A numerical investigation on the co-pyrolysis of 1,3-butadiene and propyne is performed to explore the synergistic effect between fuel components on aromatic hydrocarbon formation. A detailed kinetic model of 1,3-buta...A numerical investigation on the co-pyrolysis of 1,3-butadiene and propyne is performed to explore the synergistic effect between fuel components on aromatic hydrocarbon formation. A detailed kinetic model of 1,3-butadiene/propyne co-pyrolysis with the sub-mechanism of aromatic hydrocarbon formation is developed and validated on previous 1,3-butadiene and propyne pyrolysis experiments. The model is able to reproduce both the single component pyrolysis and the co-pyrolysis experiments, as well as the synergistic effect between 1,3- butadiene and propyne on the formation of a series of aromatic hydrocarbons. Based on the rate of production and sensitivity analyses, key reaction pathways in the fuel decomposition and aromatic hydrocarbon formation processes are revealed and insight into the synergistic effect on aromatic hydrocarbon formation is also achieved. The synergistic effect results from the interaction between 1,3-butadiene and propyne. The easily happened chain initiation in the 1,3-butadiene decomposition provides an abundant radical pool for propyne to undergo the H-atom abstraction and produce propargyl radical which plays key roles in the formation of aromatic hydrocarbons. Besides, the 1,3-butadiene/propyne co-pyrolysis includes high concentration levels of C3 and C4 precursors simultaneously, which stimulates the formation of key aromatic hydrocarbons such as toluene and naphthalene.展开更多
Study of the relationship between plant litter-derived dissolved organic matter(DOM) and organic pollutant transport in soil is important for understanding the role of forest litter carbon cycling in influencing pollu...Study of the relationship between plant litter-derived dissolved organic matter(DOM) and organic pollutant transport in soil is important for understanding the role of forest litter carbon cycling in influencing pollutant behaviour and fate in forest soil.With the aim of providing insight into the capacity of plant litter-derived DOM to influence sorption and desorption of selected polycyclic aromatic hydrocarbons(PAHs) on soil, batch experiments were carried out with application of a sorption-desorption model incorporating DOM effects. Freshly fallen pine(Pinus elliottii) needles were used as the source of organic matter. Input of the pine needle litter-derived DOM was found to significantly decrease desorption hysteresis as well as soil adsorption capacity of phenanthrene(PHE) and fluoranthene(FLA). Addition of 1 728 mg L-1dissolved organic carbon(DOC) lowered the organic carbon-normalized sorption distribution coefficient of PHE from 7 776 to 2 541 L kg-1C and of FLA from 11 503 to 4 368 L kg-1C. Decreases of the apparent sorption-desorption distribution coefficients of PHE and FLA with increased DOC concentration indicated that DOM favored desorption of PAHs from soil. Increases in the fraction of apparently dissolved PAHs were attributable to the dissolved PAH-DOM complexes, accounting for the dissolved proportions of 39% to 69% for PHE and 26% to 72% for FLA in the sorption and desorption processes as the concentration of the added DOM solution rose from 0 to 1 728 mg L-1. Our results suggest that pine needle litterderived DOM can have a substantial effect of inhibiting PAHs sorption and promoting PAHs desorption, thus leading to enhanced leaching in soil, which should be taken into account in risk assessment of PAHs accumulated in forest soil.展开更多
基金This work is supported by the National Natural Science Foundation of China （No.51476155, No.51622605, No.91541201）, the National Key Sci- entific Instruments and Equipment Development Program of China （No.2012YQ22011305）, the National Postdoctoral Program for Innovative Talents （No.BX201600100）, and China Postdoctoral Science Foundation （No.2016M600312）.
文摘A numerical investigation on the co-pyrolysis of 1,3-butadiene and propyne is performed to explore the synergistic effect between fuel components on aromatic hydrocarbon formation. A detailed kinetic model of 1,3-butadiene/propyne co-pyrolysis with the sub-mechanism of aromatic hydrocarbon formation is developed and validated on previous 1,3-butadiene and propyne pyrolysis experiments. The model is able to reproduce both the single component pyrolysis and the co-pyrolysis experiments, as well as the synergistic effect between 1,3- butadiene and propyne on the formation of a series of aromatic hydrocarbons. Based on the rate of production and sensitivity analyses, key reaction pathways in the fuel decomposition and aromatic hydrocarbon formation processes are revealed and insight into the synergistic effect on aromatic hydrocarbon formation is also achieved. The synergistic effect results from the interaction between 1,3-butadiene and propyne. The easily happened chain initiation in the 1,3-butadiene decomposition provides an abundant radical pool for propyne to undergo the H-atom abstraction and produce propargyl radical which plays key roles in the formation of aromatic hydrocarbons. Besides, the 1,3-butadiene/propyne co-pyrolysis includes high concentration levels of C3 and C4 precursors simultaneously, which stimulates the formation of key aromatic hydrocarbons such as toluene and naphthalene.
基金Supported by the National Natural Science Foundation of China(No.41001322)the National Funds for Distinguished Young Scientists of China(No.41225004)+2 种基金the Guangdong Province Higher Vocational Colleges and Schools Pearl River Scholar Funded Scheme,Chinathe Special Fund for Scientific Research in the Public Interest of Environmental Protection,Ministry of Environmental Protection of China(No.201109020)the Fundamental Research Funds for the Central Universities of China(No.11lgpy98)
文摘Study of the relationship between plant litter-derived dissolved organic matter(DOM) and organic pollutant transport in soil is important for understanding the role of forest litter carbon cycling in influencing pollutant behaviour and fate in forest soil.With the aim of providing insight into the capacity of plant litter-derived DOM to influence sorption and desorption of selected polycyclic aromatic hydrocarbons(PAHs) on soil, batch experiments were carried out with application of a sorption-desorption model incorporating DOM effects. Freshly fallen pine(Pinus elliottii) needles were used as the source of organic matter. Input of the pine needle litter-derived DOM was found to significantly decrease desorption hysteresis as well as soil adsorption capacity of phenanthrene(PHE) and fluoranthene(FLA). Addition of 1 728 mg L-1dissolved organic carbon(DOC) lowered the organic carbon-normalized sorption distribution coefficient of PHE from 7 776 to 2 541 L kg-1C and of FLA from 11 503 to 4 368 L kg-1C. Decreases of the apparent sorption-desorption distribution coefficients of PHE and FLA with increased DOC concentration indicated that DOM favored desorption of PAHs from soil. Increases in the fraction of apparently dissolved PAHs were attributable to the dissolved PAH-DOM complexes, accounting for the dissolved proportions of 39% to 69% for PHE and 26% to 72% for FLA in the sorption and desorption processes as the concentration of the added DOM solution rose from 0 to 1 728 mg L-1. Our results suggest that pine needle litterderived DOM can have a substantial effect of inhibiting PAHs sorption and promoting PAHs desorption, thus leading to enhanced leaching in soil, which should be taken into account in risk assessment of PAHs accumulated in forest soil.
