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 propagat...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.展开更多
The thermal degradation of two synthetic lubricants base oils, poly-a-olefins （PAO） and di-esters （DE）, was investigated under oxidative pyrolysis condition and their properties were characterized in simulated ＂a...The thermal degradation of two synthetic lubricants base oils, poly-a-olefins （PAO） and di-esters （DE）, was investigated under oxidative pyrolysis condition and their properties were characterized in simulated ＂areo-engine＂ by comparing the thermal stability and identifying the products of thermal decomposition as a function of exposure temperature. The characterization of the products were performed by means of Fourier transform infrared spectrometry （FTIR）, gas chromatography/mass spectrometry （GC/MS） and viscosity experiments. The results show that PAO has the lower thermal stability, being degraded at 200℃ different from 300 ℃ for DE. Several by-products are identified during the thermal degradation of two lubricant base oils. The majority of PAO products consist of alkenes and olefins, while more oxygen-contained organic compounds are detected in DE samples based on GC/MS analysis. The related reaction mechanisms are discussed based on the experimental results.展开更多
Pyrolysis is a cost-effective and safe method for the disposal of radioactive spent resins.In this work,the catalytic effects of V_(2)O_(5) on the pyrolysis of cation exchange resin are investigated for the first time...Pyrolysis is a cost-effective and safe method for the disposal of radioactive spent resins.In this work,the catalytic effects of V_(2)O_(5) on the pyrolysis of cation exchange resin are investigated for the first time.The results show that it is a better catalyst than others so far studied and achieves a lowering of final pyrolysis temperature and residual rate simultaneously when aided by physical blending.The maximum reductions of the final pyrolysis temperature and the residual rate are 173℃and 11.9%(in weight),respectively.Under the action of V_(2)O_(5),low-temperature(445℃)removal of partial sulfonic acid groups occurs and the pyrolysis of the resin copolymer matrix is promoted.This is demonstrated by the analysis of pyrolysis residues at different temperatures by X-ray photoelectron spectroscopy(XPS)and element analysis.The catalytic activity of V_(2)O_(5) is determined by effects both at acid sites and oxidation-reduction centers via H2-TPR(temperature programmed reduction),V_(2)-TPD(temperature programmed desorption),CV_(2)-TPD,and NH3-TPD.The catalytic effect of oxidation-reduction centers in V_(2)O_(5) is achieved by close contact with the sulfur bond through chemisorption under the effect of acid sites.V_(2)O_(5) is also believed to be the reason for the removal of partial sulfonic acid groups at lower temperatures(445℃).V_(2)O_(5) is an effective catalyst for spent resin pyrolysis and can be further applied in industry.展开更多
The physiochemical properties of chars produced by coal pyrolysis in a laboratory-scale fluidized bed reactor with a continuous coal feed and char discharge at temperatures of 750 to 980 ~ C under N2-based atmospheres...The physiochemical properties of chars produced by coal pyrolysis in a laboratory-scale fluidized bed reactor with a continuous coal feed and char discharge at temperatures of 750 to 980 ~ C under N2-based atmospheres containing 02, H2, CO, CH4, and CO2 were studied. The specific surface area of the char was found to decrease with increasing pyrolysis temperature. The interlayer spacing of the char also decreased, while the average stacking height and carbon crystal size increased at higher temperatures, suggesting that the char generated at high temperatures had a highly ordered structure. The char obtained using an ER value of 0.064 exhibited the highest specific surface area and oxidation reactivity. Rela- tively high 02 concentrations degraded the pore structure of the char, decreasing the surface area. The char produced in an atmosphere incorporating H2 showed a more condensed crystalline structure and consequently had lower oxidation reactivity.展开更多
基金the grant support from the National Natural Science Foundation of China (No. 21975018, 22278032)。
文摘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.
基金Supported by the Fund from the Air Force Armament Department of China for Innovative Research Group(Grant KJ2012283)
文摘The thermal degradation of two synthetic lubricants base oils, poly-a-olefins （PAO） and di-esters （DE）, was investigated under oxidative pyrolysis condition and their properties were characterized in simulated ＂areo-engine＂ by comparing the thermal stability and identifying the products of thermal decomposition as a function of exposure temperature. The characterization of the products were performed by means of Fourier transform infrared spectrometry （FTIR）, gas chromatography/mass spectrometry （GC/MS） and viscosity experiments. The results show that PAO has the lower thermal stability, being degraded at 200℃ different from 300 ℃ for DE. Several by-products are identified during the thermal degradation of two lubricant base oils. The majority of PAO products consist of alkenes and olefins, while more oxygen-contained organic compounds are detected in DE samples based on GC/MS analysis. The related reaction mechanisms are discussed based on the experimental results.
基金Project supported by the National Natural Science Foundation of China(No.U1862203)the National Science Fund for Distinguished Young Scholars(No.21525627)the Science Fund for Creative Research Groups of National Natural Science Foundation of China(No.61621002)。
文摘Pyrolysis is a cost-effective and safe method for the disposal of radioactive spent resins.In this work,the catalytic effects of V_(2)O_(5) on the pyrolysis of cation exchange resin are investigated for the first time.The results show that it is a better catalyst than others so far studied and achieves a lowering of final pyrolysis temperature and residual rate simultaneously when aided by physical blending.The maximum reductions of the final pyrolysis temperature and the residual rate are 173℃and 11.9%(in weight),respectively.Under the action of V_(2)O_(5),low-temperature(445℃)removal of partial sulfonic acid groups occurs and the pyrolysis of the resin copolymer matrix is promoted.This is demonstrated by the analysis of pyrolysis residues at different temperatures by X-ray photoelectron spectroscopy(XPS)and element analysis.The catalytic activity of V_(2)O_(5) is determined by effects both at acid sites and oxidation-reduction centers via H2-TPR(temperature programmed reduction),V_(2)-TPD(temperature programmed desorption),CV_(2)-TPD,and NH3-TPD.The catalytic effect of oxidation-reduction centers in V_(2)O_(5) is achieved by close contact with the sulfur bond through chemisorption under the effect of acid sites.V_(2)O_(5) is also believed to be the reason for the removal of partial sulfonic acid groups at lower temperatures(445℃).V_(2)O_(5) is an effective catalyst for spent resin pyrolysis and can be further applied in industry.
文摘The physiochemical properties of chars produced by coal pyrolysis in a laboratory-scale fluidized bed reactor with a continuous coal feed and char discharge at temperatures of 750 to 980 ~ C under N2-based atmospheres containing 02, H2, CO, CH4, and CO2 were studied. The specific surface area of the char was found to decrease with increasing pyrolysis temperature. The interlayer spacing of the char also decreased, while the average stacking height and carbon crystal size increased at higher temperatures, suggesting that the char generated at high temperatures had a highly ordered structure. The char obtained using an ER value of 0.064 exhibited the highest specific surface area and oxidation reactivity. Rela- tively high 02 concentrations degraded the pore structure of the char, decreasing the surface area. The char produced in an atmosphere incorporating H2 showed a more condensed crystalline structure and consequently had lower oxidation reactivity.
