研究报告

  • 张良佺,盖希坤,杨瑞芹,戚倩,程燕飞,孙杰楠.双驱动反应器中热钾碱吸收二氧化碳的动力学研究[J].环境科学学报,2017,37(7):2490-2497

  • 双驱动反应器中热钾碱吸收二氧化碳的动力学研究
  • Kinetic study of absorption of carbon dioxide in biogas using hot potassium carbonate solution process in a dual-driver reactor
  • 基金项目:浙江省农产品化学与生物加工技术重点实验室开放基金(No.2016KF0045);浙江省废弃生物质循环利用与生态处理技术重点实验室开放基金(No.2016REWB13)
  • 作者
  • 单位
  • 张良佺
  • 1 浙江省农产品化学与生物加工技术重点实验室/浙江省农业生物资源生化制造协同创新中心, 杭州 310023;2 浙江科技学院浙江省废弃生物质循环利用与生态处理技术重点实验室, 杭州 310023
  • 盖希坤
  • 浙江省农产品化学与生物加工技术重点实验室/浙江省农业生物资源生化制造协同创新中心, 杭州 310023
  • 杨瑞芹
  • 浙江省农产品化学与生物加工技术重点实验室/浙江省农业生物资源生化制造协同创新中心, 杭州 310023
  • 戚倩
  • 浙江省农产品化学与生物加工技术重点实验室/浙江省农业生物资源生化制造协同创新中心, 杭州 310023
  • 程燕飞
  • 浙江省农产品化学与生物加工技术重点实验室/浙江省农业生物资源生化制造协同创新中心, 杭州 310023
  • 孙杰楠
  • 浙江省农产品化学与生物加工技术重点实验室/浙江省农业生物资源生化制造协同创新中心, 杭州 310023
  • 摘要:采用双驱动反应器研究了热钾碱吸收二氧化碳的反应动力学,根据双膜理论,应用CO2-H2O体系,实验首先对气相传质过程进行了研究,结果表明:当气相体积流量为80 mL·min-1时,气相搅拌速度在100 r·min-1时可认为气膜阻力消去.通过改变液相搅拌转速,研究了液相传质系数kL变化规律,获得了kL的无因次关联式.根据热钾碱吸收CO2反应机理,获得了宏观动力学方程,并结合溶液的非理想性,对速率方程中的浓度效应进行了校正,通过实验测定并进行了模型参数估值,各参数分别为:表观活化能Eob=21.9308 kJ·mol-1,表观反应级数n=0.1399,表观指前因子K0'=1.1908×10-4 mol·m-2·s-1·Pa-1.在此基础上,通过计算获得了热钾碱吸收CO2的本征动力学方程,各模型参数分别为:本征反应活化能E=59.57 kJ·mol-1,指前因子k0=2.1802×1011 m3·mol-1·s-1.为进行整个过程反应机制的判断,计算了膜内转化系数γ,结果表明该值远大于2,可知CO2吸收为快速反应过程,反应主要集中在膜内完成,并由此可知工业反应器选型应采用比相界面积较大的填料塔为优.
  • Abstract:This paper focuses on kinetics study of hot potash absorbing carbon dioxide by a dual-driver reactor. By applying the two-film theory and CO2-H2O system, we investigated the gas phase mass transfer first. The results show that when the gas volume flow reaches 80 mL·min-1 and stirring rate is at 100 r·min-1, gas film resistance can be considered eliminated. By changing the liquid phase stirring speed, the change law of liquid phase mass transfer coefficient kL is investigated and its dimensionless correlation is obtained. According to reaction mechanism of the hot potash absorbing CO2, macroscopic kinetic equation is also obtained. By combining the non-ideality of solution, the concentration effect of rate equation is corrected. Model parameters estimated by experiment are apparent activation energy Eob=21.9308 kJ·mol-1, observed order of reaction n=0.1399, and pre-exponential factor K0'=1.1908×10-4 mol·m-1·s-1·Pa-1. On this basis, the intrinsic kinetic equations of the hot potash absorbing CO2 are obtained by calculation, with intrinsic activation energy E=59.57 kJ·mol-1 and pre-exponential factor k0=2.1802×1011 m3·mol-1·s-1. To determine the process of reaction mechanism, the membrane conversion coefficient γ has been calculated, and the result indicates that the value is much greater than 2, which means that CO2 absorption is a rapid reaction process and the reaction is mainly completed in the membrane. As a result, packed towers, which should be larger than the phase boundary, are optimal in the selection of industrial reactor.

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