新型复合吸收剂液相同时脱硫脱硝的实验研究
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摘要
到目前为止,就烟尘、SO2、NOx等单一污染物而言,国际上已经先后发展出了一系列相应的成熟技术,其中一部分到了工程应用,成为市场上的主流工艺,如静电除尘、钙基烟气脱硫、选择性催化还原(SCR)和选择性非催化还原(SNCR)脱硝、活性炭脱汞。这些技术的特点是：一项技术仅针对一种污染物,通过一套专门的设备实现污染物的脱除。这种污染物分级治理方式,存在占地面积大、设备投资和运行费用及能耗高、烟气系统稳定性差等问题,严重影响燃煤污染控制的经济性和适用性。因此开展烟气多污染物同时脱除的研究具有重要现实意义,已成为当前国内外新兴的研究领域。
基于当前研究热点,论文详细地研究了亚氯酸钠/次氯酸钠溶液和过氧化氢/碱性溶液两种新型复合吸收剂体系中影响同时脱硫脱硝的因素,发现吸收剂溶液pH、吸收剂浓度、反应温度和吸收剂组成及比例对脱除效率影响显著。研究获得了两种新型复合吸收剂体系最佳脱硫脱硝实验条件。其中以亚氯酸钠／次氯酸钠溶液为吸收剂的最佳实验条件为：溶液pH为5.5,次氯酸钠与亚氯酸钠摩尔比为4,反应温度为50℃；在最佳条件下,二氧化硫脱除效率几乎达到100%,氮氧化物脱除效率达到80%。过氧化氢／碱性溶液为吸收剂的最佳实验条件为：溶液pH为10.5,过氧化氢浓度为0.8175 mol·L-1,反应温度为47.5℃；在最佳条件下,二氧化硫脱除效率几乎达到100%,氮氧化物脱除效率达到70%。
通过新型复合吸收剂同时脱硫脱硝产物分析,揭示了脱除反应机理,其中亚氯酸钠/次氯酸钠溶液同时脱硫脱硝反应历程为以亚氯酸根离子、次氯酸及中间产物二氧化氯和氯气共同与二氧化硫和一氧化氮发生了氧化吸收反应,且反应可同时发生于气液两相；过氧化氢碱性溶液同时脱硫脱硝反应历程为过氧化氢、过氧氢根离子及相关自由基在液相共同与二氧化硫和一氧化氮发生了氧化吸收反应。
基于新型复合吸收剂同时脱硫脱硝宏观反应动力学研究表明,亚氯酸钠/次氯酸钠溶液同时脱硫脱硝反应过程中二氧化硫分压和一氧化氮分压的分级数均为一级,宏观反应平均活化能分别为21.598 kJ·mol-1和8.166 kJ·mol-1。过氧化氢碱性溶液脱硫脱硝反应过程中二氧化硫分压和一氧化氮分压的分级数均为一级,宏观反应平均活化能分别为1.378 kJ·mol-1和3.722 kJ·mol-1;同时脱硫脱硝时,二氧化硫对一氧化氮吸收具有抑制作用,对一氧化氮吸收速率影响与其气相分压成1.2次方关系,抑制反应活化能为46.634 kJ·mol-1;一氧化氮对二氧化硫的吸收具有促进作用,对二氧化硫吸收速率影响与其气相分压成2.8次方关系,促吸收反应活化能为155.86 kJ·mol-1;同时脱硫脱硝传质反应动力学研究表明,二氧化硫吸收为传质控制步骤,一氧化氮吸收为反应控制步骤,一级反应平均活化能分别为42.654 kJ·mol-1和27.768 kJ·mol-1。
So far, a series of mature technologies have successively developed to remove single pollutant such as dust, SO2, NOx, and some have been the mainstream processes in the market and applied in engineering, such as electrostatic precipitation technology, wet flue gas dcsulfurization technology with calcium base absorbent, selective catalytic reduction (SCR) denitration technology, selective non-catalytic reduction (SNCR) denitration technology and mercury technology with activated carbon. But it has obvious characteristic that one technology is only used to remove one pollutant by a set of special equipment. For multi-pollutant removal, the graded treatment mode has some problems such as big floor occupation, high equipment investment and operating cost, high energy consumption, less stability of flue gas system. In order to obtain better economy and applicability of the coal-fired pollution control, the research on simultaneous removal of multi-pollutants has important realistic significance, and has become a current new field in both at home and abroad.
Based on the current research focus, the influence factors on removal efficiencies of SO2 and NO in two new complex absorbent system including the solution of NaClO2/NaCIO and alkaline solution of H2O2 were investigated detailedly in this paper.These factors such as solution pH, absorbent concentration, reaction temperature, absorbent composition and proportion have significant effects on removal efficiencies of SO2 and NO. The best experimental conditions of desulfurization and denitration were obtained based on two new complex absorbent system. The optimal removal conditions based on the solution of NaClO2/NaClO included the solution pH was 5.5, the molar ratio of NaCIO to NaCIO2 was 4, and the absorption temperature was 50℃. Under the best conditions, the removal efficiency of SO2 reached almost 100%, and the removal efficiency of NOx reached 80%. The optimal removal conditions based on the alkaline solution of H2O2 included the solution pH was 10.5, the H2O2 concentration was 0.8175 mol·L-1, and the absorption temperature was 47.5℃. Under the best conditions, the removal efficiency of SO2 reached almost 100%, and the removal efficiency of NOx reached 70%.
The removal reaction mechanisms was revealed according to product analysis results of desulfurization and denitration, the oxidation absorption reactions of SO2 and NO with chlorite anion, hypochlorite and intermediate products such as chlorine dioxide and chlorine could occur when solution of NaClO2/NaClO was used as complex absorbent. Moreover, the oxidation reactions may happen in both gas phase and liquid phase. The oxidation absorption reactions of SO2 and NO with hydrogen peroxide, peroxide anion and related free radicals could occur when alkaline solution of H2O2 was used as complex absorbent.
The macro-kinetics experimental results of simultaneous desulfurization and denitration indicated that the apparent reaction orders of SO2 and NO were both one order, and the apparent activation energies were 21.598 kJ·mol-1 and 8.166 kJ·mol-1 respectively when the solution of NaClO2/NaC10 was used as complex absorbent; the apparent reaction orders of SO2 and NO were both one order, the apparent activation energies were 1.3784 kJ·mol-1 and 3.7220 kJ·mol-1 respectively when the alkaline solution of H2O2 was used as complex absorbent. For simultaneous desulfurization and denitration using alkaline solution of H2O2, the inhibition of SO2 existed in the absorption of NO and the facilitation of NO existed in the absorption of SO2; the effect of SO2 on NO absorption rate was liner with 1.2 power exponent of its partial pressure in gas phase, and the apparent activation energy was 46.634 kJ·mol-1; the effect of NO on SO2 absorption rate was liner with 2.8 power exponent of its partial pressure in gas phase, and the apparent activation energy was 155.86 kJ·mol-1. The experimental results of mass transfer and reaction kinetics indicated that the mass transfer was the control step in the absorption of SO2 and reaction process was the control step in the absorption of NO; the obtained apparent activation energies for pseudo-first-order reaction were 42.654 kJ·mol-1 and 27.768 kJ·mol-1 respectively.
基于当前研究热点,论文详细地研究了亚氯酸钠/次氯酸钠溶液和过氧化氢/碱性溶液两种新型复合吸收剂体系中影响同时脱硫脱硝的因素,发现吸收剂溶液pH、吸收剂浓度、反应温度和吸收剂组成及比例对脱除效率影响显著。研究获得了两种新型复合吸收剂体系最佳脱硫脱硝实验条件。其中以亚氯酸钠／次氯酸钠溶液为吸收剂的最佳实验条件为：溶液pH为5.5,次氯酸钠与亚氯酸钠摩尔比为4,反应温度为50℃；在最佳条件下,二氧化硫脱除效率几乎达到100%,氮氧化物脱除效率达到80%。过氧化氢／碱性溶液为吸收剂的最佳实验条件为：溶液pH为10.5,过氧化氢浓度为0.8175 mol·L-1,反应温度为47.5℃；在最佳条件下,二氧化硫脱除效率几乎达到100%,氮氧化物脱除效率达到70%。
通过新型复合吸收剂同时脱硫脱硝产物分析,揭示了脱除反应机理,其中亚氯酸钠/次氯酸钠溶液同时脱硫脱硝反应历程为以亚氯酸根离子、次氯酸及中间产物二氧化氯和氯气共同与二氧化硫和一氧化氮发生了氧化吸收反应,且反应可同时发生于气液两相；过氧化氢碱性溶液同时脱硫脱硝反应历程为过氧化氢、过氧氢根离子及相关自由基在液相共同与二氧化硫和一氧化氮发生了氧化吸收反应。
基于新型复合吸收剂同时脱硫脱硝宏观反应动力学研究表明,亚氯酸钠/次氯酸钠溶液同时脱硫脱硝反应过程中二氧化硫分压和一氧化氮分压的分级数均为一级,宏观反应平均活化能分别为21.598 kJ·mol-1和8.166 kJ·mol-1。过氧化氢碱性溶液脱硫脱硝反应过程中二氧化硫分压和一氧化氮分压的分级数均为一级,宏观反应平均活化能分别为1.378 kJ·mol-1和3.722 kJ·mol-1;同时脱硫脱硝时,二氧化硫对一氧化氮吸收具有抑制作用,对一氧化氮吸收速率影响与其气相分压成1.2次方关系,抑制反应活化能为46.634 kJ·mol-1;一氧化氮对二氧化硫的吸收具有促进作用,对二氧化硫吸收速率影响与其气相分压成2.8次方关系,促吸收反应活化能为155.86 kJ·mol-1;同时脱硫脱硝传质反应动力学研究表明,二氧化硫吸收为传质控制步骤,一氧化氮吸收为反应控制步骤,一级反应平均活化能分别为42.654 kJ·mol-1和27.768 kJ·mol-1。
So far, a series of mature technologies have successively developed to remove single pollutant such as dust, SO2, NOx, and some have been the mainstream processes in the market and applied in engineering, such as electrostatic precipitation technology, wet flue gas dcsulfurization technology with calcium base absorbent, selective catalytic reduction (SCR) denitration technology, selective non-catalytic reduction (SNCR) denitration technology and mercury technology with activated carbon. But it has obvious characteristic that one technology is only used to remove one pollutant by a set of special equipment. For multi-pollutant removal, the graded treatment mode has some problems such as big floor occupation, high equipment investment and operating cost, high energy consumption, less stability of flue gas system. In order to obtain better economy and applicability of the coal-fired pollution control, the research on simultaneous removal of multi-pollutants has important realistic significance, and has become a current new field in both at home and abroad.
Based on the current research focus, the influence factors on removal efficiencies of SO2 and NO in two new complex absorbent system including the solution of NaClO2/NaCIO and alkaline solution of H2O2 were investigated detailedly in this paper.These factors such as solution pH, absorbent concentration, reaction temperature, absorbent composition and proportion have significant effects on removal efficiencies of SO2 and NO. The best experimental conditions of desulfurization and denitration were obtained based on two new complex absorbent system. The optimal removal conditions based on the solution of NaClO2/NaClO included the solution pH was 5.5, the molar ratio of NaCIO to NaCIO2 was 4, and the absorption temperature was 50℃. Under the best conditions, the removal efficiency of SO2 reached almost 100%, and the removal efficiency of NOx reached 80%. The optimal removal conditions based on the alkaline solution of H2O2 included the solution pH was 10.5, the H2O2 concentration was 0.8175 mol·L-1, and the absorption temperature was 47.5℃. Under the best conditions, the removal efficiency of SO2 reached almost 100%, and the removal efficiency of NOx reached 70%.
The removal reaction mechanisms was revealed according to product analysis results of desulfurization and denitration, the oxidation absorption reactions of SO2 and NO with chlorite anion, hypochlorite and intermediate products such as chlorine dioxide and chlorine could occur when solution of NaClO2/NaClO was used as complex absorbent. Moreover, the oxidation reactions may happen in both gas phase and liquid phase. The oxidation absorption reactions of SO2 and NO with hydrogen peroxide, peroxide anion and related free radicals could occur when alkaline solution of H2O2 was used as complex absorbent.
The macro-kinetics experimental results of simultaneous desulfurization and denitration indicated that the apparent reaction orders of SO2 and NO were both one order, and the apparent activation energies were 21.598 kJ·mol-1 and 8.166 kJ·mol-1 respectively when the solution of NaClO2/NaC10 was used as complex absorbent; the apparent reaction orders of SO2 and NO were both one order, the apparent activation energies were 1.3784 kJ·mol-1 and 3.7220 kJ·mol-1 respectively when the alkaline solution of H2O2 was used as complex absorbent. For simultaneous desulfurization and denitration using alkaline solution of H2O2, the inhibition of SO2 existed in the absorption of NO and the facilitation of NO existed in the absorption of SO2; the effect of SO2 on NO absorption rate was liner with 1.2 power exponent of its partial pressure in gas phase, and the apparent activation energy was 46.634 kJ·mol-1; the effect of NO on SO2 absorption rate was liner with 2.8 power exponent of its partial pressure in gas phase, and the apparent activation energy was 155.86 kJ·mol-1. The experimental results of mass transfer and reaction kinetics indicated that the mass transfer was the control step in the absorption of SO2 and reaction process was the control step in the absorption of NO; the obtained apparent activation energies for pseudo-first-order reaction were 42.654 kJ·mol-1 and 27.768 kJ·mol-1 respectively.
引文
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