生物质燃烧过程氮和硫的迁移、转化特性研究
摘要
目前,直接燃烧发电是最为成熟和应用最广的生物质能源化利用技术。然而,尽管生物质中的氮和硫元素含量要低于燃煤等化石燃料中的值,但是随着环保法规的日益严格,其热化学转化利用过程中的氮氧化物和硫氧化物排放依然不容忽视。本文依托十二五国家科技支撑计划项目“先进生物质发电技术示范”,以开发先进的高效、低污染生物质燃烧发电技术为目的,采用热重红外联用分析仪、固定床反应装置和0.5MW循环流化床燃烧系统对生物质燃烧过程氮和硫的迁移、转化机理进行了系统的研究。本文主要研究内容和结论如下：
(1)选取国内具有代表性的几种农业废弃生物质(稻草、麦秆、玉米杆、甘蔗叶桉树皮)为研究对象,对生物质热解过程中氮的析出特性进行了系统的研究。在低温热解条件下(250℃),生物质中的氮便开始有明显的析出,并且氮的析出大部分发生在400℃以前,当热解温度达到900℃时,生物质燃料中的氮仅有不到30%残留在焦炭中。NH3和HCN是热解过程中最主要的气相含氮前驱物,且二者显示出不同的析出特性。慢速热解条件下,稻草在低温阶段(<500℃)的主要含氮气体为NH3,而在高温阶段,NH3基本停止析出,HCN仍然有较为明显的生成。快速热解条件下,特别是在高温条件下,HCN的生成量要明显高于NH3的值,鉴于HCN是生成N2O的重要前驱体,推测生物质燃烧过程的N2O排放从理论上不容忽视。
(2)采用氨基酸作为含氮前驱物制备了生物质模型焦炭化合物,并分析和研究了焦炭中的含氮结构。试验结果表明,氨基酸和纤维素混合热解过程发生了强烈的耦合反应。通过对生物质模型焦炭化合物的XPS分析发现,不论是在含氮官能团的种类,还是含氮官能团各自所占的比例方面,生物质焦都具有与低阶煤焦类似的特性。
(3)在条件可控的固定床反应装置上研究了对生物质燃烧过程中NO和N2O的生成特性。虽然生物质燃烧过程中燃料氮中的很大一部分转化为NO,但同时也有相当程度的N2O生成率。氮氧化物的生成大部分来源于挥发份氮,因此,生物质燃料具备良好的炉内脱硝潜力。在700℃～900℃的温度范围内,燃料氮向NO的转化率先升高,在达到750℃后呈微弱的降低趋势,而其对N2O的转化率则是一直降低。NO和N2O的生成率均随着氧浓度的增加而呈现出增加趋势,并且在高温条件下,上述增加的趋势变的更为明显。
(4)相比煤焦,生物质焦具有良好的还原NO活性,这对实际燃烧过程中降低NO排放具有重要的意义。研究结果表明,生物质焦炭对NO的还原作用很大程度上受到焦炭物理化学性质和反应条件的影响。随着焦炭制备温度的升高,其对NO的还原作用逐渐下降,而反应温度的升高则会明显导致焦炭还原NO的能力增强。
(5)以稻草为对象,深入研究了生物质燃烧过程中硫的迁移、转化机理。试验结果表明,稻草热解过程硫的析出主要发生在低温阶段(<400℃),且主要源于有机硫的分解。稻草焦具有很强的吸附SO2的能力,且吸附的硫主要与焦炭中的碳结构结合形成较为稳定的有机硫结构,而不是直接与K、Ca等元素反应生成无机盐类。而在焦炭后续的燃烧过程中,大部分吸附在有机碳结构上的硫能转变为无机硫酸盐的形式固存在灰相中,而这一过程主要受控于焦炭中能参与硫酸盐化反应的K、Ca等无机元素的含量。
(6)循环流化床炉内良好的气固相接触条件大大强化了燃烧过程的自固硫作用。在本文的低温燃烧模式下(<800℃),能够实现生物质燃烧SO2的零排放。提高过量空气系数能大幅度的降低CO排放,但却导致NO浓度的增加。过量空气系数对N20没有明显的影响。提高床层温度会导致NO排放的而增加,但同时却降低了N20浓度。在高温工况下,空气分级燃烧能够很大程度上的降低NO浓度,但二次风比例存在一个最佳值。在低温工况下,空气分级燃烧反而增加了NO的排放浓度。
Among various biomass utilization technologies, combustion for electricity is the most developed and widely applied because of its low costs and high reliability. However, although the nitrogen and sulfur contents in biomass fuels are relatively lower compared to coal and other fossil fuels, the nitrogen oxides and sulfur oxides during thermo-chemical conversion processes still can not be ignored with increasingly stringent environmental regulations. Funded by National Key Technology R&D Program of China (2012BAA09B01), the nitrogen and sulfur conversion mechanism during biomass combustion were systematic investigated in the present study. The main contents and conclusions in current dissertation are as follows:
(1) Five domestic representative agricultural wastes (rice straw, wheat straw, corn stalk, sugarcane leave, eucalyptus bark) were selected for this study, to investigate the nitrogen transformation characteristics during biomass pyrolysis process. The results showed that, most part of nitrogen was released in the lower temperature range (<400℃), and there was no more than30%of fuel-N retained in the char when the the pyrolysis temperature of900℃. NH3and HCN are the main N-containing species from slow pyrolysis of rice straw. Howerver, HCN yield is much higher than that of NH3during fast pyrolysis.
(2) Biomass model char samples was prepared by using amino acid as N precusors. It was found that strong coupling reactions occurred during co-pyrolysis of amino acids and cellulose. Morover, through XPS analysis, it was found that the model char samples have similar characteristics compared to low-grade coal char, concerning the type of nitrogen-containing functional group.
(3) The NO and N2O formation characteristics during biomass combustion were investigated in a well-controlled fixed bed system. It showed that there was still considerable degree of N2O conversion for biomass fuels, although NO was formed in much larger amount. Most part of NO and N2O yields were formed during devolatilization stage for biomass fuels, therefore, it can be expected to achieve ultra-low emissions of nitrogen oxides by optimizing the supply of air and fuel during biomass combustion in actual boilers. In the temperature range of700℃-900℃, the fuel-N conversion to NO increased first and then reduced slightly, while the conversion to N2O showed a continuous decreasing trend. The fuel-N conversion to NO and N2O shows a general increase trend with the increase of inlet oxygen concentration, and this phenomenon seems more obvious at higher temperatures.
(4) Compared to coal char, biomass char has excellent capability for NO reduction, which is largely influenced by char properties and reaction conditions. Chars made at lower pyrolysis temperature showed higher reactivity with NO. Moreover, the NO reduction was proportionally higher with increasing reaction temperature.
(5) The sulfur transfonnation characteristics during rice straw combustion was deeply studied. It was found that most part of fuel-S is released in the lower temperature range (<400℃), which mainly caused by decompsition of organic sulfur. SO2can be largely captured by char in the temperature range of700-900℃. And most part of the captured sulfur was incorporated with organic char matrix rather than directly retained by inherent alkali and alkaline-earth matters in the form of inorganic salts. During char combustion, substantial amounts of the captured sulfur could be retained in the ash, which was mainly limited by the alkali and alkali-earth matters available.
(6) Within the CFB combustor, the excellent gas-solid contact would greatly enhance the self-desulfurization effect during biomass combustion. And there was nearly no SO2emission when the combustion temperature was controlled below800℃. Increase the excess air ratio would greatly reduce CO emission, but lead to higher NO concentration, while there is no clear effect on N2O emission. Raise the bed temperature would increase NO emission, but at the same time reduce N2O concentration. In high temperature condition, air-staging combustion is conducive for NO reduction, but there exists an optimized secondary air ratio. However, in the low temperature condition, air-staging combustion increase NO emission on the contrary.
(1)选取国内具有代表性的几种农业废弃生物质(稻草、麦秆、玉米杆、甘蔗叶桉树皮)为研究对象,对生物质热解过程中氮的析出特性进行了系统的研究。在低温热解条件下(250℃),生物质中的氮便开始有明显的析出,并且氮的析出大部分发生在400℃以前,当热解温度达到900℃时,生物质燃料中的氮仅有不到30%残留在焦炭中。NH3和HCN是热解过程中最主要的气相含氮前驱物,且二者显示出不同的析出特性。慢速热解条件下,稻草在低温阶段(<500℃)的主要含氮气体为NH3,而在高温阶段,NH3基本停止析出,HCN仍然有较为明显的生成。快速热解条件下,特别是在高温条件下,HCN的生成量要明显高于NH3的值,鉴于HCN是生成N2O的重要前驱体,推测生物质燃烧过程的N2O排放从理论上不容忽视。
(2)采用氨基酸作为含氮前驱物制备了生物质模型焦炭化合物,并分析和研究了焦炭中的含氮结构。试验结果表明,氨基酸和纤维素混合热解过程发生了强烈的耦合反应。通过对生物质模型焦炭化合物的XPS分析发现,不论是在含氮官能团的种类,还是含氮官能团各自所占的比例方面,生物质焦都具有与低阶煤焦类似的特性。
(3)在条件可控的固定床反应装置上研究了对生物质燃烧过程中NO和N2O的生成特性。虽然生物质燃烧过程中燃料氮中的很大一部分转化为NO,但同时也有相当程度的N2O生成率。氮氧化物的生成大部分来源于挥发份氮,因此,生物质燃料具备良好的炉内脱硝潜力。在700℃～900℃的温度范围内,燃料氮向NO的转化率先升高,在达到750℃后呈微弱的降低趋势,而其对N2O的转化率则是一直降低。NO和N2O的生成率均随着氧浓度的增加而呈现出增加趋势,并且在高温条件下,上述增加的趋势变的更为明显。
(4)相比煤焦,生物质焦具有良好的还原NO活性,这对实际燃烧过程中降低NO排放具有重要的意义。研究结果表明,生物质焦炭对NO的还原作用很大程度上受到焦炭物理化学性质和反应条件的影响。随着焦炭制备温度的升高,其对NO的还原作用逐渐下降,而反应温度的升高则会明显导致焦炭还原NO的能力增强。
(5)以稻草为对象,深入研究了生物质燃烧过程中硫的迁移、转化机理。试验结果表明,稻草热解过程硫的析出主要发生在低温阶段(<400℃),且主要源于有机硫的分解。稻草焦具有很强的吸附SO2的能力,且吸附的硫主要与焦炭中的碳结构结合形成较为稳定的有机硫结构,而不是直接与K、Ca等元素反应生成无机盐类。而在焦炭后续的燃烧过程中,大部分吸附在有机碳结构上的硫能转变为无机硫酸盐的形式固存在灰相中,而这一过程主要受控于焦炭中能参与硫酸盐化反应的K、Ca等无机元素的含量。
(6)循环流化床炉内良好的气固相接触条件大大强化了燃烧过程的自固硫作用。在本文的低温燃烧模式下(<800℃),能够实现生物质燃烧SO2的零排放。提高过量空气系数能大幅度的降低CO排放,但却导致NO浓度的增加。过量空气系数对N20没有明显的影响。提高床层温度会导致NO排放的而增加,但同时却降低了N20浓度。在高温工况下,空气分级燃烧能够很大程度上的降低NO浓度,但二次风比例存在一个最佳值。在低温工况下,空气分级燃烧反而增加了NO的排放浓度。
Among various biomass utilization technologies, combustion for electricity is the most developed and widely applied because of its low costs and high reliability. However, although the nitrogen and sulfur contents in biomass fuels are relatively lower compared to coal and other fossil fuels, the nitrogen oxides and sulfur oxides during thermo-chemical conversion processes still can not be ignored with increasingly stringent environmental regulations. Funded by National Key Technology R&D Program of China (2012BAA09B01), the nitrogen and sulfur conversion mechanism during biomass combustion were systematic investigated in the present study. The main contents and conclusions in current dissertation are as follows:
(1) Five domestic representative agricultural wastes (rice straw, wheat straw, corn stalk, sugarcane leave, eucalyptus bark) were selected for this study, to investigate the nitrogen transformation characteristics during biomass pyrolysis process. The results showed that, most part of nitrogen was released in the lower temperature range (<400℃), and there was no more than30%of fuel-N retained in the char when the the pyrolysis temperature of900℃. NH3and HCN are the main N-containing species from slow pyrolysis of rice straw. Howerver, HCN yield is much higher than that of NH3during fast pyrolysis.
(2) Biomass model char samples was prepared by using amino acid as N precusors. It was found that strong coupling reactions occurred during co-pyrolysis of amino acids and cellulose. Morover, through XPS analysis, it was found that the model char samples have similar characteristics compared to low-grade coal char, concerning the type of nitrogen-containing functional group.
(3) The NO and N2O formation characteristics during biomass combustion were investigated in a well-controlled fixed bed system. It showed that there was still considerable degree of N2O conversion for biomass fuels, although NO was formed in much larger amount. Most part of NO and N2O yields were formed during devolatilization stage for biomass fuels, therefore, it can be expected to achieve ultra-low emissions of nitrogen oxides by optimizing the supply of air and fuel during biomass combustion in actual boilers. In the temperature range of700℃-900℃, the fuel-N conversion to NO increased first and then reduced slightly, while the conversion to N2O showed a continuous decreasing trend. The fuel-N conversion to NO and N2O shows a general increase trend with the increase of inlet oxygen concentration, and this phenomenon seems more obvious at higher temperatures.
(4) Compared to coal char, biomass char has excellent capability for NO reduction, which is largely influenced by char properties and reaction conditions. Chars made at lower pyrolysis temperature showed higher reactivity with NO. Moreover, the NO reduction was proportionally higher with increasing reaction temperature.
(5) The sulfur transfonnation characteristics during rice straw combustion was deeply studied. It was found that most part of fuel-S is released in the lower temperature range (<400℃), which mainly caused by decompsition of organic sulfur. SO2can be largely captured by char in the temperature range of700-900℃. And most part of the captured sulfur was incorporated with organic char matrix rather than directly retained by inherent alkali and alkaline-earth matters in the form of inorganic salts. During char combustion, substantial amounts of the captured sulfur could be retained in the ash, which was mainly limited by the alkali and alkali-earth matters available.
(6) Within the CFB combustor, the excellent gas-solid contact would greatly enhance the self-desulfurization effect during biomass combustion. And there was nearly no SO2emission when the combustion temperature was controlled below800℃. Increase the excess air ratio would greatly reduce CO emission, but lead to higher NO concentration, while there is no clear effect on N2O emission. Raise the bed temperature would increase NO emission, but at the same time reduce N2O concentration. In high temperature condition, air-staging combustion is conducive for NO reduction, but there exists an optimized secondary air ratio. However, in the low temperature condition, air-staging combustion increase NO emission on the contrary.
引文
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