低温等离子体用于柴油机尾气脱硝的实验

doi:10.16085/j.issn.1000-6613.042

摘要/Abstract

摘要：

柴油机作为卡车、重型机械以及船舶的主动力装置仍被广泛采用，其尾气中氮氧化物的脱除技术也是目前的研究热点。本文搭建了模拟柴油机尾气的配气系统，采用介质阻挡放电产生低温等离子体（non-thermal plasma，NTP）的方法对模拟柴油机尾气进行了脱硝的实验研究。实验结果表明：针对本系统，电源效率和能量密度随着输入电压的增大而升高，当输入电压高于60V时，电源效率在90%以上；在O₂/N₂条件下，随着O₂浓度以及能量密度的增加，NO生成量逐渐增加，NO₂生成量先增加后降低最终趋于稳定；在NO/N₂条件下，低温等离子体对NO的脱除率接近100%；在NO/O₂/N₂条件下，随着NO浓度的增加，临界O₂浓度升高，O₂体积分数为1%时脱硝效率在90%以上，O₂体积分数高于14%时低温等离子体的脱硝率为负值，且随着能量密度的增加，生成的NO _x 浓度也更高，O₂浓度对低温等离子体的脱硝性能起决定性作用；在低能量密度时，加入NH₃会提高脱硝性能，高能量密度时NH₃会略微降低NTP的脱硝性能，当加入H₂O模拟真实柴油机尾气成分且喷氨时，获得的脱硝率最高为40.6%。

关键词: 柴油机尾气, 氮氧化物, 介质阻挡放电, 低温等离子体, 脱硝率

Abstract:

Diesel engines are still widely used as main power equipment for trucks, heavy machinery and ships. The technologies of nitrogen oxides removal from diesel exhaust are hot research topics. This paper sets up a gas supply system that simulates the diesel exhaust, and uses a dielectric barrier discharger (DBD) to generate non-thermal plasma (NTP) to investigate the removal of nitrogen oxides. The experimental results showed that the power efficiency and energy density increase with the input voltage for this system. The power efficiency is above 90% when the input voltage is higher than 60V. In the O₂/N₂ system, NO generation increases with the O₂ concentration and energy density, while NO₂ increases first, then decreases and stabilizes. The removal rate of NO is close to 100% by NTP in NO/N₂ system. For the NO/O₂/N₂ system, the critical O₂ concentration increases with NO concentration. With the increase of energy density, the denitrification efficiency is above 90% at 1% O₂ volume fraction and negative when O₂ volume fraction is higher than 14%. The O₂ concentration plays a decisive role in the denitration performance of the NTP. NH₃ improves the denitration rate at low energy density while slightly reduces the denitration rate at high energy density. The denitration rate is 40.6% at simulating real diesel exhaust conditions when H₂O and ammonia is added.

Key words: diesel exhaust, nitrogen oxides, dielectric barrier discharger, non-thermal plasma, denitration rate

中图分类号:

X511

汪宗御,邝海浪,张继锋,褚李林,纪玉龙. 低温等离子体用于柴油机尾气脱硝的实验[J]. 化工进展, 2019, 38(10): 4755-4766.

Zongyu WANG,Hailang KUANG,Jifeng ZHANG,Lilin CHU,Yulong JI. Experimental of diesel engine denitration by non-thermal plasma[J]. Chemical Industry and Engineering Progress, 2019, 38(10): 4755-4766.

图/表 15

图1 DBD脱硝实验系统

图2 DBD反应器结构及参数

图3 电源初始输出的正弦波（局部）

图4 电源输出的脉冲信号（2个周期）

图5 电压-电荷法求放电功率等效电路

图6 李萨如积分面积图

图7 1000μL·L-1 NO+1000μL·L-1 NH3+14%O2时电源能量密度和效率随输入电压的变化

图8 不同NO浓度时电源输出效率随输入电压的变化

图9 O2+N2条件下不同能量密度时NTP产生的影响 ·N +O2 → NO+·O (14)

图10 不同能量密度时NTP的脱硝性能（NO/N2）

图11 不同NO和O2条件下NTP的脱硝性能

图12 不同O2和NH3条件下，NTP的脱硝性能

图13 H2O对氮氧化物浓度的影响

图14 H2O和NH3对脱硝率的影响 e+H2O → e+·H+·OH (37)O(1D)+ H2O → ·OH+·OH (38)

图15 NO x 在NTP反应体系中的转化途径

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