动力用煤混烧生物质燃烧特性及污染物排放特性研究
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摘要
本文应用热分析技术,研究了三种不同变质程度的动力用煤和六种常见生物质(瓜子皮、甘蔗渣、糠醛渣、酒糟、梧桐木和玉米芯)及其混合物的燃烧特性,深入探讨了生物质种类、升温速率和混合比例等参数对样品燃烧特性的影响,进而得到各样品燃烧的动力学特性；应用静态燃烧试验系统对生物质和煤单独燃烧及混合燃烧的污染物排放特性进行了研究,分析了炉温、混合比例等条件对污染物排放特性的影响。
首先,本文利用TGA/SDTA851e综合热分析仪对动力用煤混烧生物质的燃烧特性进行了研究。生物质的燃烧失重分为两个阶段：第一阶段(240～380℃)是生物质中纤维和木质裂解以及挥发分释放燃烧阶段；第二阶段(>380℃)是生物质裂解后焦炭燃烧阶段。第一阶段失重范围较大,反应温度区间较窄,为生物质燃烧的主体阶段。在该区域,农业废弃物(瓜子皮、甘蔗渣、梧桐木和玉米芯)的失重率高达70%以上,工业废弃物(糠醛渣和酒糟)失重率亦在50%以上；第二阶段失重相对缓和,反应的温度变化范围较宽,此阶段的失重量和失重速率明显低于第一阶段。生物质以不同比例与煤混合燃烧的燃烧速率试验曲线与按比例折算后的曲线基本吻合,但略有差别：挥发分析出阶段试验值比折算值稍低,而在焦炭燃烧阶段试验值比折算值偏高。随着升温速率的提高,不论是单煤、单生物质还是混煤,TG曲线都向高温区移动,DTG曲线最高峰的位置也向右偏移,最大失重速率相应增大,燃烧时间缩短,可燃性指数增大。
其次,本文利用Freeman-Carroll法、改进Coats-Redfern法和Ozawa法等不同热分析曲线处理方法对试验数据进行了计算处理,求解其燃烧反应动力学参数。根据改进Coats-Redfern法,计算得到了六种生物质和三种不同变质程度煤燃烧机理函数的最佳n值,并求出了其各阶段表观活化能。结合三种动力学分析方法,可以得到,对于生物质与煤单独燃烧,在着火初始阶段,生物质和煤的反应活化能和频率因子均较大,而对于其燃烧的主要阶段来说,随着升温速率的升高,活化能和频率因子均逐渐减小,从而使生物质和煤的燃烧速率随升温速率的升高而逐渐增大,说明升温速率的升高有利于生物质和煤活性的提高。Ozawa法求解结果从另一角度进一步表明,在不同的燃烧阶段,生物质与煤燃烧反应的活化能是不同的,随着反应度α的增大,生物质的活化能先增大后减小,而煤及生物质混煤的活化能则逐渐减小。
最后,本文利用静态燃烧试验系统研究了动力用煤混烧生物质时的硫、氮污染物排放特性,并考察了炉温及混合比例等因素对其影响规律。研究表明,单一煤燃烧时,SO2排放明显分为两个阶段：第一阶段对应煤挥发分析出着火阶段,为煤中有机硫和部分黄铁矿硫燃烧形成；第二阶段为需要更高温度才能燃烧的有机硫燃烧、黄铁矿硫及少量的硫酸盐硫形成。单一生物质燃烧时,除糠醛渣外,均形成单一SO2释放峰,而糠醛渣的SO2释放特点则与煤相似。除糠醛渣外,生物质与煤混烧时,随着生物质比例增大,SO2释放峰减小,SO2排放总量减小,SO2排放时间缩短；对于糠醛渣,随着糠醛渣比例的增大,当其含硫量低于煤时,SO2排放总量减小；当其含硫量高于煤时,SO2排放总量则增大。对于生物质混煤,在燃烧前期,炉温越低,易分解有机硫析出越快,SO2析出越快,燃烧后期则是炉温越高,难分解有机硫析出越快,SO2析出越快,与单一煤的规律基本一致；除甘蔗渣和梧桐木外,随着炉温的升高,SO2排放总量先增大后减小,而甘蔗渣和梧桐木混煤的SO2排放总量则逐渐增大；随着炉温的升高,SO2排放时间缩短,SO2转化率先增大,后减小。
单一煤燃烧时,烟煤形成两个NO释放峰,贫煤和无烟煤均形成较平坦的一个NO释放峰；单一生物质燃烧时,除酒糟和糠醛渣外,生物质皆为一个NO释放峰,而酒糟的NO释放呈明显的双峰结构,糠醛渣的NO释放不均匀,但总体上呈双峰趋势；相对于煤来说,生物质的NO释放时间较短,主要集中在燃烧前期。煤和生物质单独燃烧时,随着样品含氮量的增大,煤和生物质的NO转化率总体呈减小趋势,但NO排放总量与样品自身含氮量之间无明显的规律性。生物质与不同变质程度的煤混烧时,生物质的加入使得NO释放提前,释放所用时间缩短,且随着生物质比例的增大,NO排放时间越来越短。除酒糟外,随着生物质比例的增大,NO排放总量呈下降趋势,而对于含氮量大于煤的酒糟,NO排放总量则是先增大,后减小。
In this paper, the combustion characteristics of three different ranks of steam coal and six common biomass (including sunflower-seed husks, bagasse, furfural residue, vinasse, platanewood and corncob) and their blending were studied using thermo-gravimetric analysis technique respectively, and impacts of biomass type, heating rate and the blending ratio on the combustion characteristics of samples were researched, which led to the dynamics of the sample combustion; a tube heating furnace was applied to study the pollutant emission characteristics of separate biomass, coal and their blending, and analyze the impacts of furnace temperature and blending ratio on the pollutant emission characteristics.
First, this paper utilized TGA/SDTA851e comprehensive thermal analyzer to study the combustion characteristics of steam coal blended with biomass. Weight loss of biomass combustion fell into two stages:the first stage (240～380℃) was cellulose and lignin pyrolysis and release and combustion of volatile; the second one (＞380℃) was the coke combustion stage. The scope of weight loss in the first phase was large, with a narrow temperature range, which was the main phase of biomass combustion. In the region, the weight loss rate of agricultural waste (sunflower-seed husks, bagasse, platanewood and corncob) was as high as 70%, and that of industrial waste (furfural residue and vinasse) was 50% or more. The weight loss in the second stage was relatively smoothing, with a wide reaction temperature range, whose weight loss and weight loss rate were significantly lower than those of the first stage. The actual burning rate curves of coal blended with biomass in various ratios were basically in agreement with calculated ones, but slightly different:the experimental data of devolatilization stage was slightly lower than the calculated value, and that of coke combustion stage was higher than the calculated value. With the increase of heating rate, to whether single coal, biomass or their blending, TG curves moved to higher temperature, DTG curve peak position was also deviated to the right, the maximum weight loss rate correspondingly increased, while the combustion time reduced, and flammability index increased.
Secondly, in this paper, different treatments of thermal analysis curves containing Freeman-Carroll method, improved Coats-Redfern method and Ozawa method were utilized to compute the experimental data, solving the kinetic parameters of its combustion. According to the improved Coats-Redfern method, the best'n'value of combustion mechanism function of six kinds of biomass and three different ranks of coal were calculated, solving the apparent activation energy of their various stages. With a combination of three kinds of dynamic analysis methods, it was found that for the combustion of biomass and coal alone, in the initial stages of combustion, the reaction activation energy and frequency factor of biomass and coal were large, and for the main stage of combustion, as the heating rate increased, the activation energy and frequency factor were gradually reduced, so that burning rate of biomass and coal gradually increased with the increased heating rate, indicating the increase of heating rate was conducive to biomass and coal activity. Ozawa method results further showed from another side, in different stages of combustion, combustion activation energy of biomass and coal was different, and as the reaction degree'a'increased, the activation energy of biomass increased first and then decreased, while activation energy of coal and blending of coal and biomass was decreased.
Finally, using the tube heating furnace the sulfur and nitrogen emission characteristics of combustion of steam coal blended with biomass, and influence laws of factors such as furnace temperature and blending ratio were investigated. The results showed that in coal combustion, SO2 release was divided into two phases:the first one corresponded to the combustion stage of devolatilization in coal, which was formed by combustion of the organic sulfur and part of pyrite sulfur in coal; the second one was formed by organic sulfur, pyrite sulfur and a small amount of sulfate sulfur, whose combustion needed a high temperature. In biomass combustion except furfural residue, one single peak of SO2 release was formed, and SO2 release characteristics of furfural residue were similar to coal. Except furfural residue, in the combustion of coal blended with biomass, as the proportion of biomass increased, there was a reduction in SO2 release peak, SO2 emissions, and SO2 emission time; for furfural residue, with the increase of the furfural residue ratio, SO2 emissions reduced when its sulfur content was lower than coal; when higher, SO2 emissions increased. For coal blended with biomass, in the former combustion, the lower furnace temperature was, the faster the precipitation of easily decomposable organic sulfur was, the faster SO2 release was, and in the latter combustion, the higher the furnace temperature was, the faster the precipitation of refractory organic sulfur was, the faster SO2 release was, which was consistent with the rule of single coal; Except bagasse and platanewood, with the rise of furnace temperature, SO2 emissions first increased and then decreased, while for coal blended with bagasse and platanewood, SO2 emissions increased gradually; With the increase of furnace temperature, SO2 emission time decreased, and SO2 conversion ratio first increased, then decreased.
In single coal combustion, NO release of bituminous coal formed two peaks, while that of lean coal and anthracite both formed one relatively flat peak; While in single biomass combustion, except vinasse and furfural residue, the NO release of all biomass was one peak, while that of vinasse was apparent double peak structure, and that of furfural residue was uneven, with a overall double peak trend. Compared with coal, the NO release time of biomass was short, and mainly concentrated in the former combustion. In combustion of coal and biomass alone, with the increase of nitrogen content in samples, the NO conversion ratio of coal and biomass decreased overall, but the NO emissions had no obvious regularity with nitrogen content of the sample itself. In combustion of coal blended with biomass, the biomass made NO release earlier, and release time decrease, and with the increase of the biomass ratio, NO emission time reduced. Except vinasse, with the increase of biomass ratio, NO emissions decreased, while for vinasse whose nitrogen was higher than that of coal, NO emissions first increased, then decreased.
首先,本文利用TGA/SDTA851e综合热分析仪对动力用煤混烧生物质的燃烧特性进行了研究。生物质的燃烧失重分为两个阶段：第一阶段(240～380℃)是生物质中纤维和木质裂解以及挥发分释放燃烧阶段；第二阶段(>380℃)是生物质裂解后焦炭燃烧阶段。第一阶段失重范围较大,反应温度区间较窄,为生物质燃烧的主体阶段。在该区域,农业废弃物(瓜子皮、甘蔗渣、梧桐木和玉米芯)的失重率高达70%以上,工业废弃物(糠醛渣和酒糟)失重率亦在50%以上；第二阶段失重相对缓和,反应的温度变化范围较宽,此阶段的失重量和失重速率明显低于第一阶段。生物质以不同比例与煤混合燃烧的燃烧速率试验曲线与按比例折算后的曲线基本吻合,但略有差别：挥发分析出阶段试验值比折算值稍低,而在焦炭燃烧阶段试验值比折算值偏高。随着升温速率的提高,不论是单煤、单生物质还是混煤,TG曲线都向高温区移动,DTG曲线最高峰的位置也向右偏移,最大失重速率相应增大,燃烧时间缩短,可燃性指数增大。
其次,本文利用Freeman-Carroll法、改进Coats-Redfern法和Ozawa法等不同热分析曲线处理方法对试验数据进行了计算处理,求解其燃烧反应动力学参数。根据改进Coats-Redfern法,计算得到了六种生物质和三种不同变质程度煤燃烧机理函数的最佳n值,并求出了其各阶段表观活化能。结合三种动力学分析方法,可以得到,对于生物质与煤单独燃烧,在着火初始阶段,生物质和煤的反应活化能和频率因子均较大,而对于其燃烧的主要阶段来说,随着升温速率的升高,活化能和频率因子均逐渐减小,从而使生物质和煤的燃烧速率随升温速率的升高而逐渐增大,说明升温速率的升高有利于生物质和煤活性的提高。Ozawa法求解结果从另一角度进一步表明,在不同的燃烧阶段,生物质与煤燃烧反应的活化能是不同的,随着反应度α的增大,生物质的活化能先增大后减小,而煤及生物质混煤的活化能则逐渐减小。
最后,本文利用静态燃烧试验系统研究了动力用煤混烧生物质时的硫、氮污染物排放特性,并考察了炉温及混合比例等因素对其影响规律。研究表明,单一煤燃烧时,SO2排放明显分为两个阶段：第一阶段对应煤挥发分析出着火阶段,为煤中有机硫和部分黄铁矿硫燃烧形成；第二阶段为需要更高温度才能燃烧的有机硫燃烧、黄铁矿硫及少量的硫酸盐硫形成。单一生物质燃烧时,除糠醛渣外,均形成单一SO2释放峰,而糠醛渣的SO2释放特点则与煤相似。除糠醛渣外,生物质与煤混烧时,随着生物质比例增大,SO2释放峰减小,SO2排放总量减小,SO2排放时间缩短；对于糠醛渣,随着糠醛渣比例的增大,当其含硫量低于煤时,SO2排放总量减小；当其含硫量高于煤时,SO2排放总量则增大。对于生物质混煤,在燃烧前期,炉温越低,易分解有机硫析出越快,SO2析出越快,燃烧后期则是炉温越高,难分解有机硫析出越快,SO2析出越快,与单一煤的规律基本一致；除甘蔗渣和梧桐木外,随着炉温的升高,SO2排放总量先增大后减小,而甘蔗渣和梧桐木混煤的SO2排放总量则逐渐增大；随着炉温的升高,SO2排放时间缩短,SO2转化率先增大,后减小。
单一煤燃烧时,烟煤形成两个NO释放峰,贫煤和无烟煤均形成较平坦的一个NO释放峰；单一生物质燃烧时,除酒糟和糠醛渣外,生物质皆为一个NO释放峰,而酒糟的NO释放呈明显的双峰结构,糠醛渣的NO释放不均匀,但总体上呈双峰趋势；相对于煤来说,生物质的NO释放时间较短,主要集中在燃烧前期。煤和生物质单独燃烧时,随着样品含氮量的增大,煤和生物质的NO转化率总体呈减小趋势,但NO排放总量与样品自身含氮量之间无明显的规律性。生物质与不同变质程度的煤混烧时,生物质的加入使得NO释放提前,释放所用时间缩短,且随着生物质比例的增大,NO排放时间越来越短。除酒糟外,随着生物质比例的增大,NO排放总量呈下降趋势,而对于含氮量大于煤的酒糟,NO排放总量则是先增大,后减小。
In this paper, the combustion characteristics of three different ranks of steam coal and six common biomass (including sunflower-seed husks, bagasse, furfural residue, vinasse, platanewood and corncob) and their blending were studied using thermo-gravimetric analysis technique respectively, and impacts of biomass type, heating rate and the blending ratio on the combustion characteristics of samples were researched, which led to the dynamics of the sample combustion; a tube heating furnace was applied to study the pollutant emission characteristics of separate biomass, coal and their blending, and analyze the impacts of furnace temperature and blending ratio on the pollutant emission characteristics.
First, this paper utilized TGA/SDTA851e comprehensive thermal analyzer to study the combustion characteristics of steam coal blended with biomass. Weight loss of biomass combustion fell into two stages:the first stage (240～380℃) was cellulose and lignin pyrolysis and release and combustion of volatile; the second one (＞380℃) was the coke combustion stage. The scope of weight loss in the first phase was large, with a narrow temperature range, which was the main phase of biomass combustion. In the region, the weight loss rate of agricultural waste (sunflower-seed husks, bagasse, platanewood and corncob) was as high as 70%, and that of industrial waste (furfural residue and vinasse) was 50% or more. The weight loss in the second stage was relatively smoothing, with a wide reaction temperature range, whose weight loss and weight loss rate were significantly lower than those of the first stage. The actual burning rate curves of coal blended with biomass in various ratios were basically in agreement with calculated ones, but slightly different:the experimental data of devolatilization stage was slightly lower than the calculated value, and that of coke combustion stage was higher than the calculated value. With the increase of heating rate, to whether single coal, biomass or their blending, TG curves moved to higher temperature, DTG curve peak position was also deviated to the right, the maximum weight loss rate correspondingly increased, while the combustion time reduced, and flammability index increased.
Secondly, in this paper, different treatments of thermal analysis curves containing Freeman-Carroll method, improved Coats-Redfern method and Ozawa method were utilized to compute the experimental data, solving the kinetic parameters of its combustion. According to the improved Coats-Redfern method, the best'n'value of combustion mechanism function of six kinds of biomass and three different ranks of coal were calculated, solving the apparent activation energy of their various stages. With a combination of three kinds of dynamic analysis methods, it was found that for the combustion of biomass and coal alone, in the initial stages of combustion, the reaction activation energy and frequency factor of biomass and coal were large, and for the main stage of combustion, as the heating rate increased, the activation energy and frequency factor were gradually reduced, so that burning rate of biomass and coal gradually increased with the increased heating rate, indicating the increase of heating rate was conducive to biomass and coal activity. Ozawa method results further showed from another side, in different stages of combustion, combustion activation energy of biomass and coal was different, and as the reaction degree'a'increased, the activation energy of biomass increased first and then decreased, while activation energy of coal and blending of coal and biomass was decreased.
Finally, using the tube heating furnace the sulfur and nitrogen emission characteristics of combustion of steam coal blended with biomass, and influence laws of factors such as furnace temperature and blending ratio were investigated. The results showed that in coal combustion, SO2 release was divided into two phases:the first one corresponded to the combustion stage of devolatilization in coal, which was formed by combustion of the organic sulfur and part of pyrite sulfur in coal; the second one was formed by organic sulfur, pyrite sulfur and a small amount of sulfate sulfur, whose combustion needed a high temperature. In biomass combustion except furfural residue, one single peak of SO2 release was formed, and SO2 release characteristics of furfural residue were similar to coal. Except furfural residue, in the combustion of coal blended with biomass, as the proportion of biomass increased, there was a reduction in SO2 release peak, SO2 emissions, and SO2 emission time; for furfural residue, with the increase of the furfural residue ratio, SO2 emissions reduced when its sulfur content was lower than coal; when higher, SO2 emissions increased. For coal blended with biomass, in the former combustion, the lower furnace temperature was, the faster the precipitation of easily decomposable organic sulfur was, the faster SO2 release was, and in the latter combustion, the higher the furnace temperature was, the faster the precipitation of refractory organic sulfur was, the faster SO2 release was, which was consistent with the rule of single coal; Except bagasse and platanewood, with the rise of furnace temperature, SO2 emissions first increased and then decreased, while for coal blended with bagasse and platanewood, SO2 emissions increased gradually; With the increase of furnace temperature, SO2 emission time decreased, and SO2 conversion ratio first increased, then decreased.
In single coal combustion, NO release of bituminous coal formed two peaks, while that of lean coal and anthracite both formed one relatively flat peak; While in single biomass combustion, except vinasse and furfural residue, the NO release of all biomass was one peak, while that of vinasse was apparent double peak structure, and that of furfural residue was uneven, with a overall double peak trend. Compared with coal, the NO release time of biomass was short, and mainly concentrated in the former combustion. In combustion of coal and biomass alone, with the increase of nitrogen content in samples, the NO conversion ratio of coal and biomass decreased overall, but the NO emissions had no obvious regularity with nitrogen content of the sample itself. In combustion of coal blended with biomass, the biomass made NO release earlier, and release time decrease, and with the increase of the biomass ratio, NO emission time reduced. Except vinasse, with the increase of biomass ratio, NO emissions decreased, while for vinasse whose nitrogen was higher than that of coal, NO emissions first increased, then decreased.
引文
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