loaded on Al_(2)O_(3) coupled with plasma was used to enhance low-temperature oxidation of DPM and HCs.Removals of DPM and HCs at 200°C using the catalyst were as high as 90%with plasma but below 30%without plasma.Operando plasma diffuse reflectance infrared Fourier transform spectroscopy coupled with mass spectrometry was conducted to reveal the functional mechanism of the oxygen species in the DPM oxidation process.It was found that Cu–CeO_(2) can promote the formation of adsorbed oxygen(–)and terminal oxygen(M=O),which can react with DPM to form carbonates that are easily converted to gaseous CO_(2).Our results provide a practical plasma catalysis technology to obtain simultaneous removals of DPM and HCs at low temperatures.展开更多
In this paper the effect of catalyst and carrier in electric field enhanced plasma on methane conversion into C2 hydrocarbons was investigated. Methane coupling reaction was studied in the system of continuous flow r...In this paper the effect of catalyst and carrier in electric field enhanced plasma on methane conversion into C2 hydrocarbons was investigated. Methane coupling reaction was studied in the system of continuous flow reactor on Ni, MoO3, MnO2 catalysts and different ZSM-5 carriers. The per pass conversion of methane can be as high as 22%, the selectivity of ethylene can be as high as 23.8%, of acetylene 60.8%, of ethane 5.4% and of total C2 hydrocarbons was more than 90%. ZSM-5-25 was the better carrier and MnO2 was the better active component. The efficiency of energy was as high as 7.81%.展开更多
Methane partial oxidation to methanol （MPOM） using dielectric barrier discharge over a Fe2O3-CuO/γ-Al2O3 catalyst was performed.The multicomponent catalyst was combined with plasma in two different configurations,i...Methane partial oxidation to methanol （MPOM） using dielectric barrier discharge over a Fe2O3-CuO/γ-Al2O3 catalyst was performed.The multicomponent catalyst was combined with plasma in two different configurations,i.e.,in-plasma catalysis （IPC） and post-plasma catalysis （PPC）.It was found that the catalytic performance of the catalysts for MPOM was strongly dependent on the hybrid configuration.A better synergistic performance of plasma and catalysis was achieved in the IPC configuration,but the catalysts packed in the discharge zone showed lower stability than those connected to the discharge zone in sequence.Active species,such as ozone,atomic oxygen and methyl radicals,were produced from the plasma-catalysis process,and made a major contribution to methanol synthesis.These active species were identified by the means of in situ optical emission spectra,ozone measurement and FT-IR spectra.It was confirmed that the amount of active species in the IPC system was greater than that in the PPC system.The results of TG,XRD,and N2 adsorption-desorption revealed that carbon deposition on the spent catalyst surface was responsible for the catalyst deactivation in the IPC configuration.展开更多
A study of the behaviors of air discharge plasma inside a catalyst’s pores is important to understand the plasma catalysis mechanism;however,few articles have reported the generation characteristics of air plasma in ...A study of the behaviors of air discharge plasma inside a catalyst’s pores is important to understand the plasma catalysis mechanism;however,few articles have reported the generation characteristics of air plasma in the pores of catalysts.The production of air microdischarge in a pore was studied by a two-dimensional fluid model,mainly focusing on the effect of pore size and applied voltage.The results show that an increase in the pore size in the range of 20–100μm facilitates the occurrence of microdischarge in the pore.In addition,at an applied voltage of 9 kV,the ionization of air mainly occurs near the topside of the pore when the pore diameter is less than 20μm,leading to a low plasma density in the pore,but the time-averaged plasma density in the pore reaches a maximum value at a 70μm pore diameter.Moreover,the applied voltage also has an important effect on the production of air microdischarge in the pore.The existence of a pore of 80μm diameter on the dielectric has no obvious influence on the plasma density in the pore at 2 kV applied voltage,but the plasma density in the pore begins to sharply rise when the voltage exceeds 3 kV due to the enhanced air ionization at higher applied voltage.The study indicates that microdischarge can be generated in a pore with a size of tens of micrometers,and the microdischarge in porous catalysts will affect the catalytic degradation efficacy of gaseous pollutants.展开更多
Catalysis of molecular radicals is often performed in interesting experimental configurations.One possible configuration is tubular geometry.The radicals are introduced into the tubes on one side,and stable molecules ...Catalysis of molecular radicals is often performed in interesting experimental configurations.One possible configuration is tubular geometry.The radicals are introduced into the tubes on one side,and stable molecules are exhausted on the other side.The penetration depth of radicals depends on numerous parameters,so it is not always feasible to calculate it.This article presents systematic measurements of the penetration depth of oxygen atoms along tubes made from nickel,cobalt,and copper.The source of O atoms was a surfatron-type microwave plasma.The initial density of O atoms depended on the gas flow and was 0.7×10^(21)m^(-3),2.4×10^(21)m^(-3),and 4.2×10^(21)m^(-3)at the flow rates of 50,300,and 600 sccm,and pressures of 10,35,and 60 Pa,respectively.The gas temperature remained at room temperature throughout the experiments.The dissociation fraction decreased exponentially along the length of the tubes in all cases.The penetration depths for well-oxidized nickel were 1.2,1.7,and 2.4 cm,respectively.For cobalt,they were slightly lower at 1.0,1.3,and 1.6 cm,respectively,while for copper,they were 1.1,1.3,and 1.7 cm,respectively.The results were explained by gas dynamics and heterogeneous surface association.These data are useful in any attempt to estimate the loss of molecular fragments along tubes,which serve as catalysts for the association of various radicals to stable molecules.展开更多
This paper is aimed to investigate the effect of packing material on plasma characteristic from the viewpoint of charge transfer process.Both the charge accumulation and release processes in the dielectric barrier dis...This paper is aimed to investigate the effect of packing material on plasma characteristic from the viewpoint of charge transfer process.Both the charge accumulation and release processes in the dielectric barrier discharge reactor and packed-bed reactor were investigated by measuring voltage and current waveforms and taking ICCD images.The packing material was ZrO2 pellets and the reactors were driven by a parameterized nanosecond pulse source.The quantity of transferred charges in the dielectric barrier discharge reactor was enhanced when decreasing pulse rise time or increasing pulse width(within 150 ns),but reduced when the gas gap was packed with pellets.The quantity of accumulated charges in the primary discharge was larger than the quantity of released charges in the secondary discharges in the dielectric barrier discharge reactor,but they were almost equal in the packed-bed reactor.It indicates that the discharge behavior has been changed from the view of charge transfer process once the gas gap was packed with pellets,and the ICCD images confirmed it.展开更多
基金partially supported by the Australian Research Council(ARC)the National Science Fund for Distinguished Young Scholars(grant number 51925703)。
文摘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.
基金the financial support from the Jiangsu Specially-Appointed Professors Program and the European Commission under the Marie Skłodowska-Curie Individual Fellowship(H2020-MSCA-IFNTPleasure-748196).
文摘C1 chemistrymainly involves the catalytic transformation of C1molecules(i.e.,CO,CO2,CH4 and CH3OH),which usually encounters thermodynamic and/or kinetic limitations.To address these limitations,non-thermal plasma(NTP)activated heterogeneous catalysis offers a number of advantages,such as relatively mild reaction conditions and energy efficiency,in comparison to the conventional thermal catalysis.This review presents the state-of-the-art for the application of NTP-catalysis towards C1 chemistry,including the CO2 hydrogenation,reforming of CH4 and CH3OH,and water-gas shift(WGS)reaction.In the hybrid NTP-catalyst system,the plasma-catalyst interactions aremultifaceted.Accordingly,this reviewalso includes a brief discussion on the fundamental research into themechanisms of NTP activated catalytic C1 chemistry,such as the advanced characterisation methods(e.g.,in situ diffuse reflectance infrared Fourier transform spectroscopy,DRIFTS),temperatureprogrammed plasma surface reaction(TPPSR),kinetic studies.Finally,prospects for the future research on the development of tailor-made catalysts for NTP-catalysis systems(which will enable the further understanding of its mechanism)and the translation of the hybrid technique to practical applications of catalytic C1 chemistry are discussed.
基金supported by the FWO-SBO project PlasMaCatDESIGN (FWO grant ID S001619N)the FWO fellowship of R. Michiels (FWO grant ID 1114921N)+2 种基金the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project)funded by the Research Foundation - Flanders (FWO)the Flemish Government。
文摘Plasma-catalytic dry reforming of CH_(4)(DRM) is promising to convert the greenhouse gasses CH_(4) and CO_(2) into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products,because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex,as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, high-lighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems.Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures,at which vibrational excitation can enhance the surface reactions.
基金This project received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No. 813393the funding from the National Natural Science Foundation of China (No. 52177149)
文摘This study investigates the dry reformation of methane(DRM)over Ni/Al_(2)O_(3)catalysts in a dielectric barrier discharge(DBD)non-thermal plasma reactor.A novel hybrid machine learning(ML)model is developed to optimize the plasma-catalytic DRM reaction with limited experimental data.To address the non-linear and complex nature of the plasma-catalytic DRM process,the hybrid ML model integrates three well-established algorithms:regression trees,support vector regression,and artificial neural networks.A genetic algorithm(GA)is then used to optimize the hyperparameters of each algorithm within the hybrid ML model.The ML model achieved excellent agreement with the experimental data,demonstrating its efficacy in accurately predicting and optimizing the DRM process.The model was subsequently used to investigate the impact of various operating parameters on the plasma-catalytic DRM performance.We found that the optimal discharge power(20 W),CO_(2)/CH_(4)molar ratio(1.5),and Ni loading(7.8 wt%)resulted in the maximum energy yield at a total flow rate of∼51 mL/min.Furthermore,we investigated the relative significance of each operating parameter on the performance of the plasma-catalytic DRM process.The results show that the total flow rate had the greatest influence on the conversion,with a significance exceeding 35%for each output,while the Ni loading had the least impact on the overall reaction performance.This hybrid model demonstrates a remarkable ability to extract valuable insights from limited datasets,enabling the development and optimization of more efficient and selective plasma-catalytic chemical processes.
基金supported by National Natural Science Foundation of China(nos 12075037 and 22206013)。
文摘Diesel particulate matter(DPM)and hydrocarbons(HCs)emitted from diesel engines have a negative affect on air quality and human health.Catalysts for oxidative removal of DPM and HCs are currently used universally but their low removal efficiency at low temperatures is a problem.In this study,Cu-doped CeO_(2) loaded on Al_(2)O_(3) coupled with plasma was used to enhance low-temperature oxidation of DPM and HCs.Removals of DPM and HCs at 200℃ using the catalyst were as high as 90%with plasma but below 30%without plasma.Operando plasma diffuse reflectance infrared Fourier transform spectroscopy coupled with mass spectrometry was conducted to reveal the functional mechanism of the oxygen species in the DPM oxidation process.It was found that Cu-CeO_(2) can promote the formation of adsorbed oxygen(M^(+)-O_(2)^(-))and terminal oxygen(M=O),which can react with DPM to form carbonates that are easily converted to gaseous CO_(2).Our results provide a practical plasma catalysis technology to obtain simultaneous removals of DPM and HCs at low temperatures.M+O-2Diesel particulate matter(DPM)and hydrocarbons(HCs)emitted from diesel engines have a negative affect on air quality and human health.Catalysts for oxidative removal of DPM and HCs are currently used universally but their low removal efficiency at low temperatures is a problem.In this study,Cu-doped CeO_(2) loaded on Al_(2)O_(3) coupled with plasma was used to enhance low-temperature oxidation of DPM and HCs.Removals of DPM and HCs at 200°C using the catalyst were as high as 90%with plasma but below 30%without plasma.Operando plasma diffuse reflectance infrared Fourier transform spectroscopy coupled with mass spectrometry was conducted to reveal the functional mechanism of the oxygen species in the DPM oxidation process.It was found that Cu–CeO_(2) can promote the formation of adsorbed oxygen(–)and terminal oxygen(M=O),which can react with DPM to form carbonates that are easily converted to gaseous CO_(2).Our results provide a practical plasma catalysis technology to obtain simultaneous removals of DPM and HCs at low temperatures.
基金Supports from the National Natural Science Foundation of China(No 29776037)
文摘In this paper the effect of catalyst and carrier in electric field enhanced plasma on methane conversion into C2 hydrocarbons was investigated. Methane coupling reaction was studied in the system of continuous flow reactor on Ni, MoO3, MnO2 catalysts and different ZSM-5 carriers. The per pass conversion of methane can be as high as 22%, the selectivity of ethylene can be as high as 23.8%, of acetylene 60.8%, of ethane 5.4% and of total C2 hydrocarbons was more than 90%. ZSM-5-25 was the better carrier and MnO2 was the better active component. The efficiency of energy was as high as 7.81%.
基金supported by the National Natural Science Foundation of China(No. 20836008 and U0633003)the Zhejiang Provincial Natural Science Foundation of China(No. Y5080192)+3 种基金the Project of Science and Technology Department of Zhejiang Province of China(2007C13061)MOST Project of China(No. 2007AA06Z339,No. 2008BAC32B06 and No. 2007AA06A409)the Open Project Program of Key Laboratory of Non-point Sources Pollution Controlthe Ministry of Agriculture of the People’s Republic of China and Science Foundation of Chinese University
文摘Methane partial oxidation to methanol （MPOM） using dielectric barrier discharge over a Fe2O3-CuO/γ-Al2O3 catalyst was performed.The multicomponent catalyst was combined with plasma in two different configurations,i.e.,in-plasma catalysis （IPC） and post-plasma catalysis （PPC）.It was found that the catalytic performance of the catalysts for MPOM was strongly dependent on the hybrid configuration.A better synergistic performance of plasma and catalysis was achieved in the IPC configuration,but the catalysts packed in the discharge zone showed lower stability than those connected to the discharge zone in sequence.Active species,such as ozone,atomic oxygen and methyl radicals,were produced from the plasma-catalysis process,and made a major contribution to methanol synthesis.These active species were identified by the means of in situ optical emission spectra,ozone measurement and FT-IR spectra.It was confirmed that the amount of active species in the IPC system was greater than that in the PPC system.The results of TG,XRD,and N2 adsorption-desorption revealed that carbon deposition on the spent catalyst surface was responsible for the catalyst deactivation in the IPC configuration.
基金National Natural Science Foundation of China(Nos.51977024 and 21577011).
文摘A study of the behaviors of air discharge plasma inside a catalyst’s pores is important to understand the plasma catalysis mechanism;however,few articles have reported the generation characteristics of air plasma in the pores of catalysts.The production of air microdischarge in a pore was studied by a two-dimensional fluid model,mainly focusing on the effect of pore size and applied voltage.The results show that an increase in the pore size in the range of 20–100μm facilitates the occurrence of microdischarge in the pore.In addition,at an applied voltage of 9 kV,the ionization of air mainly occurs near the topside of the pore when the pore diameter is less than 20μm,leading to a low plasma density in the pore,but the time-averaged plasma density in the pore reaches a maximum value at a 70μm pore diameter.Moreover,the applied voltage also has an important effect on the production of air microdischarge in the pore.The existence of a pore of 80μm diameter on the dielectric has no obvious influence on the plasma density in the pore at 2 kV applied voltage,but the plasma density in the pore begins to sharply rise when the voltage exceeds 3 kV due to the enhanced air ionization at higher applied voltage.The study indicates that microdischarge can be generated in a pore with a size of tens of micrometers,and the microdischarge in porous catalysts will affect the catalytic degradation efficacy of gaseous pollutants.
基金funded by the Slovenian Research Agency,Core Funding(No.P2-0082)and Project(No.L24487)。
文摘Catalysis of molecular radicals is often performed in interesting experimental configurations.One possible configuration is tubular geometry.The radicals are introduced into the tubes on one side,and stable molecules are exhausted on the other side.The penetration depth of radicals depends on numerous parameters,so it is not always feasible to calculate it.This article presents systematic measurements of the penetration depth of oxygen atoms along tubes made from nickel,cobalt,and copper.The source of O atoms was a surfatron-type microwave plasma.The initial density of O atoms depended on the gas flow and was 0.7×10^(21)m^(-3),2.4×10^(21)m^(-3),and 4.2×10^(21)m^(-3)at the flow rates of 50,300,and 600 sccm,and pressures of 10,35,and 60 Pa,respectively.The gas temperature remained at room temperature throughout the experiments.The dissociation fraction decreased exponentially along the length of the tubes in all cases.The penetration depths for well-oxidized nickel were 1.2,1.7,and 2.4 cm,respectively.For cobalt,they were slightly lower at 1.0,1.3,and 1.6 cm,respectively,while for copper,they were 1.1,1.3,and 1.7 cm,respectively.The results were explained by gas dynamics and heterogeneous surface association.These data are useful in any attempt to estimate the loss of molecular fragments along tubes,which serve as catalysts for the association of various radicals to stable molecules.
基金supported by the National Science Fund for Distinguished Young Scholars(No.51925703)National Natural Science Foundation of China(Nos.51637010,51707186 and 51807190)。
文摘This paper is aimed to investigate the effect of packing material on plasma characteristic from the viewpoint of charge transfer process.Both the charge accumulation and release processes in the dielectric barrier discharge reactor and packed-bed reactor were investigated by measuring voltage and current waveforms and taking ICCD images.The packing material was ZrO2 pellets and the reactors were driven by a parameterized nanosecond pulse source.The quantity of transferred charges in the dielectric barrier discharge reactor was enhanced when decreasing pulse rise time or increasing pulse width(within 150 ns),but reduced when the gas gap was packed with pellets.The quantity of accumulated charges in the primary discharge was larger than the quantity of released charges in the secondary discharges in the dielectric barrier discharge reactor,but they were almost equal in the packed-bed reactor.It indicates that the discharge behavior has been changed from the view of charge transfer process once the gas gap was packed with pellets,and the ICCD images confirmed it.
