CF3I gas mixtures have attracted considerable attention as potential environmentally-friendly alternatives to SF6 gas,owing to their excellent insulating performance.This paper attempts to study the CF3I ternary gas m...CF3I gas mixtures have attracted considerable attention as potential environmentally-friendly alternatives to SF6 gas,owing to their excellent insulating performance.This paper attempts to study the CF3I ternary gas mixtures with c-C4F8 and buffer gases N2 and CO2 by considering dielectric strength from electron transport parameters based on the Boltzmann method and synergistic effect analysis,compared with SF6 gas mixtures.The results confirm that the critical electric field strength of CF3I/c-C4F8/70%CO2 is greater than that of 30%SF6/70%CO2 when the CF3I content is greater than 17%.Moreover,a higher content of c-C4F8 decreases the sensitivity of gas mixtures to an electric field,and this phenomenon is more obvious in CF3I/c-C4F8/CO2 gas mixtures.The synergistic effects for CF3I/c-C4F8/70%N2 were most obvious when the c-C4F8 content was approximately 20%,and for CF3I/c-C4F8/70%CO2 when the c-C4F8 content was approximately 10%.On the basis of this research,CF3I/c-C4F8/70%N2 shows better insulation performance when the c-C4F8 content is in the15%–20%range.For CF3I/c-C4F8/70%CO2,when the c-C4F8 content is in the 10%–15%range,the gas mixtures have excellent performance.Hence,these gas systems might be used as alternative gas mixtures to SF6 in high-voltage equipment.展开更多
We calculated the uniform dielectric breakdown field strength of residual 30% CF3I/CO2 gas mixtures during the arc extinction process over the temperature range 300-3500 K at 0.1 MPa. The limiting reduced field streng...We calculated the uniform dielectric breakdown field strength of residual 30% CF3I/CO2 gas mixtures during the arc extinction process over the temperature range 300-3500 K at 0.1 MPa. The limiting reduced field strengths are decided by a balance of electron generation and loss based on chemical reactions estimated by the electron energy distribution function （EEDF）, which employs the Boltzmann equation method with two-term expanding approximation in the steady-state Townsend （SST） condition. During the insulation recovery phase, the hot CF3I/CO2 gas mixtures have maximum dielectric strength at a temperature of about 1500 K. At room temperature 300 K, the electric strength after arc extinction （90.3 Td, 1 Td=10-21 V.m2） is only 38% of the original value before arc （234.9 Td）. The adverse insulation recovery ability of CF3I/CO2 gas mixtures in arc extinction hinders its application in electric circuit breakers and other switchgears as an arc quenching and insulating medium.展开更多
The dynamics of negative surface discharges in c-C_(4)F_(8)/CF_(3)I/CO_(2) gas mixture is investigated here with a 2D fuid model.The distributions of ion concentration,electric field strength and photon flux during th...The dynamics of negative surface discharges in c-C_(4)F_(8)/CF_(3)I/CO_(2) gas mixture is investigated here with a 2D fuid model.The distributions of ion concentration,electric field strength and photon flux during the propagation of the streamer are obtained by solving the drift-diffusion equations of particles and Poisson's equation,and the photon flux variation function during the propagation is also fitted.It is found that the streamer branches occur when the streamer transitions from the upper surface of the insulator to the side surface,and then when the streamer approaches the plane electrode,the photon flux will increase significantly.On this basis,the positive and negative surface discharge models are compared in terms of streamer characteristics,particle characteristics and streamer branches.It is found that the streamer has a higher electron concentration and electric field in the positive model.The streamer develops“floating”in the positive surface discharge,while it is close to the surface of the insulator in the negative model.In addition,the negative streamer branch has a wider width and develops further.展开更多
SnO_(2)/Co_(3)O_(4)nanofibers(NFs)are synthesized by using a homopolar electrospinning system with double jets of positive polarity electric fields.The morphology and structure of SnO_(2)/Co_(3)O_(4)hetero-nanofibers ...SnO_(2)/Co_(3)O_(4)nanofibers(NFs)are synthesized by using a homopolar electrospinning system with double jets of positive polarity electric fields.The morphology and structure of SnO_(2)/Co_(3)O_(4)hetero-nanofibers are characterized by using field emission scanning electron microscope(FE-SEM),transmission electron microscope(TEM),x-ray diffraction(XRD),and x-ray photoelectron spectrometer(XPS).The analyses of SnO_(2)/Co_(3)O_(4)NFs by EDS and HRTEM show that the cobalt and tin exist on one nanofiber,which is related to the homopolar electrospinning and the crystallization during sintering.As a typical n-type semiconductor,Sn O_(2)has the disadvantages of high optimal operating temperature and poor reproducibility.Comparing with Sn O_(2),the optimal operating temperature of SnO_(2)/Co_(3)O_(4)NFs is reduced from 350℃to 250℃,which may be related to the catalysis of Co_(2)O_(2).The response of SnO_(2)/Co_(3)O_(4)to 100-ppm ethanol at 250℃is 50.9,9 times higher than that of pure Sn O_(2),which may be attributed to the p–n heterojunction between the n-type Sn O_(2)crystalline grain and the p-type Co_(2)O_(2)crystalline grain.The nanoscale p–n heterojunction promotes the electron migration and forms an interface barrier.The synergy effects between Sn O_(2)and Co_(2)O_(2),the crystalline grain p–n heterojunction,the existence of nanofibers and the large specific surface area all jointly contribute to the improved gas sensing performance.展开更多
Cycloaddition of CO_(2) and epoxide into cyclic carbonate is one of the most efficient ways for CO_(2) conversion with 100% atom-utilization. Metal–organic frameworks are a kind of potential heterogeneous catalysts, ...Cycloaddition of CO_(2) and epoxide into cyclic carbonate is one of the most efficient ways for CO_(2) conversion with 100% atom-utilization. Metal–organic frameworks are a kind of potential heterogeneous catalysts, however, high temperature, high pressure, and high-purity CO_(2) are still required for the reaction.Here, we report two new Zn(Ⅱ) imidazolate frameworks incoporating MoO_(4)^(2–)or WO_(4)^(2–)units, which can catalyse cycloaddition of CO_(2) and epichlorohydrin at room temperature and atomospheric pressure, giving 95% yield after 24 h in pure CO_(2) and 98% yield after 48 h in simulated flue gas(15% CO_(2)+ 85% N_(2)),respectively. For comparison, the analogic Zn(Ⅱ) imidazolate framework MAF-6 without non-3d metal oxide units showed 71% and 33% yields under the same conditions, respectively. The insightful modulation mechanisms of the MoO_(4)^(2–)unit in optimizing the electronic structure of Zn(Ⅱ) centre, facilitating the rate-determined ring opening process, and minimizing the reaction activation energy, were revealed by X-ray photoelectron spectroscopy, temperature programmed desorption and computational calculations.展开更多
CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS acti...CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability.展开更多
This paper presents our study on removal of carbon dioxide(CO_(2)) greenhouse gas emissions by using the mixture of ammonia and soil.CO_(2) capture capacity using this method is 15%higher than the sum of ammonia chemi...This paper presents our study on removal of carbon dioxide(CO_(2)) greenhouse gas emissions by using the mixture of ammonia and soil.CO_(2) capture capacity using this method is 15%higher than the sum of ammonia chemical absorption capacity and soil physical adsorption capacity.Scanning electron microscopy(SEM)and Fourier transform infrared spectroscopy(FTIR)are utilized to study this synergism.The removal effect is not only reflected in ammonia chemical reaction with CO_(2).CO_(2) can also be absorbed by ammonium bicarbonate(NH_(4)HCO_(3)) crystal,which is the main component of the product,or wrapped in the pore of the crystal or packed in the gap between the crystal and the soil.CO_(2) can be permanently deposited as carbonated minerals in the subsoil earth layers.展开更多
Nanomaterials integrated surface acoustic wave(SAW)gas sensing technology has emerged as a promising candidate for realtime toxic gas sensing applications for environmental and human health safety.However,the developm...Nanomaterials integrated surface acoustic wave(SAW)gas sensing technology has emerged as a promising candidate for realtime toxic gas sensing applications for environmental and human health safety.However,the development of novel chemical interface based on two-dimensional(2D)sensing materials for SAW sensors for the rapid and sensitive detection of NH_(3)gas at room temperature(RT)still remains challenging.Herein,we report a highly selective RT NH_(3)gas sensor based on sulfur-doped graphitic carbon nitride quantum dots(S@g-C_(3)N_(4)QD)coated langasite(LGS)SAW sensor with enhanced sensitivity and recovery rate under ultraviolet(UV)illumination.Fascinatingly,the sensitivity of the S@g-C_(3)N_(4)QD/LGS SAW sensor to NH_(3)(500 ppb)at RT is dramatically enhanced by~4.5-fold with a low detection limit(~85 ppb),high selectivity,excellent reproducibility,fast response/recovery time(70 s/79 s)under UV activation(365 nm)as compared to dark condition.Additionally,the proposed sensor exhibited augmented NH_(3)detection capability across the broad range of relative humidity(20%–80%).Such remarkable gas sensing performances of the as-prepared sensor to NH_(3)are attributed to the high surface area,enhanced functional groups,sulfur defects,UV photogenerated charge carriers,facile charge transfer in the S@g-C_(3)N_(4)QD sensing layer,which further helps to improve the gas molecules adsorption that causes the increase in conductivity,resulting in larger frequency responses.The gas sensing mechanism of S@g-C_(3)N_(4)QD/LGS SAW sensor is ascribed to the enhanced electroacoustic effect,which is supported by the correlation of resistive type and COMSOL Multiphysics simulation studies.We envisage that the present work paves a promising strategy to develop the next generation 2D g-C_(3)N_(4)based high responsive RT SAW gas sensors.展开更多
基金supported by National Natural Science Foundation of China(No.51337006)。
文摘CF3I gas mixtures have attracted considerable attention as potential environmentally-friendly alternatives to SF6 gas,owing to their excellent insulating performance.This paper attempts to study the CF3I ternary gas mixtures with c-C4F8 and buffer gases N2 and CO2 by considering dielectric strength from electron transport parameters based on the Boltzmann method and synergistic effect analysis,compared with SF6 gas mixtures.The results confirm that the critical electric field strength of CF3I/c-C4F8/70%CO2 is greater than that of 30%SF6/70%CO2 when the CF3I content is greater than 17%.Moreover,a higher content of c-C4F8 decreases the sensitivity of gas mixtures to an electric field,and this phenomenon is more obvious in CF3I/c-C4F8/CO2 gas mixtures.The synergistic effects for CF3I/c-C4F8/70%N2 were most obvious when the c-C4F8 content was approximately 20%,and for CF3I/c-C4F8/70%CO2 when the c-C4F8 content was approximately 10%.On the basis of this research,CF3I/c-C4F8/70%N2 shows better insulation performance when the c-C4F8 content is in the15%–20%range.For CF3I/c-C4F8/70%CO2,when the c-C4F8 content is in the 10%–15%range,the gas mixtures have excellent performance.Hence,these gas systems might be used as alternative gas mixtures to SF6 in high-voltage equipment.
基金supported by National Natural Science Foundation of China(No.10875093)
文摘We calculated the uniform dielectric breakdown field strength of residual 30% CF3I/CO2 gas mixtures during the arc extinction process over the temperature range 300-3500 K at 0.1 MPa. The limiting reduced field strengths are decided by a balance of electron generation and loss based on chemical reactions estimated by the electron energy distribution function （EEDF）, which employs the Boltzmann equation method with two-term expanding approximation in the steady-state Townsend （SST） condition. During the insulation recovery phase, the hot CF3I/CO2 gas mixtures have maximum dielectric strength at a temperature of about 1500 K. At room temperature 300 K, the electric strength after arc extinction （90.3 Td, 1 Td=10-21 V.m2） is only 38% of the original value before arc （234.9 Td）. The adverse insulation recovery ability of CF3I/CO2 gas mixtures in arc extinction hinders its application in electric circuit breakers and other switchgears as an arc quenching and insulating medium.
基金the National Natural Science Foundation of China(No.62075045)。
文摘The dynamics of negative surface discharges in c-C_(4)F_(8)/CF_(3)I/CO_(2) gas mixture is investigated here with a 2D fuid model.The distributions of ion concentration,electric field strength and photon flux during the propagation of the streamer are obtained by solving the drift-diffusion equations of particles and Poisson's equation,and the photon flux variation function during the propagation is also fitted.It is found that the streamer branches occur when the streamer transitions from the upper surface of the insulator to the side surface,and then when the streamer approaches the plane electrode,the photon flux will increase significantly.On this basis,the positive and negative surface discharge models are compared in terms of streamer characteristics,particle characteristics and streamer branches.It is found that the streamer has a higher electron concentration and electric field in the positive model.The streamer develops“floating”in the positive surface discharge,while it is close to the surface of the insulator in the negative model.In addition,the negative streamer branch has a wider width and develops further.
文摘SnO_(2)/Co_(3)O_(4)nanofibers(NFs)are synthesized by using a homopolar electrospinning system with double jets of positive polarity electric fields.The morphology and structure of SnO_(2)/Co_(3)O_(4)hetero-nanofibers are characterized by using field emission scanning electron microscope(FE-SEM),transmission electron microscope(TEM),x-ray diffraction(XRD),and x-ray photoelectron spectrometer(XPS).The analyses of SnO_(2)/Co_(3)O_(4)NFs by EDS and HRTEM show that the cobalt and tin exist on one nanofiber,which is related to the homopolar electrospinning and the crystallization during sintering.As a typical n-type semiconductor,Sn O_(2)has the disadvantages of high optimal operating temperature and poor reproducibility.Comparing with Sn O_(2),the optimal operating temperature of SnO_(2)/Co_(3)O_(4)NFs is reduced from 350℃to 250℃,which may be related to the catalysis of Co_(2)O_(2).The response of SnO_(2)/Co_(3)O_(4)to 100-ppm ethanol at 250℃is 50.9,9 times higher than that of pure Sn O_(2),which may be attributed to the p–n heterojunction between the n-type Sn O_(2)crystalline grain and the p-type Co_(2)O_(2)crystalline grain.The nanoscale p–n heterojunction promotes the electron migration and forms an interface barrier.The synergy effects between Sn O_(2)and Co_(2)O_(2),the crystalline grain p–n heterojunction,the existence of nanofibers and the large specific surface area all jointly contribute to the improved gas sensing performance.
基金supported by the National Natural Science Foundation of China (Nos. 22090061, 21731007, 21890380 and 22161021)the Guangdong Pearl River Talents Program (No. 2017BT01C161)the support of Jiangxi Province (No. jxsq2018106041)。
文摘Cycloaddition of CO_(2) and epoxide into cyclic carbonate is one of the most efficient ways for CO_(2) conversion with 100% atom-utilization. Metal–organic frameworks are a kind of potential heterogeneous catalysts, however, high temperature, high pressure, and high-purity CO_(2) are still required for the reaction.Here, we report two new Zn(Ⅱ) imidazolate frameworks incoporating MoO_(4)^(2–)or WO_(4)^(2–)units, which can catalyse cycloaddition of CO_(2) and epichlorohydrin at room temperature and atomospheric pressure, giving 95% yield after 24 h in pure CO_(2) and 98% yield after 48 h in simulated flue gas(15% CO_(2)+ 85% N_(2)),respectively. For comparison, the analogic Zn(Ⅱ) imidazolate framework MAF-6 without non-3d metal oxide units showed 71% and 33% yields under the same conditions, respectively. The insightful modulation mechanisms of the MoO_(4)^(2–)unit in optimizing the electronic structure of Zn(Ⅱ) centre, facilitating the rate-determined ring opening process, and minimizing the reaction activation energy, were revealed by X-ray photoelectron spectroscopy, temperature programmed desorption and computational calculations.
基金The research was carried out within the State Assignment of the Ministry of Science and Higher Education of the Russian Federation(project No.FFUG-2024-0036)。
文摘CO_(2) is the most cost-eff ective and abundant carbon resource,while the reverse water-gas reaction(rWGS)is one of the most eff ective methods of CO_(2) utilization.This work presents a comparative study of rWGS activity for perovskite systems based on AFeO_(3)(where A=Ce,La,Y).These systems were synthesized by solution combustion synthesis(SCS)with diff erent ratios of fuel(glycine)and oxidizer(φ),diff erent amounts of NH 4 NO_(3),and the addition of alumina or silica as supports.Various techniques,including X-ray diff raction analysis,thermogravimetric analysis,Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy,energy-dispersive X-ray spectroscopy,N 2-physisorption,H_(2) temper-ature-programmed reduction,temperature-programmed desorption of H_(2) and CO_(2),Raman spectroscopy,and in situ FTIR,were used to relate the physicochemical properties with the catalytic performance of the obtained composites.Each specifi c perovskite-containing system(either bulk or supported)has its own optimalφand NH_(4) NO_(3) amount to achieve the highest yield and dispersion of the perovskite phase.Among all synthesized systems,bulk SCS-derived La-Fe-O systems showed the highest resistance to reducing environments and the easiest hydrogen desorption,outperforming La-Fe-O produced by solgel combustion(SGC).CO_(2) conversion into CO at 600°C for bulk ferrite systems,depending on the A-cation type and preparation method,follows the order La(SGC)<Y<Ce<La(SCS).The diff erences in properties between La-Fe-O obtained by the SCS and SGC methods can be attributed to diff erent ratios of oxygen and lanthanum vacancy contributions,hydroxyl coverage,morphology,and free iron oxide presence.In situ FTIR data revealed that CO_(2) hydrogenation occurs through formates generated under reaction conditions on the bulk system based on La-Fe-O,obtained by the SCS method.γ-Al_(2)O_(3) improves the dispersion of CeFeO_(3) and LaFeO_(3) phases,the specifi c surface area,and the quantity of adsorbed H_(2) and CO_(2).This led to a signifi cant increase in CO_(2) conversion for supported CeFeO_(3) but not for the La-based system compared to bulk and SiO_(2)-supported perovskite catalysts.However,adding alumina increased the activity per mass for both Ce-and La-based perovskite systems,reducing the amount of rare-earth components in the catalyst and thereby lowering the cost without substantially compromising stability.
基金the support by the National Development Programming of Key Fundamental Researches of China(2004CB217700)Program for Changjiang Scholars and Innovative Research Team of Ministry of Education(PCSIRT-IRT0620)Subsidy Scheme of Outstanding Academic Leaders in Shanghai(08XD1401300).
文摘This paper presents our study on removal of carbon dioxide(CO_(2)) greenhouse gas emissions by using the mixture of ammonia and soil.CO_(2) capture capacity using this method is 15%higher than the sum of ammonia chemical absorption capacity and soil physical adsorption capacity.Scanning electron microscopy(SEM)and Fourier transform infrared spectroscopy(FTIR)are utilized to study this synergism.The removal effect is not only reflected in ammonia chemical reaction with CO_(2).CO_(2) can also be absorbed by ammonium bicarbonate(NH_(4)HCO_(3)) crystal,which is the main component of the product,or wrapped in the pore of the crystal or packed in the gap between the crystal and the soil.CO_(2) can be permanently deposited as carbonated minerals in the subsoil earth layers.
基金the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2020R1A2C2013385)Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(No.NRF-2020R1A6A1A03047771)Korea Institute of Planning and Evaluation for Technology in Food,Agriculture and Forestry(IPET),Korea Smart Farm Research and Development Foundation(KosFarm)through Smart Farm Innovation Technology Development Program,funded by Ministry of Agriculture,Food,and Rural Affairs(MAFRA)and Ministry of Science and ICT(MSIT),Rural Development Administration(RDA)(No.421029-4).
文摘Nanomaterials integrated surface acoustic wave(SAW)gas sensing technology has emerged as a promising candidate for realtime toxic gas sensing applications for environmental and human health safety.However,the development of novel chemical interface based on two-dimensional(2D)sensing materials for SAW sensors for the rapid and sensitive detection of NH_(3)gas at room temperature(RT)still remains challenging.Herein,we report a highly selective RT NH_(3)gas sensor based on sulfur-doped graphitic carbon nitride quantum dots(S@g-C_(3)N_(4)QD)coated langasite(LGS)SAW sensor with enhanced sensitivity and recovery rate under ultraviolet(UV)illumination.Fascinatingly,the sensitivity of the S@g-C_(3)N_(4)QD/LGS SAW sensor to NH_(3)(500 ppb)at RT is dramatically enhanced by~4.5-fold with a low detection limit(~85 ppb),high selectivity,excellent reproducibility,fast response/recovery time(70 s/79 s)under UV activation(365 nm)as compared to dark condition.Additionally,the proposed sensor exhibited augmented NH_(3)detection capability across the broad range of relative humidity(20%–80%).Such remarkable gas sensing performances of the as-prepared sensor to NH_(3)are attributed to the high surface area,enhanced functional groups,sulfur defects,UV photogenerated charge carriers,facile charge transfer in the S@g-C_(3)N_(4)QD sensing layer,which further helps to improve the gas molecules adsorption that causes the increase in conductivity,resulting in larger frequency responses.The gas sensing mechanism of S@g-C_(3)N_(4)QD/LGS SAW sensor is ascribed to the enhanced electroacoustic effect,which is supported by the correlation of resistive type and COMSOL Multiphysics simulation studies.We envisage that the present work paves a promising strategy to develop the next generation 2D g-C_(3)N_(4)based high responsive RT SAW gas sensors.
