选用甲苯模拟焦油芳香环物质,研究微波辅助生物质焦炭诱导甲苯裂解和重整反应规律、产物特性和焦炭变化。试验结果表明,焦炭对甲苯裂解有催化作用,微波环境易于甲苯裂解。甲苯裂解率和氢气选择性与温度正相关,750℃是适宜的温度选项,此...选用甲苯模拟焦油芳香环物质,研究微波辅助生物质焦炭诱导甲苯裂解和重整反应规律、产物特性和焦炭变化。试验结果表明,焦炭对甲苯裂解有催化作用,微波环境易于甲苯裂解。甲苯裂解率和氢气选择性与温度正相关,750℃是适宜的温度选项,此温度下裂解率与氢气选择性分别为92.77%和91.94%,此后无明显变化。通入CO2促使甲苯重整制备合成气,700℃最高转化率92.03%和最大合成气收率91.30%均在CO2流量为80 m L/min时实现,H2/CO值随CO2流量的加大而降低直至0.22。通入CO2导致焦炭碳质量变化率增加,700℃最高达5.42%,此部分碳转化合成气,对合成气产率的贡献率最高可达15.40%。通入CO2可减缓积碳对甲苯转化的不利影响。展开更多
该文以甲苯为焦油模型化合物,利用生物质焦炭诱导其转化合成气,探讨加热方式和通入CO2对甲苯转化的影响。结果表明:同等工况下,微波加热(microwave heating,MH)下甲苯转化率高于常规加热(electrical heating,EH),甲苯转化率最大差值为15...该文以甲苯为焦油模型化合物,利用生物质焦炭诱导其转化合成气,探讨加热方式和通入CO2对甲苯转化的影响。结果表明:同等工况下,微波加热(microwave heating,MH)下甲苯转化率高于常规加热(electrical heating,EH),甲苯转化率最大差值为15.58%。通入CO2可促进甲苯转化,MH和EH下分别在CO2流量为80和40 m L/min达到最高转化率93.73%和82.13%。引入CO2可调控甲苯定向制备合成气,且对生物质焦炭造成碳损耗。损耗碳可转化合成气,且CO2通入量越高,其贡献越大。MH下合成气最大产率为173.66 m L/min,为裂解反应的5.68倍。甲苯裂解率持续降至49.0%,之后趋于稳定。甲苯重整转化率维持较高水平,140 min后开始减弱,同时合成气收率平缓降低。该文研究结果对高效利用焦油和减排CO2有借鉴意义。展开更多
Nitrogen oxides (NOx) emission during the regeneration ofcoked fluid catalytic cracking (FCC) catalysts is an en- vironmental issue. In order to identify the correlations between nitrogen species in coke and diffe...Nitrogen oxides (NOx) emission during the regeneration ofcoked fluid catalytic cracking (FCC) catalysts is an en- vironmental issue. In order to identify the correlations between nitrogen species in coke and different nitrogen- containing products in tail gas, three coked catalysts with multilayer structural coke molecules were prepared in a fixed bed with model compounds (o-xylene and quinoline) at first. A series of characterization methods were used to analyze coke, including elemental analysis, FT-IR, XPS, and TG-MS. XPS characterization indicates all coked catalysts present two types of nitrogen species and the type with a higher binding energy is related with the inner part nitrogen atoms interacting with acid sites. Due to the stronger adsorption ability on acid sites for basic nitrogen compounds, the multilayer structural coke has unbalanced distribution of carbon and ni- trogen atoms between the inner part and the outer edge, which strongly affects gas product formation. At the early stage of regeneration, oxidation starts from the outer edge and the product NO can be reduced to N2 in high CO concentration. At the later stage, the inner part rich in nitrogen begins to be exposed to 02. At this period, the formation of CO decreases due to lack of carbon atoms, which is not beneficial to the reduction of NO. There- fore, nitrogen species in the inner part of multilayer structural coke contributes more to NOx formation. Based on the multilayer structure model of coke molecule and its oxidation behavior, a possible strategy to control NOx emission was discussed merely from concept.展开更多
文摘选用甲苯模拟焦油芳香环物质,研究微波辅助生物质焦炭诱导甲苯裂解和重整反应规律、产物特性和焦炭变化。试验结果表明,焦炭对甲苯裂解有催化作用,微波环境易于甲苯裂解。甲苯裂解率和氢气选择性与温度正相关,750℃是适宜的温度选项,此温度下裂解率与氢气选择性分别为92.77%和91.94%,此后无明显变化。通入CO2促使甲苯重整制备合成气,700℃最高转化率92.03%和最大合成气收率91.30%均在CO2流量为80 m L/min时实现,H2/CO值随CO2流量的加大而降低直至0.22。通入CO2导致焦炭碳质量变化率增加,700℃最高达5.42%,此部分碳转化合成气,对合成气产率的贡献率最高可达15.40%。通入CO2可减缓积碳对甲苯转化的不利影响。
文摘该文以甲苯为焦油模型化合物,利用生物质焦炭诱导其转化合成气,探讨加热方式和通入CO2对甲苯转化的影响。结果表明:同等工况下,微波加热(microwave heating,MH)下甲苯转化率高于常规加热(electrical heating,EH),甲苯转化率最大差值为15.58%。通入CO2可促进甲苯转化,MH和EH下分别在CO2流量为80和40 m L/min达到最高转化率93.73%和82.13%。引入CO2可调控甲苯定向制备合成气,且对生物质焦炭造成碳损耗。损耗碳可转化合成气,且CO2通入量越高,其贡献越大。MH下合成气最大产率为173.66 m L/min,为裂解反应的5.68倍。甲苯裂解率持续降至49.0%,之后趋于稳定。甲苯重整转化率维持较高水平,140 min后开始减弱,同时合成气收率平缓降低。该文研究结果对高效利用焦油和减排CO2有借鉴意义。
基金Supported by the National Natural Science Foundation of China(21476263)the National Natural Science Foundation for Young Scholars(21206198)
文摘Nitrogen oxides (NOx) emission during the regeneration ofcoked fluid catalytic cracking (FCC) catalysts is an en- vironmental issue. In order to identify the correlations between nitrogen species in coke and different nitrogen- containing products in tail gas, three coked catalysts with multilayer structural coke molecules were prepared in a fixed bed with model compounds (o-xylene and quinoline) at first. A series of characterization methods were used to analyze coke, including elemental analysis, FT-IR, XPS, and TG-MS. XPS characterization indicates all coked catalysts present two types of nitrogen species and the type with a higher binding energy is related with the inner part nitrogen atoms interacting with acid sites. Due to the stronger adsorption ability on acid sites for basic nitrogen compounds, the multilayer structural coke has unbalanced distribution of carbon and ni- trogen atoms between the inner part and the outer edge, which strongly affects gas product formation. At the early stage of regeneration, oxidation starts from the outer edge and the product NO can be reduced to N2 in high CO concentration. At the later stage, the inner part rich in nitrogen begins to be exposed to 02. At this period, the formation of CO decreases due to lack of carbon atoms, which is not beneficial to the reduction of NO. There- fore, nitrogen species in the inner part of multilayer structural coke contributes more to NOx formation. Based on the multilayer structure model of coke molecule and its oxidation behavior, a possible strategy to control NOx emission was discussed merely from concept.