Desulfurization and denitrification of the marine diesel exhaust by non-thermal plasma method with the addition of monoethanolamine
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摘要: 采用自行设计的介质阻挡耦合电晕放电等离子体反应装置进行了模拟船舶尾气同时脱硫脱硝的研究。分别考察了尾气中各气体组分及乙醇胺用量、放电电流和气体流量等因素对NOx 和SO2脱除的影响，探究了放电脱除NOx 的机理。结果表明，在模拟船舶尾气（N2/O2/SO2/NOx /CO2/H2O）中，保持放电电流为1.67 A和气体总流量为650 mL/min，添加0.48%乙醇胺后可以有效减弱O2和H2O对等离子体放电脱除NOx 的抑制作用，同时乙醇胺会吸收进入体系中的部分CO2，减弱CO2对NOx 脱除的抑制，最终脱硝率达94%。添加乙醇胺后，由于其可高效吸收SO2，且不受尾气中O2、CO2和H2O等组分的影响，SO2脱除率可达97%。Abstract: Simultaneous desulfurization and denitrification of marine diesel exhaust was carried out by coupling the dielectric barrier discharge (DBD) with corona discharge pulse (CDP) to generate non-thermal plasma (NTP). The effect of various gas components in the exhaust gas and the amount of monoethanolamine, discharge current, gas flow rate and other factors on the desulfurization and denitrification were then investigated and the mechanism of denitrification by NTP was discussed. The results show that when the total gas flow rate is 650 mL/min, applying 1.67 A current discharge and adding 0.48% monoethanolamine to the simulated marine diesel exhaust (N2/O2/SO2/NOx/CO2/H2O) can weaken the negative effects of oxygen and water vapor on the denitrification. Besides, monoethanolamine can also weaken the negative effects of carbon dioxide by absorbing carbon dioxide from the exhaust and the final denitrification rate reaches 94%. Meanwhile, a high desulfurization rate (97%) is also achieved, as monoethanolamine can absorb sulfur dioxide rapidly, which is almost unaffected by any exhaust gas components.
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图 1 实验流程示意图
Figure 1 Schematic diagram of the experimental setup
1：N2 gas cylinders；2：O2 gas cylinders；3：NO gas cylinders；4：SO2 gas cylinders；5：CO2 gas cylinders；6：mass flow controllers；7：check valves；8：buffer；9：water vapor generator；10：additives mixer；11：reactor；12：dehumidifier；13：check valve；14：high voltage power supply；15：gas analyzer；16：mass spectrometry
图 2 不同气氛下NOx体积分数随放电时间的变化
Figure 2 NOx removal efficiency under different gas compositions
a: N2+900 μL/L NOx+450 μL/L SO2+15% O2; b: N2+900 μL/L NOx+450 μL/L SO2+15% O2+5% CO2+5% H2O; c: N2+900 μL/L NOx+450 μL/L SO2+5% H2O; d: N2+900 μL/L NOx+450 μL/L SO2+5% CO2; e: N2+900 μL/L NOx+450 μL/L SO2
图 3 不同气氛下SO2体积分数随放电时间的变化
Figure 3 SO2 removal efficiency under different gas compositions
a: N2+900 μL/L NOx+450 μL/L SO2+15% O2; b: N2+900 μL/L NOx+450 μL/L SO2; c: N2+900 μL/L NOx+450 μL/L SO2+5% CO2; d: N2+900 μL/L NOx+450 μL/L SO2+15% O2+5% CO2+5% H2O; e: N2+900 μL/L NOx+450 μL/L SO2 +5% H2O
图 4 脱除率随乙醇胺加热温度的变化
Figure 4 Variation of the NOx /SO2 removal efficiency with the MEA heating temperature
图 5 脱除率随乙醇胺添加量的变化
Figure 5 Variation of the NOx /SO2 removal efficiency with the amount of MEA
图 6 脱除率随电流的变化
Figure 6 Variation of the NOx /SO2 removal efficiency with the applied current
图 8 放电后产物的红外光谱谱图
Figure 8 Infrared spectrum of the reaction products from the plasma reactor
图 9 脱除率随氧气含量的变化
Figure 9 Variation of the NOx /SO2 removal efficiency with the oxygen concentration
(N2 as the carrier gas; initial NOx concentrations is 900 μL/L, initial SO2 concentration is 450 μL/L, the total gas flow is 650 mL/min, and the discharge current is 1.67 A)
图 10 CO2体积分数随吸收时间的变化
Figure 10 CO2 concentration vs. absorb time with different initial CO2 concentrations
a: 12%CO2; b: 9%CO2; c: 6%CO2; d: 3%CO2;
图 11 不同CO2含量下脱除率随时间的变化
Figure 11 Variation of the NOx /SO2 removal efficiency with the CO2 concentration (parameters as mentioned above)
图 12 脱除率随H2O含量的变化
Figure 12 Variation of the NOx /SO2 removal efficiency with the H2O concentration (parameters as mentioned above)
表 1 典型柴油机尾气与电厂烟气组分对比
Table 1 Comparison of typical diesel engine exhaust and power plant flue gas
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