O_2/CO_2气氛下木醋调质石灰石脱硫脱硝特性及机理研究
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摘要
O2/CO2燃烧技术在控制C02、SO2、NOx等污染物排放方面都表现出较强的技术优势,被认为是一项具有应用前景的燃煤污染物控制技术。有机钙可用于O2/CO2燃煤气氛下SO2和NO的同时脱除,但高昂的造价限制了其工业化应用。本文采用木醋废液调质处理石灰石,并从实验研究、动力学分析及机理分析等角度,对木醋调质石灰石(Limestone Modified by Wood Vinegar, LM-WV)在O2/CO2气氛下的热解、直接硫化、再燃脱硝以及同时脱硫脱硝反应特性和反应机理进行了研究,探索了一条采用工业废液调质处理石灰石制备廉价高效有机钙的新途径。
采用热分析方法对O2/CO2气氛下LM-WV的热解特性进行了实验研究,结果表明,未调质石灰石(Original Limestone, OL)的热解过程仅表现出一个CO2析出失重阶段,而LM-WV则表现出水分析出及焦油成分热解、丙酮析出和CO2析出三个失重阶段,较多的气体析出量导致LM-WV热解固体产物比表面积和孔容积远大于OL,固体产物孔隙发达且以中孔为主,有利于脱硫,热解气体产物在低温时以CO、CH4和C2H6为主,高温时以CO、CH4、H2和C2H2为主,可用于再燃脱硝。采用FWO法和Starink法两种无模式函数法分析O2/CO2气氛下LM-WV热解反应活化能,两种方法计算结果相近且规律相同,OL在整个热解过程中,活化能表现为单一的下降趋势,活化能值为547.80～5389.29kJ·mol-1, LM-WV热解反应活化能随着反应的进行表现出先增大后降低,再增大又降低的趋势,活化能值为102.33～1504.23kJ·mol-1。O2/CO2气氛下LM-WV热解反应机理可用分段描述的方法进行分析,OL热解反应机理可以用F1模型进行揭示,LM-WV热解第一、第二阶段反应机理可以用D3模型进行揭示,第三阶段可以用D2模型进行揭示。采用热分析方法对O2/CO2气氛下LM-WV的硫化反应特性进行了实验研究,发现LM-WV表现出比OL和分析纯醋酸钙(Calcium Acetate, CA)更好的直接硫化反应性能。温度、粒径、SO2和O2浓度对LM-WV直接硫化反应都有影响,温度越高、颗粒粒径越小、反应气氛中SO2和O2浓度越高,LM-WV直接硫化钙转化率越高,浓度超过6%以后,O2浓度变化对硫化反应影响不大。钙转化率较低时,间接硫化反应速率高于直接硫化,1173K时反应约400s时直接硫化速率超过间接硫化速率,获得的间接硫化和直接硫化钙转化率分别为60.51%和81.11%。LM-WV中源自石灰石的Na、K、Fe、Ti类杂质成分对直接硫化反应有促进作用。采用缩核模型对反应过程进行了表征,得到LM-WV和OL直接硫化反应速率常数κs和扩散系数Deff的Arrhenius表达式。动力学计算结果表明,扩散对LM-WV直接硫化反应过程的影响相比石灰石要小,石灰石经木醋调质后其直接硫化反应性能得以显著提升的原因是扩散阻力的减小
在O2/CO2气氛下利用沉降炉脱硝实验台对LM-WV再燃脱硝特性进行了研究,实验结果表明,相同实验工况条件下,LM-WV的脱硝性能优于CA。LM-WV再燃脱硝合适的再燃比为14%-17%,氧浓度为3%、停留时间为0.8s,脱硝效率随着温度的升高表现为先提高后降低的趋势,最佳反应温度为1323K,再燃比为14%时获得的脱硝效率为82.70%。先进再燃可以获得较高的脱硝效率,反应适宜的温度区间也得到显著拓宽。先进再燃脱硝氧浓度不宜过高,合适的停留时间为0.6-0.8s,氨氮比为0.75,再燃比、氨氮比分别为14%和0.75条件下,1323K时获得的最高脱硝效率为93.49%。1123-1223K时LM-WV在02/N2气氛下脱硝获得的脱硝效率略高于O2/CO2气氛,超过此温度时,LM-WV在O2/CO2气氛下获得的脱硝效率高于O2/N2气氛。O2/CO2气氛下LM-WV脱硝效率随CO2浓度的增大不断提高,高浓度的CO2对脱硝反应有促进作用。
管式炉实验系统上进行的O2/CO2气氛下煤粉预混LM-WV同时脱硫脱硝实验结果表明,LM-WV脱硫脱硝性能优于OL和CA,其脱硫脱硝效率受添加量、煤的含硫量、温度等因素影响。相同实验条件下,LM-WV在O2/CO2气氛下的脱硫脱硝性能均优于O2/N2气氛。1023-1473K实验温度范围内,LM-WV表现出良好的脱硫效果,Ca/S为2时,LM-WV能够保持80.06%以上的脱硫效率。脱硝效率随LM-WV添加量的增大和温度的升高而不断提高,Ca/S为3、温度为1373K时获得的脱硝效率为53.08%。沉降炉实验系统上进行的烟气喷入LM-WV同时脱硫脱硝实验表明,钙硫摩尔比约为2、停留时间为0.8s、无NH3和有NH3条件下,在1223K时获得最大脱硫效率为75.83%和73.16%,在1323K时获得最大脱硝效率为86.61%和94.78%。煤中添加LM-WV后,着火温度、失重峰温度以及燃尽温度均向低温方向迁移,燃烧反应活化能显著降低,说明LM-WV具备一定的助燃性能。
提出了由112种物质、677步基元反应组成的丙酮脱硝反应机理模型,用以揭示O2/CO2气氛下LM-WV脱硝反应机理。模拟计算与实验结果呈现出的规律完全一致,能够较好的预测实验结果和分析反应机理。OH与C2H6、C2H4、CH4和C2H2等反应生成碳氢离子团和HCCO,进而与NO反应将其转变为HCN。HCN能够与O反应生成NCO和NH,并通过反应NCO+NO(?)N2+CO2和NH+NO(?)N2+OH将NO还原为N2。活性基团OH、O、H是保证脱硝反应顺利进行的重要物质,但过高的活性基团浓度会加剧HCN的氧化反应。低温时O2/N2和O2/CO2气氛下LM-WV脱硝性能的差异可以归结于O2/CO2气氛下较低的OH、O、H浓度,高温时两种气氛下的差异则可归结于O2/CO2气氛下较高的碳氢气体浓度。在适于脱硝的温度条件下,通过CH4(+M)(?)CH3+H(+M)、C2H4+H(+M)(?)C2H5(+M)、 C2H6(+M)(?)CH3+CH3(+M)和C2H2+H(+M)(?)C2H3(+M)等反应,CO2可促进CH4、C2H4、C2H6和C2H2转化为CH3、C2H3和C2H5等自由基,有利于脱硝。
SO2对LM、WV脱硝反应有促进作用,SO2可以通过SO2+H(+M)(?)HOSO(+M)、HOSO+H(?)SO2+H2、SO2+O(+M)(?)SO3(+M)和HOSO+OH(?)SO2H2O等反应,消耗气氛中的活性基团H、O、OH,进而抑制脱硝反应中间产物HCN的氧化,此外,SO2还能够通过一系列反应转化为SH和SN,并通过反应SH+NO(?)SN+OH和SN+NO(?)N2+SO将NO直接还原为N2。
O2/CO2combustion is recognized as a potential technology for mitigation of CO2, SO2and NOx emissions. High concentration of SO2in the furnace under O2/CO2combustion atmosphere is beneficial to desulfurization by in-furnace desulfurization technology. Low NOx emission characteristic of O2/CO2combustion is also suitable for using economical reburning denitrification technology to remove NOx. Solid and gas products produced in the thermal decomposition of organic calcium can be used for sulfur capture and reburning denitrification, which can simultaneously control of SO2and NO emissions under O2/CO2combustion atmosphere. However, high cost of organic calcium limits its industrial application.
Wood vinegar, an organic acid waste, is used to modify natural limestone to produce organic calcium absorbent with low cost and good performance in this paper, which solves the high economic cost problem of organic calcium in practical application. Charcteristics and mechanism of thermal decomposition, direct sulfation, reburning denitrification, simultaneous desulfurization and denitrification of limestone modified by wood vinegar (LM-WV) under O2/CO2atmosphere are studied from the view of experiment, kinetic analysis and mechanism analysis.
The thermal decomposition characteristics of LM-WV under O2/CO2atmosphere are measured by thermogravimetric analysis (TGA). TGA result shows that the thermal decomposition process of limestone only shows one weight loss stage, but three for LM-WV. The major composition in the product of LM-WV is hydration calcium acetate. Initial temperature of three weight loss stages is463K,673K and1179K, which corresponds to release of water and pyrolysis of tar, release of acetone, and release of CO2, respectively. The structure of thermal decomposition product of LM-WV, measured by scanning electron microscope and nitrogen adsorption method, is much looser than that of original limestone, and the main pore is in the medium size, which shows that wood vinegar improves the pore structure of thermal decomposition product of limestone. Gas products composition analysis results show that the main gas products are CO, CH4and C2H6under low temperature conditions, and CO, CH4, H2and C2H2under high temperature conditions. These gas products provide the material basis for the denitrification reaction. FWO method and Starink method, which are two typical model-free methods, are used to calculate the activation energy during the thermal decomposition process of LM-WV under O2/CO2atmosphere. Values of activation energy calculated by FWO method and Starink method are very close, and regularities of these two methods are very consistent. Activation energy of original limestone shows a single downward trend, which indicates the monotonicity of the reaction process. In contrast, activation energy of LM-WV increases firstly then decreases, increases again and decreases finally, which indicates the characteristics of multistage of the reaction process. The most probable mechanism function inference method is used to analyze reaction mechanism of thermal decomposition. F1model can be used to describe the thermal decomposition process of limestone. The first two stages of the thermal decomposition process of LM-WV can be described by D3model, and the third stage can be described by D2model. Mechanism analysis results confirm complexity of the thermal decomposition process.
The direct sulfation reaction of LM-WV is investigated by thermogravimetic analysis method under O2/CO2atmosphere. The results show that the direct sulfation performance of LM-WV is better than both original limestone and analytical grade calcium acetate. Temperature, particle size, SO2and O2concentrations can affect the direct sulfation reaction of LM-WV. Higher temperature, SO2concentration and smaller particle size are beneficial for the direct sulfation reaction. Above6%, O2concentration has little effect on the direct sulfation reaction. Reaction rate of indirect sulfation is higher than that of direct sulfation when calcium conversion fraction is relatively low. Direct sulfation rate exceeds indirect sulfation rate after400s at1173K, and the final calcium conversion fraction of indirect sulfation and direct sulfation is60.51%and81.11%, respectively. Impurity components, including Na, K, Fe, Ti, have a promoting effect on the direct sulfation reaction. Arrhenius expressions of direct sulfation rate constant and product-layer diffusivity are calculated according to the shrinking unreacted core model. The kinetic calculation result shows that the diffusion impact of LM-WV on the direct sulfation process is less than that of original limestone, which means that the LM-WV has a lower diffusion resistance.
NO reduction characteristic of reburning using LM-WV is investigated in a drop-tube experiment system under O2/CO2atmosphere. Experimental result shows that the NO reduction performance of LM-WV is better than that of analytical grade calcium acetate under the same experimental conditions. The optimum reburning fuel fraction, O2concentration and residence time for basic reburning is14%-17%,3%and0.8s. As temperature increasing, NO reduction efficiency increases first and then decreases. The maximum NO reduction efficiency of82.70%can be obtained at1323K. NO reduction efficiency can be significantly raised, while the reaction temperature window can be obviously broaden, when ammonia is injected into reburning zone. High O2concentration is not conducive to NO reduction by advanced reburning. The optimum residence time and [NH3]/[NO] molar ratio is0.6-0.8s and0.75. The maximum NO reduction efficiency of93.49%can be obtained at1323K when the reburning fuel fraction and [NHx]/[NO] molar ratio is14%and0.75. NO reduction efficiency of LM-WV under O2/N2atmosphere is higher than that under O2/CO2atmosphere at1123-1223K. This situation will change at higher temperature. NO reduction efficiency increases with CO2concentration increasing, and high concentration of CO2can promote the denitrification reaction.
The desulfurization and denitrification characteristics of LM-WV by pre-mixed with coal under O2/CO2atmosphere are investigated on the tube furnace reactor. Experimental result shows that the desulfurization and denitrification performance of LM-WV are much better than that of both original limestone and analytical grade calcium acetate. SO2and NO reduction efficiency may be affected by addition amount, sulfur content in coal and temperature. SO2and NO reduction efficiency of LM-WV under O2/CO2atmosphere are higher than that under O2/N2atmosphere under the same experimental conditions. LM-WV shows good desulfurization performance in the experimental temperature range1023-1473K, and it can maintain SO2reduction efficiency of more than80.06%at calcium/sulfur ratio being2. NO reduction efficiency increases with addition amount increasing. NO reduction efficiency of53.08%can be obtained at1373K when calcium/sulfur ratio is3. The performance of simultaneous desulfurization and denitrification of LM-WV by injected into flue gas under O2/CO2atmosphere are investigated in the drop-tube experiment system. The maximum SO2and NO reduction efficiency of75.83%and86.61%can be obtained respectively at1223K and1323K, when the calcium/sulfur ratio and residence time is about2and0.8s. In the above conditions, when ammonia is injected into reactive zone at [NH3]/[NO] molar ratio of0.75, the maximum SO2and NO reduction efficiency of73.16%and94.78%can be obtained respectively at1223K and1323K. Ignition temperature, weight loss peak temperature and burnout temperature of coal all migrate towards the direction of low temperature after LM-WV is added into coal. At the same time, activation energy of combustion reaction significantly decreases. The above phenomenon indicates that LM-WV can improve the combustion performance of pulverized coal under O2/CO2atmosphere.
Combine oxidative decomposition model of acetone with denitrification reaction model of AA, then refer to the related experimental results, and finally get acetone denitrification reaction model including112species and677elementary reactions. Mechanism analysis shows that OH can react with C2H6, C2H4, CH4and C2H2, then generate hydrocarbon ion groups and HCCO. Hydrocarbon ion groups and HCCO can react with NO and generate HCN. HCN can be converted into NCO and NH by reacting with O. NCO and NH can reduce NO to N2through NCO+NO(?)N2+CO2and NH+NO(?)N2+OH. Reactive groups of OH, O and H are important materials which can ensure the denitrification reaction to carry out smoothly. However, excessive reactive groups may exacerbate the oxidation reaction of HCN. The difference of NO reduction efficiency of LM-WV under O2/N2atmosphere and O2/CO2atmosphere at low temperature may be caused by lower concentration of reactive groups under O2/CO2atmosphere. The difference under these two atmospheres may be caused by higher concentration of hydrocarbon gases under O2/CO2atmosphere. High concentration of CO2can promote the generation of CH4, C2H4, C2H6and C2H2. In addition, CO2can also promote the conversion of CH4, C2H4, C2H6and C2H2to free radicals, such as CH3, C2H3and C2H5, through CH4(+M)<=>CH3+H(+M), C2H4+H(+M)(?) C2H5(+M),C2H6(+M)<=> CH3+CH3(+M),C2H2+H(+M)(?) C2H3(+M). These reactions are all conducive to the denitrification reaction.
SO2can promote the denitrification reaction of LM-WV. SO2can consume reactive groups of H, O, OH through SO2+H(+M)(?)HOSO(+M),HOSO+H(?)SO2+H2SO2+O(+M)(?)SO3(+M) and HOSO+OH<=> SO2+H2O, which can inhibit the oxidation of HCN. In addition, SO2can also transform into SH and SN. Through SH+NO(?) SN+OH and SN+NO(?) N2+SO, NO can be directly reduced to N2by SH and SN.
采用热分析方法对O2/CO2气氛下LM-WV的热解特性进行了实验研究,结果表明,未调质石灰石(Original Limestone, OL)的热解过程仅表现出一个CO2析出失重阶段,而LM-WV则表现出水分析出及焦油成分热解、丙酮析出和CO2析出三个失重阶段,较多的气体析出量导致LM-WV热解固体产物比表面积和孔容积远大于OL,固体产物孔隙发达且以中孔为主,有利于脱硫,热解气体产物在低温时以CO、CH4和C2H6为主,高温时以CO、CH4、H2和C2H2为主,可用于再燃脱硝。采用FWO法和Starink法两种无模式函数法分析O2/CO2气氛下LM-WV热解反应活化能,两种方法计算结果相近且规律相同,OL在整个热解过程中,活化能表现为单一的下降趋势,活化能值为547.80～5389.29kJ·mol-1, LM-WV热解反应活化能随着反应的进行表现出先增大后降低,再增大又降低的趋势,活化能值为102.33～1504.23kJ·mol-1。O2/CO2气氛下LM-WV热解反应机理可用分段描述的方法进行分析,OL热解反应机理可以用F1模型进行揭示,LM-WV热解第一、第二阶段反应机理可以用D3模型进行揭示,第三阶段可以用D2模型进行揭示。采用热分析方法对O2/CO2气氛下LM-WV的硫化反应特性进行了实验研究,发现LM-WV表现出比OL和分析纯醋酸钙(Calcium Acetate, CA)更好的直接硫化反应性能。温度、粒径、SO2和O2浓度对LM-WV直接硫化反应都有影响,温度越高、颗粒粒径越小、反应气氛中SO2和O2浓度越高,LM-WV直接硫化钙转化率越高,浓度超过6%以后,O2浓度变化对硫化反应影响不大。钙转化率较低时,间接硫化反应速率高于直接硫化,1173K时反应约400s时直接硫化速率超过间接硫化速率,获得的间接硫化和直接硫化钙转化率分别为60.51%和81.11%。LM-WV中源自石灰石的Na、K、Fe、Ti类杂质成分对直接硫化反应有促进作用。采用缩核模型对反应过程进行了表征,得到LM-WV和OL直接硫化反应速率常数κs和扩散系数Deff的Arrhenius表达式。动力学计算结果表明,扩散对LM-WV直接硫化反应过程的影响相比石灰石要小,石灰石经木醋调质后其直接硫化反应性能得以显著提升的原因是扩散阻力的减小
在O2/CO2气氛下利用沉降炉脱硝实验台对LM-WV再燃脱硝特性进行了研究,实验结果表明,相同实验工况条件下,LM-WV的脱硝性能优于CA。LM-WV再燃脱硝合适的再燃比为14%-17%,氧浓度为3%、停留时间为0.8s,脱硝效率随着温度的升高表现为先提高后降低的趋势,最佳反应温度为1323K,再燃比为14%时获得的脱硝效率为82.70%。先进再燃可以获得较高的脱硝效率,反应适宜的温度区间也得到显著拓宽。先进再燃脱硝氧浓度不宜过高,合适的停留时间为0.6-0.8s,氨氮比为0.75,再燃比、氨氮比分别为14%和0.75条件下,1323K时获得的最高脱硝效率为93.49%。1123-1223K时LM-WV在02/N2气氛下脱硝获得的脱硝效率略高于O2/CO2气氛,超过此温度时,LM-WV在O2/CO2气氛下获得的脱硝效率高于O2/N2气氛。O2/CO2气氛下LM-WV脱硝效率随CO2浓度的增大不断提高,高浓度的CO2对脱硝反应有促进作用。
管式炉实验系统上进行的O2/CO2气氛下煤粉预混LM-WV同时脱硫脱硝实验结果表明,LM-WV脱硫脱硝性能优于OL和CA,其脱硫脱硝效率受添加量、煤的含硫量、温度等因素影响。相同实验条件下,LM-WV在O2/CO2气氛下的脱硫脱硝性能均优于O2/N2气氛。1023-1473K实验温度范围内,LM-WV表现出良好的脱硫效果,Ca/S为2时,LM-WV能够保持80.06%以上的脱硫效率。脱硝效率随LM-WV添加量的增大和温度的升高而不断提高,Ca/S为3、温度为1373K时获得的脱硝效率为53.08%。沉降炉实验系统上进行的烟气喷入LM-WV同时脱硫脱硝实验表明,钙硫摩尔比约为2、停留时间为0.8s、无NH3和有NH3条件下,在1223K时获得最大脱硫效率为75.83%和73.16%,在1323K时获得最大脱硝效率为86.61%和94.78%。煤中添加LM-WV后,着火温度、失重峰温度以及燃尽温度均向低温方向迁移,燃烧反应活化能显著降低,说明LM-WV具备一定的助燃性能。
提出了由112种物质、677步基元反应组成的丙酮脱硝反应机理模型,用以揭示O2/CO2气氛下LM-WV脱硝反应机理。模拟计算与实验结果呈现出的规律完全一致,能够较好的预测实验结果和分析反应机理。OH与C2H6、C2H4、CH4和C2H2等反应生成碳氢离子团和HCCO,进而与NO反应将其转变为HCN。HCN能够与O反应生成NCO和NH,并通过反应NCO+NO(?)N2+CO2和NH+NO(?)N2+OH将NO还原为N2。活性基团OH、O、H是保证脱硝反应顺利进行的重要物质,但过高的活性基团浓度会加剧HCN的氧化反应。低温时O2/N2和O2/CO2气氛下LM-WV脱硝性能的差异可以归结于O2/CO2气氛下较低的OH、O、H浓度,高温时两种气氛下的差异则可归结于O2/CO2气氛下较高的碳氢气体浓度。在适于脱硝的温度条件下,通过CH4(+M)(?)CH3+H(+M)、C2H4+H(+M)(?)C2H5(+M)、 C2H6(+M)(?)CH3+CH3(+M)和C2H2+H(+M)(?)C2H3(+M)等反应,CO2可促进CH4、C2H4、C2H6和C2H2转化为CH3、C2H3和C2H5等自由基,有利于脱硝。
SO2对LM、WV脱硝反应有促进作用,SO2可以通过SO2+H(+M)(?)HOSO(+M)、HOSO+H(?)SO2+H2、SO2+O(+M)(?)SO3(+M)和HOSO+OH(?)SO2H2O等反应,消耗气氛中的活性基团H、O、OH,进而抑制脱硝反应中间产物HCN的氧化,此外,SO2还能够通过一系列反应转化为SH和SN,并通过反应SH+NO(?)SN+OH和SN+NO(?)N2+SO将NO直接还原为N2。
O2/CO2combustion is recognized as a potential technology for mitigation of CO2, SO2and NOx emissions. High concentration of SO2in the furnace under O2/CO2combustion atmosphere is beneficial to desulfurization by in-furnace desulfurization technology. Low NOx emission characteristic of O2/CO2combustion is also suitable for using economical reburning denitrification technology to remove NOx. Solid and gas products produced in the thermal decomposition of organic calcium can be used for sulfur capture and reburning denitrification, which can simultaneously control of SO2and NO emissions under O2/CO2combustion atmosphere. However, high cost of organic calcium limits its industrial application.
Wood vinegar, an organic acid waste, is used to modify natural limestone to produce organic calcium absorbent with low cost and good performance in this paper, which solves the high economic cost problem of organic calcium in practical application. Charcteristics and mechanism of thermal decomposition, direct sulfation, reburning denitrification, simultaneous desulfurization and denitrification of limestone modified by wood vinegar (LM-WV) under O2/CO2atmosphere are studied from the view of experiment, kinetic analysis and mechanism analysis.
The thermal decomposition characteristics of LM-WV under O2/CO2atmosphere are measured by thermogravimetric analysis (TGA). TGA result shows that the thermal decomposition process of limestone only shows one weight loss stage, but three for LM-WV. The major composition in the product of LM-WV is hydration calcium acetate. Initial temperature of three weight loss stages is463K,673K and1179K, which corresponds to release of water and pyrolysis of tar, release of acetone, and release of CO2, respectively. The structure of thermal decomposition product of LM-WV, measured by scanning electron microscope and nitrogen adsorption method, is much looser than that of original limestone, and the main pore is in the medium size, which shows that wood vinegar improves the pore structure of thermal decomposition product of limestone. Gas products composition analysis results show that the main gas products are CO, CH4and C2H6under low temperature conditions, and CO, CH4, H2and C2H2under high temperature conditions. These gas products provide the material basis for the denitrification reaction. FWO method and Starink method, which are two typical model-free methods, are used to calculate the activation energy during the thermal decomposition process of LM-WV under O2/CO2atmosphere. Values of activation energy calculated by FWO method and Starink method are very close, and regularities of these two methods are very consistent. Activation energy of original limestone shows a single downward trend, which indicates the monotonicity of the reaction process. In contrast, activation energy of LM-WV increases firstly then decreases, increases again and decreases finally, which indicates the characteristics of multistage of the reaction process. The most probable mechanism function inference method is used to analyze reaction mechanism of thermal decomposition. F1model can be used to describe the thermal decomposition process of limestone. The first two stages of the thermal decomposition process of LM-WV can be described by D3model, and the third stage can be described by D2model. Mechanism analysis results confirm complexity of the thermal decomposition process.
The direct sulfation reaction of LM-WV is investigated by thermogravimetic analysis method under O2/CO2atmosphere. The results show that the direct sulfation performance of LM-WV is better than both original limestone and analytical grade calcium acetate. Temperature, particle size, SO2and O2concentrations can affect the direct sulfation reaction of LM-WV. Higher temperature, SO2concentration and smaller particle size are beneficial for the direct sulfation reaction. Above6%, O2concentration has little effect on the direct sulfation reaction. Reaction rate of indirect sulfation is higher than that of direct sulfation when calcium conversion fraction is relatively low. Direct sulfation rate exceeds indirect sulfation rate after400s at1173K, and the final calcium conversion fraction of indirect sulfation and direct sulfation is60.51%and81.11%, respectively. Impurity components, including Na, K, Fe, Ti, have a promoting effect on the direct sulfation reaction. Arrhenius expressions of direct sulfation rate constant and product-layer diffusivity are calculated according to the shrinking unreacted core model. The kinetic calculation result shows that the diffusion impact of LM-WV on the direct sulfation process is less than that of original limestone, which means that the LM-WV has a lower diffusion resistance.
NO reduction characteristic of reburning using LM-WV is investigated in a drop-tube experiment system under O2/CO2atmosphere. Experimental result shows that the NO reduction performance of LM-WV is better than that of analytical grade calcium acetate under the same experimental conditions. The optimum reburning fuel fraction, O2concentration and residence time for basic reburning is14%-17%,3%and0.8s. As temperature increasing, NO reduction efficiency increases first and then decreases. The maximum NO reduction efficiency of82.70%can be obtained at1323K. NO reduction efficiency can be significantly raised, while the reaction temperature window can be obviously broaden, when ammonia is injected into reburning zone. High O2concentration is not conducive to NO reduction by advanced reburning. The optimum residence time and [NH3]/[NO] molar ratio is0.6-0.8s and0.75. The maximum NO reduction efficiency of93.49%can be obtained at1323K when the reburning fuel fraction and [NHx]/[NO] molar ratio is14%and0.75. NO reduction efficiency of LM-WV under O2/N2atmosphere is higher than that under O2/CO2atmosphere at1123-1223K. This situation will change at higher temperature. NO reduction efficiency increases with CO2concentration increasing, and high concentration of CO2can promote the denitrification reaction.
The desulfurization and denitrification characteristics of LM-WV by pre-mixed with coal under O2/CO2atmosphere are investigated on the tube furnace reactor. Experimental result shows that the desulfurization and denitrification performance of LM-WV are much better than that of both original limestone and analytical grade calcium acetate. SO2and NO reduction efficiency may be affected by addition amount, sulfur content in coal and temperature. SO2and NO reduction efficiency of LM-WV under O2/CO2atmosphere are higher than that under O2/N2atmosphere under the same experimental conditions. LM-WV shows good desulfurization performance in the experimental temperature range1023-1473K, and it can maintain SO2reduction efficiency of more than80.06%at calcium/sulfur ratio being2. NO reduction efficiency increases with addition amount increasing. NO reduction efficiency of53.08%can be obtained at1373K when calcium/sulfur ratio is3. The performance of simultaneous desulfurization and denitrification of LM-WV by injected into flue gas under O2/CO2atmosphere are investigated in the drop-tube experiment system. The maximum SO2and NO reduction efficiency of75.83%and86.61%can be obtained respectively at1223K and1323K, when the calcium/sulfur ratio and residence time is about2and0.8s. In the above conditions, when ammonia is injected into reactive zone at [NH3]/[NO] molar ratio of0.75, the maximum SO2and NO reduction efficiency of73.16%and94.78%can be obtained respectively at1223K and1323K. Ignition temperature, weight loss peak temperature and burnout temperature of coal all migrate towards the direction of low temperature after LM-WV is added into coal. At the same time, activation energy of combustion reaction significantly decreases. The above phenomenon indicates that LM-WV can improve the combustion performance of pulverized coal under O2/CO2atmosphere.
Combine oxidative decomposition model of acetone with denitrification reaction model of AA, then refer to the related experimental results, and finally get acetone denitrification reaction model including112species and677elementary reactions. Mechanism analysis shows that OH can react with C2H6, C2H4, CH4and C2H2, then generate hydrocarbon ion groups and HCCO. Hydrocarbon ion groups and HCCO can react with NO and generate HCN. HCN can be converted into NCO and NH by reacting with O. NCO and NH can reduce NO to N2through NCO+NO(?)N2+CO2and NH+NO(?)N2+OH. Reactive groups of OH, O and H are important materials which can ensure the denitrification reaction to carry out smoothly. However, excessive reactive groups may exacerbate the oxidation reaction of HCN. The difference of NO reduction efficiency of LM-WV under O2/N2atmosphere and O2/CO2atmosphere at low temperature may be caused by lower concentration of reactive groups under O2/CO2atmosphere. The difference under these two atmospheres may be caused by higher concentration of hydrocarbon gases under O2/CO2atmosphere. High concentration of CO2can promote the generation of CH4, C2H4, C2H6and C2H2. In addition, CO2can also promote the conversion of CH4, C2H4, C2H6and C2H2to free radicals, such as CH3, C2H3and C2H5, through CH4(+M)<=>CH3+H(+M), C2H4+H(+M)(?) C2H5(+M),C2H6(+M)<=> CH3+CH3(+M),C2H2+H(+M)(?) C2H3(+M). These reactions are all conducive to the denitrification reaction.
SO2can promote the denitrification reaction of LM-WV. SO2can consume reactive groups of H, O, OH through SO2+H(+M)(?)HOSO(+M),HOSO+H(?)SO2+H2SO2+O(+M)(?)SO3(+M) and HOSO+OH<=> SO2+H2O, which can inhibit the oxidation of HCN. In addition, SO2can also transform into SH and SN. Through SH+NO(?) SN+OH and SN+NO(?) N2+SO, NO can be directly reduced to N2by SH and SN.
引文
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