生物质燃烧及其还原氮氧化物的机理研究及应用
摘要
随着温室效应的加剧，被认为是“CO_2零排放”的生物质燃料越来越受到关注，但由于生物质中碱金属和氯含量过高，严重的结焦问题使得大多数生物质直燃设备无法正常运行，而将生物质与煤混燃则能显著缓解结焦问题；同时由于生物质中挥发份超过70%，将其作为再燃燃料还能对NOx起到显著的还原效果。本文围绕生物质燃烧技术，分别在热重、沉降炉及300MW煤粉炉内，对生物质直燃和混燃的基础燃烧特性及在工程示范应用中涉及到的关键问题进行了研究；并对生物质混燃过程中生物质焦碳和生物质气对NOx的还原机理进行了深入研究。
首先，利用热重全面系统的研究了生物质的燃烧特性及其与煤混燃的协同效应。研究发现：生物质在富氧条件下的着火相对于空气条件发生了延迟，该延迟在焦碳燃烧阶段尤为显著；氧气浓度的提高显著改善了煤的着火，但对生物质着火的影响较小；秸秆类生物质焦的着火温度显著低于于木质类生物质焦，而木质类焦的着火温度甚至高于煤焦。混燃试验表明，生物质与煤混燃总是存在对总体着火有利的协同效应，秸秆类生物质混燃对着火特性的改善幅度大于木质类生物质，而自身着火特性越恶劣的煤种与同一生物质混燃产生的协同效应则越显著；并且O_2/CO_2气氛下混燃协同效应的显著性小于O_2/N_2环境。
其次，利用沉降炉试验模拟了实际生物质直燃设备受热面上结焦核心层的形成，并将试验结果与某生物质直燃电厂的焦样数据进行了对比。研究发现：最初在受热面上沉积的是纳米级的含硫碱金属盐的气溶胶颗粒，主要的元素组成为K、S、O和Na，据此提出了以含硫的碱金属盐为核心的生物质结焦形成机理；混燃测试则证明当混燃比例低于0.2时，混燃对结焦特性无显著影响。
最后，在某300MW燃煤机组上进行了生物质的混燃试验，不需电厂增加设备投资，利用现有的磨煤机对压型生物质进行单独磨制并送入炉内燃烧，使得规模化利用生物质从工程应用的角度实现了生产组织和设备选取的简化；由于该试验的成功实施，该技术已经在某电厂得到连续应用。研究得到了该型机组混燃生物质的上限热量输入比例16.1%，并证明了在本试验范围内混燃生物质不会影响飞灰在建筑行业的应用，同时获得了大型燃煤机组混燃生物质对炉内温度、污染物排放、燃烧效率的影响规律。
作为研究生物质焦和生物质气对NOx还原的基础，首先对生物质热解过程中气相组份的析出及残余焦碳的特性进行了全面分析，获得了含N、S或Cl组份的析出规律，以及制焦温度对焦碳特性的影响。研究发现：随着热解温度升高至800℃，Cl和K含量已显著降低，当温度进一步升高至1000℃，生物质焦样中的Cl已完全析出；对于秸秆类焦存在一优化的制焦温度800℃，该温度下制得焦碳的比表面积最为发达，着火和燃烧特性最佳。生物质焦对NOx异相还原机理的研究在固定床上进行，研究发现：焦与NO反应从动力学控制到扩散控制的普遍转折区域为800~900℃；制焦温度对焦-NO反应活化能的影响不大，麦秆焦与NO反应的活化能(89.78-95.41kJ.mol~(-1))低于木屑焦(115.22~(-1)22.79kJ.mol~(-1))和烟煤焦(108.59~(-1)17.63kJ.mol~(-1))，三种燃料焦与NO的反应级数约为0.85；麦秆焦、木屑焦和烟煤焦与N_2O反应的活化能则分别为74.64kJ.mol~(-1)、122.06kJ.mol~(-1)和127.01kJ.mol~(-1)，三种焦与N_2O的反应级数均约等于1。生物质气均相还原NOx的研究主要通过动力学计算进行，首先建立了能准确预测NO和N_2O还原及SNCR过程的GRI-Miller详细反应机理模型(55组份-382步)；然后利用该机理系统的分析了不同生物质气组份再燃还原NO的最佳空气过量系数，以及温度、初始浓度、停留时间、H2O浓度和CO_2浓度等的影响；最后通过对GRI-Miller机理进行简化，发展得到了32组份~(-1)79步的骨架机理和25组份-21步的简化机理，通过与文献中有关数据及详细机理计算结果的对比，本文得到的骨架机理和简化机理可广泛应用于预测生物质气的着火、一维预混火焰特性、含NO和N_2O的再燃过程及SNCR过程。
With the deterioration in the greenhouse effects, more and more attention has been attractedby biomass which is considered as a CO_2-neutral fuel. However, because the content ofalkali and chlorine in biomass is high, combustion of100%biomass will result in severeproblems of slagging and corrosion, and this can be effectively avoided by biomass co-firingwith coal. Meanwhile, due to the high content of volatile, biomass co-firing with coal as acertain method can also achieve a high efficiency in NOx reduction. Aiming at biomasscombustion and biomass co-firing technology, the basic combustion characteristics and thekey problems during the industry application are investigated, and the investigation on thereductions of NOx by biomass char and gas are also presented. The main conclusions aresummerized as follows:
Firstly, thermogravimetry (TG) is adopted to study the biomass combustion characteristicsand the synergistic effect during biomass co-firing. Results show that the ignition of biomassis delayed under oxygen-combustion conditioin, and the delay effect is more significant forchar combustion. The increasing of oxygen concentration improves the ignition of coalsignificantly but affects the ignition of biomass less. Tests on the combustion of biomasschar show that the iginition temperature of straw char is significantly lower than that ofwood char and coal char, and the ignition temperature of wood char is even much higherthan that of coal. Tests on biomass co-firing show that there is a positive synergistic effect toimprove the general iginition characteristics of biomass and coal, and the synergistic effect ismore significant for biomass of straw, for coal of worse iginition characteristic and for thecondition of O_2/N_2than that of O_2/CO_2.
Secondly, the ash deposition and slagging on the heating surface are simulated in a drop tubefurnace of laboratory scale, and comapred with the samples from biomass-fired power plant.Results from laboratory investigation show that the initial deposition layer appear asponge-like structure of aerosols with a diameter scale of10~100nm, which should bedeveloped by the accumulation of nano-sulfate particles. There is no chlorine detected in theinitial layer, and the main elements are K, S, O and Na, and the results are correspondingwith that from the samples of biomass-fired power plant. Tests on biomass co-firing showthat biomass co-firing will not affect the slagging characteristics when the co-firing mass ratio is lower than20%. Based on the results of laboratory and industrial furnace, amechanism on the core role of sulfate aerosols in biomass ash deposition is proposed.
Finally, mold biomass pellets have been utilized on a300MW pulverized coal-fired furnacein China for the first time. Biomass was ground and transported using the existing millsystem without using any additional equipment, which achieves the simplification ofbiomass co-firing in a large scale in the practical engineering application. Experimentalresults show that the upper limit ratio of biomass heat input for this coal-fired unit is16.1%,under which, biomass co-firing will not affect the quality of the fly ash to be used in thecement industry. Meanwhile, it also obtains the effect of biomass co-firing on temperatureprofile in furnace, pollution emission and combustion efficiency. Because of the successfuloperation of this experiment, this biomass co-firing technology has been sustainably appliedin a power plant under the support of Shaanxi Provincial Development and ReformCommission.
Before the investigation on the reduction of NOx by biomass gas and biomass char, thevolatile emission and residual char properties during biomass pyrolysis are comprehensivelyanalyzed. It demonstrates the transformation rules of nitrogen, sulfur and chlorine, and theeffect of pyrolysis temperature on the properties of biomasss char. Results show that thecontents of chlorine and potassium in biomass char have greatly decreased at the processingtemperature800℃, and there is no chlorine in the residual biomass char when the processingtemperature is higher than1000℃. For biomass char of straw with high content of potassiumand chlorine, there is a optimal pyrolysis temperature800℃, under this temperature, thebiomass char holds the most developed pore structures, the largest surface area and the bestcombustion activity.
Experiments of NOx reduction by biomass char are conducted in a fixed bed system. Resultsshow that for the reaction between biomass char and NO, there is a general transitiontemperature region (800~900℃) from dynamic-control to diffusion-control, and the effect oftemperature of char preparing on the apparent activation energy is not significant. Theapparent activation energy for the reaction between NO and straw char (89.78~95.41kJ.mol~(-1)) is lower than that for wood char (115.22~122.79kJ.mol~(-1)) and that for coal char(108.59~117.63kJ.mol~(-1)), and the reaction order for all the three kinds of char is around0.85.Meanwhile, for the reaction between char and N_2O, the apparent activation energy is74.64kJ.mol~(-1),122.06kJ.mol~(-1)and127.01kJ.mol~(-1)for straw char, wood char and coal charrespectively, and the reaction order for all the three kinds of char is around1.
Investigation on the reduction of NOx by biomass gas is performed by dynamic calculation.A detailed mechanism of55species and382steps is constructed to accurately predict thereduction of NO and N_2O by biomass gas, and NH3transformation in SNCR process. Thedetailed mechanism is used to systematically analyze the potential optimal value of excess air coefficient for the maximum NO reduction rate during biomass gas reburning. The effectsof reaction temperature, initial NO concentration, residual time, H2O and CO_2concentrationare also considered. Finally, a skeletal mechanism (32species and179steps) and reducedmechanism (25species and21steps) is developed from the detailed mechanism. Bycomparing the results calculated using skeletal mechanism and reduced mechanism with theresults from experiments and calculation using detailed mechanism, it is verified that boththe skeletal mechanism and reduced mechanism can be used to well predict the iginitiondelay, flame propagation speed, NH3transformation, reduction of NO and N_2O during thecombustion of biomass gas.
首先，利用热重全面系统的研究了生物质的燃烧特性及其与煤混燃的协同效应。研究发现：生物质在富氧条件下的着火相对于空气条件发生了延迟，该延迟在焦碳燃烧阶段尤为显著；氧气浓度的提高显著改善了煤的着火，但对生物质着火的影响较小；秸秆类生物质焦的着火温度显著低于于木质类生物质焦，而木质类焦的着火温度甚至高于煤焦。混燃试验表明，生物质与煤混燃总是存在对总体着火有利的协同效应，秸秆类生物质混燃对着火特性的改善幅度大于木质类生物质，而自身着火特性越恶劣的煤种与同一生物质混燃产生的协同效应则越显著；并且O_2/CO_2气氛下混燃协同效应的显著性小于O_2/N_2环境。
其次，利用沉降炉试验模拟了实际生物质直燃设备受热面上结焦核心层的形成，并将试验结果与某生物质直燃电厂的焦样数据进行了对比。研究发现：最初在受热面上沉积的是纳米级的含硫碱金属盐的气溶胶颗粒，主要的元素组成为K、S、O和Na，据此提出了以含硫的碱金属盐为核心的生物质结焦形成机理；混燃测试则证明当混燃比例低于0.2时，混燃对结焦特性无显著影响。
最后，在某300MW燃煤机组上进行了生物质的混燃试验，不需电厂增加设备投资，利用现有的磨煤机对压型生物质进行单独磨制并送入炉内燃烧，使得规模化利用生物质从工程应用的角度实现了生产组织和设备选取的简化；由于该试验的成功实施，该技术已经在某电厂得到连续应用。研究得到了该型机组混燃生物质的上限热量输入比例16.1%，并证明了在本试验范围内混燃生物质不会影响飞灰在建筑行业的应用，同时获得了大型燃煤机组混燃生物质对炉内温度、污染物排放、燃烧效率的影响规律。
作为研究生物质焦和生物质气对NOx还原的基础，首先对生物质热解过程中气相组份的析出及残余焦碳的特性进行了全面分析，获得了含N、S或Cl组份的析出规律，以及制焦温度对焦碳特性的影响。研究发现：随着热解温度升高至800℃，Cl和K含量已显著降低，当温度进一步升高至1000℃，生物质焦样中的Cl已完全析出；对于秸秆类焦存在一优化的制焦温度800℃，该温度下制得焦碳的比表面积最为发达，着火和燃烧特性最佳。生物质焦对NOx异相还原机理的研究在固定床上进行，研究发现：焦与NO反应从动力学控制到扩散控制的普遍转折区域为800~900℃；制焦温度对焦-NO反应活化能的影响不大，麦秆焦与NO反应的活化能(89.78-95.41kJ.mol~(-1))低于木屑焦(115.22~(-1)22.79kJ.mol~(-1))和烟煤焦(108.59~(-1)17.63kJ.mol~(-1))，三种燃料焦与NO的反应级数约为0.85；麦秆焦、木屑焦和烟煤焦与N_2O反应的活化能则分别为74.64kJ.mol~(-1)、122.06kJ.mol~(-1)和127.01kJ.mol~(-1)，三种焦与N_2O的反应级数均约等于1。生物质气均相还原NOx的研究主要通过动力学计算进行，首先建立了能准确预测NO和N_2O还原及SNCR过程的GRI-Miller详细反应机理模型(55组份-382步)；然后利用该机理系统的分析了不同生物质气组份再燃还原NO的最佳空气过量系数，以及温度、初始浓度、停留时间、H2O浓度和CO_2浓度等的影响；最后通过对GRI-Miller机理进行简化，发展得到了32组份~(-1)79步的骨架机理和25组份-21步的简化机理，通过与文献中有关数据及详细机理计算结果的对比，本文得到的骨架机理和简化机理可广泛应用于预测生物质气的着火、一维预混火焰特性、含NO和N_2O的再燃过程及SNCR过程。
With the deterioration in the greenhouse effects, more and more attention has been attractedby biomass which is considered as a CO_2-neutral fuel. However, because the content ofalkali and chlorine in biomass is high, combustion of100%biomass will result in severeproblems of slagging and corrosion, and this can be effectively avoided by biomass co-firingwith coal. Meanwhile, due to the high content of volatile, biomass co-firing with coal as acertain method can also achieve a high efficiency in NOx reduction. Aiming at biomasscombustion and biomass co-firing technology, the basic combustion characteristics and thekey problems during the industry application are investigated, and the investigation on thereductions of NOx by biomass char and gas are also presented. The main conclusions aresummerized as follows:
Firstly, thermogravimetry (TG) is adopted to study the biomass combustion characteristicsand the synergistic effect during biomass co-firing. Results show that the ignition of biomassis delayed under oxygen-combustion conditioin, and the delay effect is more significant forchar combustion. The increasing of oxygen concentration improves the ignition of coalsignificantly but affects the ignition of biomass less. Tests on the combustion of biomasschar show that the iginition temperature of straw char is significantly lower than that ofwood char and coal char, and the ignition temperature of wood char is even much higherthan that of coal. Tests on biomass co-firing show that there is a positive synergistic effect toimprove the general iginition characteristics of biomass and coal, and the synergistic effect ismore significant for biomass of straw, for coal of worse iginition characteristic and for thecondition of O_2/N_2than that of O_2/CO_2.
Secondly, the ash deposition and slagging on the heating surface are simulated in a drop tubefurnace of laboratory scale, and comapred with the samples from biomass-fired power plant.Results from laboratory investigation show that the initial deposition layer appear asponge-like structure of aerosols with a diameter scale of10~100nm, which should bedeveloped by the accumulation of nano-sulfate particles. There is no chlorine detected in theinitial layer, and the main elements are K, S, O and Na, and the results are correspondingwith that from the samples of biomass-fired power plant. Tests on biomass co-firing showthat biomass co-firing will not affect the slagging characteristics when the co-firing mass ratio is lower than20%. Based on the results of laboratory and industrial furnace, amechanism on the core role of sulfate aerosols in biomass ash deposition is proposed.
Finally, mold biomass pellets have been utilized on a300MW pulverized coal-fired furnacein China for the first time. Biomass was ground and transported using the existing millsystem without using any additional equipment, which achieves the simplification ofbiomass co-firing in a large scale in the practical engineering application. Experimentalresults show that the upper limit ratio of biomass heat input for this coal-fired unit is16.1%,under which, biomass co-firing will not affect the quality of the fly ash to be used in thecement industry. Meanwhile, it also obtains the effect of biomass co-firing on temperatureprofile in furnace, pollution emission and combustion efficiency. Because of the successfuloperation of this experiment, this biomass co-firing technology has been sustainably appliedin a power plant under the support of Shaanxi Provincial Development and ReformCommission.
Before the investigation on the reduction of NOx by biomass gas and biomass char, thevolatile emission and residual char properties during biomass pyrolysis are comprehensivelyanalyzed. It demonstrates the transformation rules of nitrogen, sulfur and chlorine, and theeffect of pyrolysis temperature on the properties of biomasss char. Results show that thecontents of chlorine and potassium in biomass char have greatly decreased at the processingtemperature800℃, and there is no chlorine in the residual biomass char when the processingtemperature is higher than1000℃. For biomass char of straw with high content of potassiumand chlorine, there is a optimal pyrolysis temperature800℃, under this temperature, thebiomass char holds the most developed pore structures, the largest surface area and the bestcombustion activity.
Experiments of NOx reduction by biomass char are conducted in a fixed bed system. Resultsshow that for the reaction between biomass char and NO, there is a general transitiontemperature region (800~900℃) from dynamic-control to diffusion-control, and the effect oftemperature of char preparing on the apparent activation energy is not significant. Theapparent activation energy for the reaction between NO and straw char (89.78~95.41kJ.mol~(-1)) is lower than that for wood char (115.22~122.79kJ.mol~(-1)) and that for coal char(108.59~117.63kJ.mol~(-1)), and the reaction order for all the three kinds of char is around0.85.Meanwhile, for the reaction between char and N_2O, the apparent activation energy is74.64kJ.mol~(-1),122.06kJ.mol~(-1)and127.01kJ.mol~(-1)for straw char, wood char and coal charrespectively, and the reaction order for all the three kinds of char is around1.
Investigation on the reduction of NOx by biomass gas is performed by dynamic calculation.A detailed mechanism of55species and382steps is constructed to accurately predict thereduction of NO and N_2O by biomass gas, and NH3transformation in SNCR process. Thedetailed mechanism is used to systematically analyze the potential optimal value of excess air coefficient for the maximum NO reduction rate during biomass gas reburning. The effectsof reaction temperature, initial NO concentration, residual time, H2O and CO_2concentrationare also considered. Finally, a skeletal mechanism (32species and179steps) and reducedmechanism (25species and21steps) is developed from the detailed mechanism. Bycomparing the results calculated using skeletal mechanism and reduced mechanism with theresults from experiments and calculation using detailed mechanism, it is verified that boththe skeletal mechanism and reduced mechanism can be used to well predict the iginitiondelay, flame propagation speed, NH3transformation, reduction of NO and N_2O during thecombustion of biomass gas.
引文
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