基于尿素还原剂的选择性非催化还原高效脱硝技术的实验研究
摘要
随着我国经济的高速发展,能源的消耗也越来越大,由此而带来的环境问题也日益严重,大气中氮氧化物的迅速增加抵消了二氧化硫减排的效果,酸雨的问题依然严重,而我国氮氧化物主要来自燃煤电站,本文对燃煤电站常用的一种烟气脱硝技术SNCR进行了深入的研究。SNCR及更进一步的SNCR/SCR联合脱硝技术,其投资、工程改造量、运行成本相对单独的SCR系统要低,脱硝率适中,可以满足我国目前的NOx排放要求。
首先,本文通过实验对常用的绿色还原剂—尿素,对尿素的热解、水解及制取氨气过程进行了实验研究。实验发现：对于尿素晶体的热解,当温度高于250℃后尿素已完全分解,残留物中主要是三聚氰酸等大分子聚合物,当温度高于500℃后残留物分解完毕,尿素热解的最终产物主要是NH3和HNCO。在存在着O2的氛围下,当温度升高到850℃后,由于氧化还原反应的进行,NH3与HNCO的浓度开始急剧下降,同时伴随少量的NO与N2O的生成。HNCO在均相下非常稳定,但是在金属氧化物的催化作用下在较低的温度就能迅速与水汽进行反应生成NH3。在所考察的多种金属氧化物中,纳米γ-Al2O3由于较高的催化活性和抗磨损性,更适宜作为尿素热解制取氨气的催化剂。
然后,在试验台上对Thermal DeNOx和NOxOUT过程进行了研究并与CHEMKIN模拟结果进行对比,此外对NOxOUT过程还考察了不同添加剂的影响。实验表明：相同条件下氨水的最佳脱硝温度稍低于尿素,而氨水的最佳脱硝率略高于尿素,氨水的温度窗口要大于尿素。SNCR过程中将会生成N20,对于尿素还原剂,约有15%的NO转化成N20,高于氨水的3%。脱硝曲线随着水汽含量的增加往高温侧偏移,相反地氧量的增加则使得脱硝曲线往低温侧偏移。氧化性溶剂的添加使得NOxOUT过程在较低的温度下就能进行,但是最佳脱硝率均不同程度的下降,与氧化性溶剂相比,只需添加少量的钠盐就能起到非常好的促进效果。钠盐在高温下同样稍微降低了脱硝率,与氧化性溶剂不同的是钠盐添加能促进HNCO的水解,减少HNCO浓度而增加NH3浓度,此外钠盐本身不参与SNCR反应,其在溶液中通过循环反应生成OH活性根来促进低温下SNCR反应的进行。
接着在雾化试验台上开发适合SNCR工业应用的墙式喷枪和多孔长喷枪。通过对两通道实心圆柱形气力雾化喷嘴及Y型气力雾化喷嘴的雾化情况进行了研究,包括喷嘴出口结构尺寸、混合室尺寸、液流量、气耗率等对喷嘴雾化性能的影响。对于气力雾化喷嘴,气耗率是影响雾化粒径大小的主要因素。
最后在一台410t/h燃煤电站锅炉上对SNCR/SCR联合脱硝技术的工业应用情况展开了详细的研究。实验发现,对于单独的SNCR系统,在NSR为1.5的情况下能获得40%以上的脱硝率,同时NH3逃逸浓度在10μl/L以内。喷射层温度、喷射流量、喷射液滴的粒径均影响着脱硝率,尿素液滴分布在合适的温度区间是提高脱硝率最好的方法。通过增设补氨喷射层及高速气流扰动可实现SCR反应器入口NH3分布均匀,在NSR为1.86的情况下SNCR/SCR联合脱硝系统能获得85%以上的脱硝率。NH3逃逸一方面会导致飞灰中含氨量增加,另一方面会和烟气中的SO3、HCl反应生成铵盐,会对下游设备产生影响。此外应避免尿素溶液在高温下对炉内换热器的冲刷,减少对换热元件的腐蚀。
The energy consumption of china is increasing with rapid economic development which brought in serious environment problems. The reduction of sulfur dioxide emission will be offset by the rapid increase of nitrogen oxides (NOx) in the atmosphere. Acid rain still remains a serious problem. Considering most of the NOx emission comes from the coal-fired power boiler, SNCR (Selective Non-catalytic Reduction) as one of the common used flue gas denitrification technology was studied in this paper. SNCR and hybrid SNCR/SCR (Selective Catalytic Reduction) could get middle denitrification with low investment, easy retrofit, low operation cost compared with SCR system. SNCR or Hybrid SNCR/SCR could meet the NOx emission standard.
First, this paper studied the decomposition and hydrolysis of urea which was commonly used as green reductant. When the temperature was higher than250℃. the main composition of residue were cyanuric acid and other macromolecular polymers, no urea was found in the residue. The decomposition would finish when the temperature was over500℃. The final products form urea decomposition was NH3and HNCO. Due to the oxidation, the yield of NH3and HNCO would decline sharply when the temperature rose to850℃with O2existence. A small amount of NO and N2O was also generated. HNCO was quite stable in the homogeneous condition but easily hydrolyzed over metal oxide to yield NH3even at low temperature. γ-Al2O3was most suitable as catalytic material due to its high catalytic activity, as well as good abrasion resistance and stability.
Then, the study of Thermal DeNOx and NOxOUT process was done through experiments combined with CHEMKIN simulation. The impact of different additive on the NOxOUT process was also examined. The results showed that the Thermal DeNOx would get higher denitrification, lower favorable temperature, wider emperature window than NOxOUT on the same condition. N2O would be generated during SNCR process. About15%of NO was converted to N2O during NOxOUT process which was only3%during Thermal DeNOx process. The increase in water vapor content would make the denitrification curve offset to the high temperature side, while the oxygen had the opposite effect. The SNCR process could be carried out at lower temperature due to the addition of oxygenated liquid additives, but the best denitrification decreased. Compared with oxygenated liquid additives, a small amount of sodium salts would get very good effect. The addition of sodium salts could catalyze the HNCO hydrolysis to yield NH3. In addition the sodium salts didn't participate in the SNCR reaction but generated OH radicals to promote the SNCR reaction at low temperature.
Then the SNCR wall spray and porous nozzle were tested on the atomization test-bed. The two channel solid cone atomization spray and Y type atomization spray were researched including the effect of mixing chamber size, flow rate, air consumption on the atomization performance. The air consumption rate had great effect on the size of droplet size.
Finally, particular experimental research on hybrid SNCR/SCR applied in a410t/h power plant boiler was carried out. It was found that more than40%of NOx was eliminated and the NH3slip was below10μl/L for the SNCR system while the NSR was1.5. The denitrification was effected by the temperature of the injection layer, spray flow and particle size of spray droplets. The best way to improve the denitrification was to make the urea droplet to distribute at the right temperature. The addition of complement of urea solution injection layer and high speed air turbulence could make the NH3even distribution before the SCR catalysts. The hybrid SNCR/SCR could get85%denitrification while the NSR was1.86. NH3slip increased the ammonia content in the fly ash and would react with SO3/HCl to form ammonium salts. The ammonium salt would have bad impact on the downstream equipment. In addition the urea solution should be avoided to scour the heat exchangers which might led to the corrosion.
首先,本文通过实验对常用的绿色还原剂—尿素,对尿素的热解、水解及制取氨气过程进行了实验研究。实验发现：对于尿素晶体的热解,当温度高于250℃后尿素已完全分解,残留物中主要是三聚氰酸等大分子聚合物,当温度高于500℃后残留物分解完毕,尿素热解的最终产物主要是NH3和HNCO。在存在着O2的氛围下,当温度升高到850℃后,由于氧化还原反应的进行,NH3与HNCO的浓度开始急剧下降,同时伴随少量的NO与N2O的生成。HNCO在均相下非常稳定,但是在金属氧化物的催化作用下在较低的温度就能迅速与水汽进行反应生成NH3。在所考察的多种金属氧化物中,纳米γ-Al2O3由于较高的催化活性和抗磨损性,更适宜作为尿素热解制取氨气的催化剂。
然后,在试验台上对Thermal DeNOx和NOxOUT过程进行了研究并与CHEMKIN模拟结果进行对比,此外对NOxOUT过程还考察了不同添加剂的影响。实验表明：相同条件下氨水的最佳脱硝温度稍低于尿素,而氨水的最佳脱硝率略高于尿素,氨水的温度窗口要大于尿素。SNCR过程中将会生成N20,对于尿素还原剂,约有15%的NO转化成N20,高于氨水的3%。脱硝曲线随着水汽含量的增加往高温侧偏移,相反地氧量的增加则使得脱硝曲线往低温侧偏移。氧化性溶剂的添加使得NOxOUT过程在较低的温度下就能进行,但是最佳脱硝率均不同程度的下降,与氧化性溶剂相比,只需添加少量的钠盐就能起到非常好的促进效果。钠盐在高温下同样稍微降低了脱硝率,与氧化性溶剂不同的是钠盐添加能促进HNCO的水解,减少HNCO浓度而增加NH3浓度,此外钠盐本身不参与SNCR反应,其在溶液中通过循环反应生成OH活性根来促进低温下SNCR反应的进行。
接着在雾化试验台上开发适合SNCR工业应用的墙式喷枪和多孔长喷枪。通过对两通道实心圆柱形气力雾化喷嘴及Y型气力雾化喷嘴的雾化情况进行了研究,包括喷嘴出口结构尺寸、混合室尺寸、液流量、气耗率等对喷嘴雾化性能的影响。对于气力雾化喷嘴,气耗率是影响雾化粒径大小的主要因素。
最后在一台410t/h燃煤电站锅炉上对SNCR/SCR联合脱硝技术的工业应用情况展开了详细的研究。实验发现,对于单独的SNCR系统,在NSR为1.5的情况下能获得40%以上的脱硝率,同时NH3逃逸浓度在10μl/L以内。喷射层温度、喷射流量、喷射液滴的粒径均影响着脱硝率,尿素液滴分布在合适的温度区间是提高脱硝率最好的方法。通过增设补氨喷射层及高速气流扰动可实现SCR反应器入口NH3分布均匀,在NSR为1.86的情况下SNCR/SCR联合脱硝系统能获得85%以上的脱硝率。NH3逃逸一方面会导致飞灰中含氨量增加,另一方面会和烟气中的SO3、HCl反应生成铵盐,会对下游设备产生影响。此外应避免尿素溶液在高温下对炉内换热器的冲刷,减少对换热元件的腐蚀。
The energy consumption of china is increasing with rapid economic development which brought in serious environment problems. The reduction of sulfur dioxide emission will be offset by the rapid increase of nitrogen oxides (NOx) in the atmosphere. Acid rain still remains a serious problem. Considering most of the NOx emission comes from the coal-fired power boiler, SNCR (Selective Non-catalytic Reduction) as one of the common used flue gas denitrification technology was studied in this paper. SNCR and hybrid SNCR/SCR (Selective Catalytic Reduction) could get middle denitrification with low investment, easy retrofit, low operation cost compared with SCR system. SNCR or Hybrid SNCR/SCR could meet the NOx emission standard.
First, this paper studied the decomposition and hydrolysis of urea which was commonly used as green reductant. When the temperature was higher than250℃. the main composition of residue were cyanuric acid and other macromolecular polymers, no urea was found in the residue. The decomposition would finish when the temperature was over500℃. The final products form urea decomposition was NH3and HNCO. Due to the oxidation, the yield of NH3and HNCO would decline sharply when the temperature rose to850℃with O2existence. A small amount of NO and N2O was also generated. HNCO was quite stable in the homogeneous condition but easily hydrolyzed over metal oxide to yield NH3even at low temperature. γ-Al2O3was most suitable as catalytic material due to its high catalytic activity, as well as good abrasion resistance and stability.
Then, the study of Thermal DeNOx and NOxOUT process was done through experiments combined with CHEMKIN simulation. The impact of different additive on the NOxOUT process was also examined. The results showed that the Thermal DeNOx would get higher denitrification, lower favorable temperature, wider emperature window than NOxOUT on the same condition. N2O would be generated during SNCR process. About15%of NO was converted to N2O during NOxOUT process which was only3%during Thermal DeNOx process. The increase in water vapor content would make the denitrification curve offset to the high temperature side, while the oxygen had the opposite effect. The SNCR process could be carried out at lower temperature due to the addition of oxygenated liquid additives, but the best denitrification decreased. Compared with oxygenated liquid additives, a small amount of sodium salts would get very good effect. The addition of sodium salts could catalyze the HNCO hydrolysis to yield NH3. In addition the sodium salts didn't participate in the SNCR reaction but generated OH radicals to promote the SNCR reaction at low temperature.
Then the SNCR wall spray and porous nozzle were tested on the atomization test-bed. The two channel solid cone atomization spray and Y type atomization spray were researched including the effect of mixing chamber size, flow rate, air consumption on the atomization performance. The air consumption rate had great effect on the size of droplet size.
Finally, particular experimental research on hybrid SNCR/SCR applied in a410t/h power plant boiler was carried out. It was found that more than40%of NOx was eliminated and the NH3slip was below10μl/L for the SNCR system while the NSR was1.5. The denitrification was effected by the temperature of the injection layer, spray flow and particle size of spray droplets. The best way to improve the denitrification was to make the urea droplet to distribute at the right temperature. The addition of complement of urea solution injection layer and high speed air turbulence could make the NH3even distribution before the SCR catalysts. The hybrid SNCR/SCR could get85%denitrification while the NSR was1.86. NH3slip increased the ammonia content in the fly ash and would react with SO3/HCl to form ammonium salts. The ammonium salt would have bad impact on the downstream equipment. In addition the urea solution should be avoided to scour the heat exchangers which might led to the corrosion.
引文
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