Adequate destruction of the aromatic structure in coal is key to further reducing the emission of pollutants.In this research,activation reactions of Shenmu coal powder were carried out in a vertical tube furnace.The ...Adequate destruction of the aromatic structure in coal is key to further reducing the emission of pollutants.In this research,activation reactions of Shenmu coal powder were carried out in a vertical tube furnace.The study investigated the evolution mechanism of carbon covalent bonds during the activation process by altering the ratio of H_(2)O to CO_(2)in the activation atmosphere.The theoretical validation was conducted through density functional calculations.The two gas molecules follow different pathways to increase the reactivity of char.CO_(2)mainly participates in the cross-linking reaction by intensifying branching,while H_(2)O and char have lower adsorption energy barriers and are more likely to generate oxygen-containing functional groups.Gas molecules partially compete for active sites in a mixed gas atmosphere,but there is a synergism between the two effects.The synergism can be attributed to two possibilities.The inclusion of H_(2)O mitigates the generation of five-membered rings to a limited extent,while concurrently enhances the development of oxygen-containing functional groups.Introducing oxygen-containing functional groups can effectively diminish the adsorption energy barrier associated with the interaction between gas molecules and char,consequently leading to a reduction in the energy demand for subsequent bond cleavage.展开更多
Lorentz curve fittings are applied to frequency distributions of the concentrations of O3, CO, NOx and SO2 recorded at the Jinsha regional atmospheric background station （JSH） from June 2006 to July 2007, and the pe...Lorentz curve fittings are applied to frequency distributions of the concentrations of O3, CO, NOx and SO2 recorded at the Jinsha regional atmospheric background station （JSH） from June 2006 to July 2007, and the peak concentrations of these species for the different seasons are obtained. The peak concentrations are considered to be representative of different background levels for certain processes. The peak concentrations are compared with the corresponding mean （median） concentrations, and the suitability and limitations of the mean （median） values as the background levels are discussed. The mean （median） values might represent the background concentrations in the region under some circumstances, but in other cases these values often underestimate or overestimate the true background concentrations owing to the transport of pollutants and other factors. The effects of air masses transported from different regions on the pollutant background concentrations are obtained by analyzing the 72-hour backward trajectories of air masses 100m above the ground at JSH, These trajectories are estimated using the HYSPLIT model and then clustered for the measurement period. The spatial distribution and seasonal variations of trajectories and the corresponding mean concentrations of O3, SO〉 NOx and CO for different clusters are analyzed. After filtering the seasonal changes in pollutant concentrations, the relative influences of air masses from different regions are obtained. The results show that JSH can be used to obtain the atmospheric background information of different air masses originating from or passing over the Yangtze River Delta, Central South China and the Jianghan Plain. Air masses from Central China, South China, and the western Yangtze River Delta contribute significantly to O3 at JSH. Air masses from the north and northeast of JSH （i.e., the Jianghan Plain, Huang-Huai Plain and North China Plain） and the south （Central South China） contribute significantly to SO2, CO and NOx concentrations. Air masses originating from the ocean often bring clean air. Air masses originating from high altitudes over northwestern regions often have lower CO and NO3 concentrations, lower relative humidity, and higher concentrations of O3 and SO2.展开更多
基金supported by the CAS Project for Young Scientists in Basic Research(YSBR-028)。
文摘Adequate destruction of the aromatic structure in coal is key to further reducing the emission of pollutants.In this research,activation reactions of Shenmu coal powder were carried out in a vertical tube furnace.The study investigated the evolution mechanism of carbon covalent bonds during the activation process by altering the ratio of H_(2)O to CO_(2)in the activation atmosphere.The theoretical validation was conducted through density functional calculations.The two gas molecules follow different pathways to increase the reactivity of char.CO_(2)mainly participates in the cross-linking reaction by intensifying branching,while H_(2)O and char have lower adsorption energy barriers and are more likely to generate oxygen-containing functional groups.Gas molecules partially compete for active sites in a mixed gas atmosphere,but there is a synergism between the two effects.The synergism can be attributed to two possibilities.The inclusion of H_(2)O mitigates the generation of five-membered rings to a limited extent,while concurrently enhances the development of oxygen-containing functional groups.Introducing oxygen-containing functional groups can effectively diminish the adsorption energy barrier associated with the interaction between gas molecules and char,consequently leading to a reduction in the energy demand for subsequent bond cleavage.
基金supported by National Basic Research Program of China (Grant No. 2005CB4222002)Project of China Meteorological Administration (Grant No. GYHY[QX]200706005)National Natural Science Foundation of China (Grant No. 40705042)
文摘Lorentz curve fittings are applied to frequency distributions of the concentrations of O3, CO, NOx and SO2 recorded at the Jinsha regional atmospheric background station （JSH） from June 2006 to July 2007, and the peak concentrations of these species for the different seasons are obtained. The peak concentrations are considered to be representative of different background levels for certain processes. The peak concentrations are compared with the corresponding mean （median） concentrations, and the suitability and limitations of the mean （median） values as the background levels are discussed. The mean （median） values might represent the background concentrations in the region under some circumstances, but in other cases these values often underestimate or overestimate the true background concentrations owing to the transport of pollutants and other factors. The effects of air masses transported from different regions on the pollutant background concentrations are obtained by analyzing the 72-hour backward trajectories of air masses 100m above the ground at JSH, These trajectories are estimated using the HYSPLIT model and then clustered for the measurement period. The spatial distribution and seasonal variations of trajectories and the corresponding mean concentrations of O3, SO〉 NOx and CO for different clusters are analyzed. After filtering the seasonal changes in pollutant concentrations, the relative influences of air masses from different regions are obtained. The results show that JSH can be used to obtain the atmospheric background information of different air masses originating from or passing over the Yangtze River Delta, Central South China and the Jianghan Plain. Air masses from Central China, South China, and the western Yangtze River Delta contribute significantly to O3 at JSH. Air masses from the north and northeast of JSH （i.e., the Jianghan Plain, Huang-Huai Plain and North China Plain） and the south （Central South China） contribute significantly to SO2, CO and NOx concentrations. Air masses originating from the ocean often bring clean air. Air masses originating from high altitudes over northwestern regions often have lower CO and NO3 concentrations, lower relative humidity, and higher concentrations of O3 and SO2.
