垃圾渗沥液—烟气脱硫体系气液吸收与解吸过程研究
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摘要
寻求廉价且性能可靠的湿法烟气脱硫新工艺、新型高效吸收剂和经济有效、技术先进的城市垃圾填埋场渗滤液中高浓度氨氮预处理方法，一直是环境化学工程领域的两大热点。本研究首次提出并建立了垃圾渗滤液湿法烟气脱硫-微生物硫转化互补体系，利用垃圾渗滤液的高碱度和液相金属离子催化氧化性“以污治污”吸收二氧化硫，同时较高温度的烟气又作为汽提介质“以污治污”吹脱垃圾渗滤液的氨氮。本文系统研究了垃圾渗滤液吸收烟气中SO_2并伴随氨的解吸这一复杂过程的反应机理、宏观动力学控制步骤和工艺特性，并对这一特殊的气液吸收和解吸过程进行了数值模拟。
针对垃圾渗滤液组成复杂的特性，采用自行设计的双磁力搅拌气液反应器通过实验首次研究了含有NH_4~+-N、过渡金属离子、无机阴离子、复杂有机物的垃圾渗滤液吸收SO_2同时伴随渗滤液氨解吸过程的反应机理，采用L_9(3~4)正交试验研究了垃圾渗滤液的pH值、Fe~(2+)、Mn~(2+)、Cl~-、乙醇以及甲苯等代表性因子的显著性，并证实这些因子对SO_2吸收效率影响的大小依次为pH值、Fe~(2+)和Mn~(2+)的浓度、Cl~-浓度及乙醇和甲苯的浓度。对pH值、Fe~(2+)、Mn~(2+)、Cl~-、乙醇以及甲苯等代表性因子进行了机理分析、定量实验研究和数学模拟。结果表明，(1)垃圾渗滤液pH值是SO_2吸收率和氨氮吹脱去除率的关键因素，高的初始pH值可同时获得较高的氨氮吹脱去除率和脱硫率。(2)垃圾渗滤液的初始pH值为8.5，液气比为3L／m~3并控制吸收终点pH值为6.0，SO_2平均吸收率可达85％，氨氮吹脱累计去除率可达44％。(3)垃圾渗滤液pH值低于7时，渗滤液中较低浓度的Fe~(2+)、Mn~(2+)对液相的S(Ⅳ)氧化仍具有较显著的催化作用，在相同浓度下，Mn~(2+)的催化作用优于Fe~(2+)，但二者的催化行为总体上类似，提高Fe~(2+)、Mn~(2+)浓度可有效促进SO_2的吸收率。(4)Cl~-对SO_2吸收的促进作用主要归因于Cl~-对液相的S(Ⅳ)氧化具有较显著的催化作用，而这种催化作用必须在Fe~(2+)、Mn~(2+)的协同下才可能发生。(5)乙醇能通过抑制液相的S(Ⅳ)氧化反应降低SO_2的吸收效率，但
四川大学博士学位论文
总体上这种抑制作用明显小于Fe2+、M矛十以及cl‘的催化作用。(6)液相发生的
S(W)氧化反应对于促进苯基类难生物降解物质的破环有促进作用，有利于
后续的生物硫转化工艺。(7)垃圾渗滤液吸收烟气502的宏观动力学过程较复
杂，总体上属于传质速度控制过程而非动力学控制过程，由实验结果，可以根
据溶液pH值的变化划分传质速度控制过程，当体系的pH值较高时(pH值)8.5)，
气相扩散阻力为主导性因素，吸收过程控制步骤可视为气相扩散控制;当4簇pH
成6.5值时，液相扩散阻力为主导性因素，吸收过程控制步骤可视为液相扩散控
制;而当6.5 氨的解吸为气相扩散控制过程。
通过实验详细测定了必loomm常规填料塔内脱硫率和氨氮脱除率随液相
停留时间、操作温度、喷淋密度、液气比、烟气中502浓度和渗滤液中氨氮浓
度等的变化情况，分析了这些操作参数对过程的影响，并根据实验数据得出了
脱硫率、氨氮脱除率和操作参数之间的回归经验方程。在液相停留时间为
45min，操作温度so.c，喷淋密度3 m3/m2·h，液气t匕3L/m3，烟气502浓度zsoopm
的较佳工艺组合条件下，S仇平均吸收率可达85%，氨氮总去除率达40%，吸收
尾液COD/s比为2.1，有利于后序吸收尾液中硫的微生物转化处理。
基于经典双膜传质理论，建立了填料塔内垃圾渗滤液吸收烟气中502并伴
随氨的解吸过程的数学模型，根据工艺研究的实验条件对模型赋初值，结合模
型参数估值确定适宜的边界条件，采用MaPles.0对模型方程进行求解，得到了
液膜内各组份的浓度分布特性曲线，以及气相分压、pH值、传质阻力、传质速
率、吸收增强因子等沿塔高的分布特性，结果表明模型预测结果和实验结果吻
合良好。
通过本文研究，弄清了垃圾渗滤液吸收烟气中502并伴随氨的解吸过程的
反应机理和宏观动力学控制步骤，掌握了填料塔内垃圾渗滤液吸收烟气中502
并伴随氨的解吸过程的工艺操作特性及其规律，基于对实验数据的数学模拟给
出了较佳的操作参数范围。基于经典双膜传质理论建立了过程模拟计算的模型，
为本工艺过程和其它湿法烟气脱硫过程的传质一反应现象提供了一个定量的理
论分析和工程设计基础。
关键词:烟气脱硫垃圾渗滤液亚硫酸盐硫酸盐液相催化氧化数值模拟
It's a main issue in the field of environmental chemical engineering to find effective and cheap absorption medium for the wet flue gas desulfurization(FGD) process. At the same time, much attention have been paid on finding more effective and economy methods on ammonia stripping as pre-process for landfill leachtae bio-treatment. The study in this paper put forward and developed a system of integrating SO2 absorption into flue gas with landfill leachate coupled with ammonia stripping for the first time, in which SO2 in the flue gas could be absorbed by the alkaline and S(IV) oxidation catalyzed by metal ions in landfill leachate while the heat needed for stripping some ammonia from landfill leachate at high temperature can be provided partially or totally by the higher temperature flue gas. The reaction mechanism, macro kinetic control factors, operating parameters in normal packed column, and rate-based model of the process were systematically investigated in the present paper.Due to the complexity of landfill leachate composition, the reaction mechanism of SO2 absorption into flue gas with landfill leachate coupled with ammonia desorption was studied using a stirring vessel. The orthogonal experimental results indicated that the influence degree sequence of effect on SO2 absorption efficiency with landfill leachate form large to small was pH value, the catalysis of Fe2+ and Mn2+, the catalysis of Cl~ and the concentration of toluene and ethanol. The quantitative experiments showed that the pH value of landfill leachate was the key factor both
for SO2 absorption and ammonia stripping. Under the condition of initial pH vajue being 8.5, terminal pH value being 6.0 and L/G ratio being 3L/m3, experiment results showed that average absorption efficiency of SO2 was 85% and average desorption efficiency of ammonia was 44%. The catalysis of Fe2+ and Mn2+ was important for SO2 absorption when pH value was below 7.0. Catalysis activity of Mn2+ was better than that of Fe2+ although their react steps were very similar. The catalysis of Cl" could only be effective if companied by the catalysis of Fe2+and Mn2+. Ethanol could inhibit S(IV) oxidation. S(IV) oxidation could improve the solubility of organics such as toluene in landfill leachtae, and the products were water-soluble and belonged to biodegradable surfactants which could be used as substrates for microbiology in the post bio-process. However, positive effect of catalysis of Cl", Fe2+ and Mn2+ on S(IV) oxidation has superiority over the negative effect of ethanol inhibition on S(IV) oxidation. Macro kinetic experiment results indicated that gas phase diffusion resistance could be the control step of the process when pH value was above 8.5, and liquid phase diffuse resistance could be the control step of the process when pH value was between 4 to 6.5 due to S(IV) oxidation, and the gas phase and liquid phase diffusion resistance might both have effects on the control step of the process when pH value was between 6.5 to 8.5.Operating parameters, including liquid retention time, temperature, ratio of liquid /gas flow rate, liquid spraying density, SO2 concentration in flue gas, and NH/-N concentration in landfill leachate, were studied experimentally in a normal packed column. Based on experimental results, numerical simulation equations of SO2 absorption efficiency and ammonia desorption efficiency corresponding to the operating parameters were developed. The experimental results indicated that ammonia desorption efficiency increased when liquid retention time was below 20 min and SO2 absorption efficiency decreased when liquid retention time became long. High temperature was benefit to ammonia stripping and disbenifit to SO2 absorption. SO2 absorption efficiency and ammonia desorption efficiency both improved with increasing the ratio of liquid /gas flow rate and the liquid spraying density. High concentration of SO2 in flue gas had negative effect on SO2 absorption
and ammonia stripping, while high concentration of NH4+-N in landfill leachate had positive effect. Unde
针对垃圾渗滤液组成复杂的特性，采用自行设计的双磁力搅拌气液反应器通过实验首次研究了含有NH_4~+-N、过渡金属离子、无机阴离子、复杂有机物的垃圾渗滤液吸收SO_2同时伴随渗滤液氨解吸过程的反应机理，采用L_9(3~4)正交试验研究了垃圾渗滤液的pH值、Fe~(2+)、Mn~(2+)、Cl~-、乙醇以及甲苯等代表性因子的显著性，并证实这些因子对SO_2吸收效率影响的大小依次为pH值、Fe~(2+)和Mn~(2+)的浓度、Cl~-浓度及乙醇和甲苯的浓度。对pH值、Fe~(2+)、Mn~(2+)、Cl~-、乙醇以及甲苯等代表性因子进行了机理分析、定量实验研究和数学模拟。结果表明，(1)垃圾渗滤液pH值是SO_2吸收率和氨氮吹脱去除率的关键因素，高的初始pH值可同时获得较高的氨氮吹脱去除率和脱硫率。(2)垃圾渗滤液的初始pH值为8.5，液气比为3L／m~3并控制吸收终点pH值为6.0，SO_2平均吸收率可达85％，氨氮吹脱累计去除率可达44％。(3)垃圾渗滤液pH值低于7时，渗滤液中较低浓度的Fe~(2+)、Mn~(2+)对液相的S(Ⅳ)氧化仍具有较显著的催化作用，在相同浓度下，Mn~(2+)的催化作用优于Fe~(2+)，但二者的催化行为总体上类似，提高Fe~(2+)、Mn~(2+)浓度可有效促进SO_2的吸收率。(4)Cl~-对SO_2吸收的促进作用主要归因于Cl~-对液相的S(Ⅳ)氧化具有较显著的催化作用，而这种催化作用必须在Fe~(2+)、Mn~(2+)的协同下才可能发生。(5)乙醇能通过抑制液相的S(Ⅳ)氧化反应降低SO_2的吸收效率，但
四川大学博士学位论文
总体上这种抑制作用明显小于Fe2+、M矛十以及cl‘的催化作用。(6)液相发生的
S(W)氧化反应对于促进苯基类难生物降解物质的破环有促进作用，有利于
后续的生物硫转化工艺。(7)垃圾渗滤液吸收烟气502的宏观动力学过程较复
杂，总体上属于传质速度控制过程而非动力学控制过程，由实验结果，可以根
据溶液pH值的变化划分传质速度控制过程，当体系的pH值较高时(pH值)8.5)，
气相扩散阻力为主导性因素，吸收过程控制步骤可视为气相扩散控制;当4簇pH
成6.5值时，液相扩散阻力为主导性因素，吸收过程控制步骤可视为液相扩散控
制;而当6.5
通过实验详细测定了必loomm常规填料塔内脱硫率和氨氮脱除率随液相
停留时间、操作温度、喷淋密度、液气比、烟气中502浓度和渗滤液中氨氮浓
度等的变化情况，分析了这些操作参数对过程的影响，并根据实验数据得出了
脱硫率、氨氮脱除率和操作参数之间的回归经验方程。在液相停留时间为
45min，操作温度so.c，喷淋密度3 m3/m2·h，液气t匕3L/m3，烟气502浓度zsoopm
的较佳工艺组合条件下，S仇平均吸收率可达85%，氨氮总去除率达40%，吸收
尾液COD/s比为2.1，有利于后序吸收尾液中硫的微生物转化处理。
基于经典双膜传质理论，建立了填料塔内垃圾渗滤液吸收烟气中502并伴
随氨的解吸过程的数学模型，根据工艺研究的实验条件对模型赋初值，结合模
型参数估值确定适宜的边界条件，采用MaPles.0对模型方程进行求解，得到了
液膜内各组份的浓度分布特性曲线，以及气相分压、pH值、传质阻力、传质速
率、吸收增强因子等沿塔高的分布特性，结果表明模型预测结果和实验结果吻
合良好。
通过本文研究，弄清了垃圾渗滤液吸收烟气中502并伴随氨的解吸过程的
反应机理和宏观动力学控制步骤，掌握了填料塔内垃圾渗滤液吸收烟气中502
并伴随氨的解吸过程的工艺操作特性及其规律，基于对实验数据的数学模拟给
出了较佳的操作参数范围。基于经典双膜传质理论建立了过程模拟计算的模型，
为本工艺过程和其它湿法烟气脱硫过程的传质一反应现象提供了一个定量的理
论分析和工程设计基础。
关键词:烟气脱硫垃圾渗滤液亚硫酸盐硫酸盐液相催化氧化数值模拟
It's a main issue in the field of environmental chemical engineering to find effective and cheap absorption medium for the wet flue gas desulfurization(FGD) process. At the same time, much attention have been paid on finding more effective and economy methods on ammonia stripping as pre-process for landfill leachtae bio-treatment. The study in this paper put forward and developed a system of integrating SO2 absorption into flue gas with landfill leachate coupled with ammonia stripping for the first time, in which SO2 in the flue gas could be absorbed by the alkaline and S(IV) oxidation catalyzed by metal ions in landfill leachate while the heat needed for stripping some ammonia from landfill leachate at high temperature can be provided partially or totally by the higher temperature flue gas. The reaction mechanism, macro kinetic control factors, operating parameters in normal packed column, and rate-based model of the process were systematically investigated in the present paper.Due to the complexity of landfill leachate composition, the reaction mechanism of SO2 absorption into flue gas with landfill leachate coupled with ammonia desorption was studied using a stirring vessel. The orthogonal experimental results indicated that the influence degree sequence of effect on SO2 absorption efficiency with landfill leachate form large to small was pH value, the catalysis of Fe2+ and Mn2+, the catalysis of Cl~ and the concentration of toluene and ethanol. The quantitative experiments showed that the pH value of landfill leachate was the key factor both
for SO2 absorption and ammonia stripping. Under the condition of initial pH vajue being 8.5, terminal pH value being 6.0 and L/G ratio being 3L/m3, experiment results showed that average absorption efficiency of SO2 was 85% and average desorption efficiency of ammonia was 44%. The catalysis of Fe2+ and Mn2+ was important for SO2 absorption when pH value was below 7.0. Catalysis activity of Mn2+ was better than that of Fe2+ although their react steps were very similar. The catalysis of Cl" could only be effective if companied by the catalysis of Fe2+and Mn2+. Ethanol could inhibit S(IV) oxidation. S(IV) oxidation could improve the solubility of organics such as toluene in landfill leachtae, and the products were water-soluble and belonged to biodegradable surfactants which could be used as substrates for microbiology in the post bio-process. However, positive effect of catalysis of Cl", Fe2+ and Mn2+ on S(IV) oxidation has superiority over the negative effect of ethanol inhibition on S(IV) oxidation. Macro kinetic experiment results indicated that gas phase diffusion resistance could be the control step of the process when pH value was above 8.5, and liquid phase diffuse resistance could be the control step of the process when pH value was between 4 to 6.5 due to S(IV) oxidation, and the gas phase and liquid phase diffusion resistance might both have effects on the control step of the process when pH value was between 6.5 to 8.5.Operating parameters, including liquid retention time, temperature, ratio of liquid /gas flow rate, liquid spraying density, SO2 concentration in flue gas, and NH/-N concentration in landfill leachate, were studied experimentally in a normal packed column. Based on experimental results, numerical simulation equations of SO2 absorption efficiency and ammonia desorption efficiency corresponding to the operating parameters were developed. The experimental results indicated that ammonia desorption efficiency increased when liquid retention time was below 20 min and SO2 absorption efficiency decreased when liquid retention time became long. High temperature was benefit to ammonia stripping and disbenifit to SO2 absorption. SO2 absorption efficiency and ammonia desorption efficiency both improved with increasing the ratio of liquid /gas flow rate and the liquid spraying density. High concentration of SO2 in flue gas had negative effect on SO2 absorption
and ammonia stripping, while high concentration of NH4+-N in landfill leachate had positive effect. Unde
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