We report the investigation on the low-temperature oxidation of cyclohexane in a jet-stirred reactor over 500-742 K. Synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) was used for identify...We report the investigation on the low-temperature oxidation of cyclohexane in a jet-stirred reactor over 500-742 K. Synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) was used for identifying and quantifying the oxidation species. Major products, cyclic olefins, and oxygenated products including reactive hydroperoxides and high oxygen compounds were detected. Compared with n-alkanes, a narrow low-temperature window (-80 K) was observed in the low-temperature oxidation of cyclohexane. Besides, a kinetic model for cyclohexane oxidation was developed based on the CNRS model [Combust. Flame 160, 2319 (2013)], which can better capture the experimental results than previous models. Based on the modeling analysis, the 1,5-H shift dominates the crucial isomerization steps of the first and second O2 addition products in the low-temperature chain branching process of cyclohexane. The negative temperature coefficient behavior of cyclohexane oxidation results from the reduced chain branching due to the competition from chain inhibition and propagation reactions, i.e. the reaction between cyclohexyl radical and O2 and the de- composition of cyclohexylperoxy radical, both producing cyclohexene and HO2 radical, as well as the decomposition of cyclohexylhydroperoxy radical producing hex-5-en-l-al and OH radical.展开更多
The metallurgical sewage has very complex component and a significant environmental perniciousness and needs high treatment costs. In addition, too much low-temperature waste heat is emitted owing to the lack of suita...The metallurgical sewage has very complex component and a significant environmental perniciousness and needs high treatment costs. In addition, too much low-temperature waste heat is emitted owing to the lack of suitable users. Considering these concerns, a low-temperature-driven pretreatment method via vacuum distillation was proposed to treat the sewage from the metallurgical production. It uses the sensible heat carried by low-temperature exhausted gases to drive the distillation of sewage. The distilled water can be reused into the process as new water supply, while the enriched wastewater is discharged into the sewage treatment center for subsequent treatment. Converter dust removal sewage was chosen to perform an experimental observation. The variations of chemical oxygen demand, ammonia nitrogen, suspended solids, electrical conductivity, and pH of the condensate under different vacuum degrees and evaporation rates were mainly investigated. It can be found that the quality of the condensate gets better under certain conditions, which validates the feasibility of the proposed approach. Furthermore, by comprehensively analyzing the water quality indices and their influencing factors, the optimal vacuum degree was suggested to be controlled between 0.07 and 0.09 MPa, and the best evaporation rate was between 40 and 60%.展开更多
基金supported by the National Natural Science Foundation of China(No.91641205,No.51622605,No.91541201)the Shanghai Science and Technology Committee(No.17XD1402000)
文摘We report the investigation on the low-temperature oxidation of cyclohexane in a jet-stirred reactor over 500-742 K. Synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) was used for identifying and quantifying the oxidation species. Major products, cyclic olefins, and oxygenated products including reactive hydroperoxides and high oxygen compounds were detected. Compared with n-alkanes, a narrow low-temperature window (-80 K) was observed in the low-temperature oxidation of cyclohexane. Besides, a kinetic model for cyclohexane oxidation was developed based on the CNRS model [Combust. Flame 160, 2319 (2013)], which can better capture the experimental results than previous models. Based on the modeling analysis, the 1,5-H shift dominates the crucial isomerization steps of the first and second O2 addition products in the low-temperature chain branching process of cyclohexane. The negative temperature coefficient behavior of cyclohexane oxidation results from the reduced chain branching due to the competition from chain inhibition and propagation reactions, i.e. the reaction between cyclohexyl radical and O2 and the de- composition of cyclohexylperoxy radical, both producing cyclohexene and HO2 radical, as well as the decomposition of cyclohexylhydroperoxy radical producing hex-5-en-l-al and OH radical.
基金This work was sponsored by the National Natural Science Foundation of China (51734004, 21561122001), the China Scholarship Council (201702660037) and the Fundamental Research Funds for the China Central Universities (N162504011).
文摘The metallurgical sewage has very complex component and a significant environmental perniciousness and needs high treatment costs. In addition, too much low-temperature waste heat is emitted owing to the lack of suitable users. Considering these concerns, a low-temperature-driven pretreatment method via vacuum distillation was proposed to treat the sewage from the metallurgical production. It uses the sensible heat carried by low-temperature exhausted gases to drive the distillation of sewage. The distilled water can be reused into the process as new water supply, while the enriched wastewater is discharged into the sewage treatment center for subsequent treatment. Converter dust removal sewage was chosen to perform an experimental observation. The variations of chemical oxygen demand, ammonia nitrogen, suspended solids, electrical conductivity, and pH of the condensate under different vacuum degrees and evaporation rates were mainly investigated. It can be found that the quality of the condensate gets better under certain conditions, which validates the feasibility of the proposed approach. Furthermore, by comprehensively analyzing the water quality indices and their influencing factors, the optimal vacuum degree was suggested to be controlled between 0.07 and 0.09 MPa, and the best evaporation rate was between 40 and 60%.