The pyrolysis of n-butane and i-butane at low pressure was investigated from 823-1823 K in an electrically heated flow reactor using synchrotron vacuum ultraviolet photoionization mass spectrometry. More than 20 speci...The pyrolysis of n-butane and i-butane at low pressure was investigated from 823-1823 K in an electrically heated flow reactor using synchrotron vacuum ultraviolet photoionization mass spectrometry. More than 20 species, especially several radicals and isomers, were detected and identified from the measurements of photoionization efficiency （PIE） spectra. Based on the mass spectrometric analysis, the characteristics of n-butane and i-butane pyrolysis were discussed, which provided experimental evidences for the discussion of decomposition pathways of butane isomers. It is concluded that the isomeric structures of n-butane and i-butane have strong influence on their main decomposition pathways, and lead to dramatic differences in their mass spectra and PIE spectra such as the different dominant products and isomeric structures of butene products. Furthermore, compared with n-butane,i-butane can produce strong signals of benzene at low temperature in its pyrolysis due to the enhanced formation of benzene precursors like propargyl and C4 species, which provides experimental clues to explain the higher sooting tendencies of iso-alkanes than n-alkanes.展开更多
Ultrasound (US)-induced cavitation is an effective way in oxidizing organic contaminants in wastewater either as the independent operation unit or in combination with other oxidation methods. In this paper, black liqu...Ultrasound (US)-induced cavitation is an effective way in oxidizing organic contaminants in wastewater either as the independent operation unit or in combination with other oxidation methods. In this paper, black liquor and filtrate after acidifying and settling were sonicated. The effect of working parameters on ultrasonic degradation of black liquor, such as different combination methods, frequency, power supply, initial concentration, pH, duration time, ionic strength and catalyst were studied. The results were as follows: (1) At the conditions of 40kHz, 100W, 4h, pH at 6 and temperature 30?℃, utilizing US/US-H2O2/US-Fenton, weak-orange filtrate turned to colloid with the increase of time and little sediment produced after settling. Especially filtrate came to be milk white collides and upper water approached to nearly achromatic by US-Fenton. Compared with the US, US-H2O2/US-Fenton COD (Chemical oxidation demand) removal ratio can increase 15%, 30% respectively. Because of more hydroxyl radicals produced in the reaction process; (2) At the condition of 100W and 4h, the degradation efficiency of black liquor was better at 40kHz over at 20kHz. Moreover black liquor can be biodegraded easily. Those based on that the big molecule of contaminants in aqueous solution can be changed into the little molecule with ultrasound (3) At the condition of 40kHz and 4h, the COD removal ratio of black liquor was more higher at 60W than at 80W, while the removal ratio of COD at 60W was nearly close to the ratio at 100W; (4) The initial concentration of black liquor influenced the effect of sonochemical degradation; (5) The variation of pH had no effect on degradation; (6) The longer the duration time, the greater the removal ratio of COD. But this ratio increased slowly after 4h; (7) Adding 0.2g/L NaCl to change the ionic strength of the black liquor, the COD removal ratio can increase 10%; (8) The degradation rates increased by the coexistent catalysts of TiO2, Co2+ and Ag+.展开更多
基金This work is supported by the National. Natural Science Foundation of China （No.51106146, No.51036007, No.U1232127）, the China Postdoctoral Science Foundation （No.20100480047 and No.201104326）, the Chinese Universities Scientific Fund （No.WK2310000010）, the Anhui Science ＆ Technology Department （No.l1040606Q49）, and the Chinese Academy of Sciences.
文摘The pyrolysis of n-butane and i-butane at low pressure was investigated from 823-1823 K in an electrically heated flow reactor using synchrotron vacuum ultraviolet photoionization mass spectrometry. More than 20 species, especially several radicals and isomers, were detected and identified from the measurements of photoionization efficiency （PIE） spectra. Based on the mass spectrometric analysis, the characteristics of n-butane and i-butane pyrolysis were discussed, which provided experimental evidences for the discussion of decomposition pathways of butane isomers. It is concluded that the isomeric structures of n-butane and i-butane have strong influence on their main decomposition pathways, and lead to dramatic differences in their mass spectra and PIE spectra such as the different dominant products and isomeric structures of butene products. Furthermore, compared with n-butane,i-butane can produce strong signals of benzene at low temperature in its pyrolysis due to the enhanced formation of benzene precursors like propargyl and C4 species, which provides experimental clues to explain the higher sooting tendencies of iso-alkanes than n-alkanes.
文摘Ultrasound (US)-induced cavitation is an effective way in oxidizing organic contaminants in wastewater either as the independent operation unit or in combination with other oxidation methods. In this paper, black liquor and filtrate after acidifying and settling were sonicated. The effect of working parameters on ultrasonic degradation of black liquor, such as different combination methods, frequency, power supply, initial concentration, pH, duration time, ionic strength and catalyst were studied. The results were as follows: (1) At the conditions of 40kHz, 100W, 4h, pH at 6 and temperature 30?℃, utilizing US/US-H2O2/US-Fenton, weak-orange filtrate turned to colloid with the increase of time and little sediment produced after settling. Especially filtrate came to be milk white collides and upper water approached to nearly achromatic by US-Fenton. Compared with the US, US-H2O2/US-Fenton COD (Chemical oxidation demand) removal ratio can increase 15%, 30% respectively. Because of more hydroxyl radicals produced in the reaction process; (2) At the condition of 100W and 4h, the degradation efficiency of black liquor was better at 40kHz over at 20kHz. Moreover black liquor can be biodegraded easily. Those based on that the big molecule of contaminants in aqueous solution can be changed into the little molecule with ultrasound (3) At the condition of 40kHz and 4h, the COD removal ratio of black liquor was more higher at 60W than at 80W, while the removal ratio of COD at 60W was nearly close to the ratio at 100W; (4) The initial concentration of black liquor influenced the effect of sonochemical degradation; (5) The variation of pH had no effect on degradation; (6) The longer the duration time, the greater the removal ratio of COD. But this ratio increased slowly after 4h; (7) Adding 0.2g/L NaCl to change the ionic strength of the black liquor, the COD removal ratio can increase 10%; (8) The degradation rates increased by the coexistent catalysts of TiO2, Co2+ and Ag+.
