脉冲电晕放电去除NO的反应途径研究

对脉冲放电等离子体条件下去除NO的宏观反应机理进行研究结果表明,不同氧含量的氮气流中NO的脱除均同时存在氧化、分解与还原三条途径。气流中氧含量不同,起主导的反应也不相同。还考察了NH₃气、H₂O蒸气等调质剂对反应途径的影响。NH₃的加入有利于NO通过还原途径脱除,但同时导致生成N2O反应的加剧,而产生二次污染,由此说明NH3加入位置的重要性。水蒸气在等离子体作用下产生氧化性物种,有利于NO的氧化脱除。本实验条件下加入气流量1％的水气即能使NO氧化脱除率增加20％左右。实验还考察了电参数（峰值电压、脉冲重复频率等）对NO脱除反应的影响。最后对本实验条件下的反应机理进行推断,所得结果对脉冲电晕等离子体烟气脱NO工艺研究具有一定的指导意义。     

Simultaneous oxidation of NO, SO2 and Hg0 from flue gas by pulsed corona discharge

A process capable of oxidizing NO, SO2 and Hg0 was proposed simultaneously, which utilized a high-voltage and short-duration positive pulsed corona discharge. By focusing on NO, SO2, and Hg0 oxidation efficiencies, the influences of pulse peak voltage, pulse frequency, initial concentration, electrode number, residence time and water vapor addition were investigated. The results indicate that NO, SO2 and Hg0 oxidation efficiencies depend primarily on the radicals (OH, HO2, O) and the active species (O3, H2O2), etc. produced by the pulsed corona discharge. The NO, SO2 and Hg0 oxidation efficiencies improved as increasing pulse peak voltage, pulse frequency, electrode number and residence time, while they are reduced with an increasing initial concentration. By adding water vapor, SO2 oxidation efficiency is improved remarkably, while NO oxidation efficiency is decreased slightly. In our experiments, the simultaneous NO, SO2, and Hg0 oxidation efficiencies reached to 40%, 98% and 55% with the initial concentrations 479 mg/m3, 1040 mg/m3, and 15.0 ug/m3, respectively.     

窄脉冲电晕等离子体烟气脱硫产物收集研究

对窄脉总电晕等离子体烟气脱硫过程中的产物收集进行了研究与探讨，结果表明正脉冲流注电晕放电烟气脱硫过程中产生的电粉尘以及电晕极肥大等问题，对脱硫产物的收集有很大影响。     

Characteristics of NO reduction with non-thermal plasma

As a new type of NO removal system, NO reduction in N2-NO plasma was applied to solve the difficulties in the traditional methods, such as higher energy-consumption, larger equipment size and high cost, and so on. Using the experimental NO reduction system with single-pair electrode tip discharge structure, the NO reduction characteristics of N~-NO system were revealed to guide the engineering practice; the results of NO reduction with single-pair electrode tip discharge plasma also have the same instructive meaning to the NO reduction with multi-pair electrode tip discharge plasma. The amount of both active N atom and NO removal rate increased with the distance /g increasing between the two electrode tips and then dropped when the distance exceeded a certain value. The NO removal rate increased while the voltage between two electrode tips or the resident time of gas flow increased. The distance is a key geometrical variable factor that can determine the intensity of electric field between two electrode tips and the resident time of gas. In this paper, the effects of the dielectric features on NO reduction using dielectric-barrier discharge plasma system were also studied. The results of NO removal rate with different dielectrics such as Al2O3, CaO. MgO and glass showed that the electric field intensity is different with different dielectric, because it brings different energy to particles in discharge room and thus it causes different NO removal rate.     

低温等离子体分解脱除NO影响因素研究

为优化低温等离子体反应器设计、提高NO分解率,在低放电电压下通过改变介质阻挡放电参数(放电电压、介质材料、放电间隙等)考察其对分解NO的影响.研究结果表明:在低电压范围条件下(≤6.5 kV),放电电压对提高NO分解率的效果是非线性的,其影响随电压的升高而减弱;选择介电常数较大的介质材料更易获得较高的分解率;当反应器其它特征参数确定后,放电间隙并非越小越好,而是存在一个最佳值;实际应用中,应选用二次电子发射系数较大的电极材料;NTP反应器中加入填充材料不仅具有吸附和存储性能,还具有介质阻挡放电的功能,选择适合的填充材料能更大程度地提高能量利用率,提高NO分解率.     

介质阻挡放电去除NO的实验研究

设计了一套高压电源和同轴圆柱 -筒介质阻挡放电反应器装置 ,进行了冷等离子体去除NO的实验研究 ,结果表明该方法是有效的 .研究了气体流量、NO初始浓度、放电电压、O2 含量以及中心电极尺寸对NO去除效率的影响 .当流量较小或NO初始浓度较低时 ,有较高的去除率 ;流量变大和NO初始浓度增加时 ,NO的去除率将下降 .放电电压升高 ,NO去除率将增大 .O2 的存在会降低NO的去除率 .放电管其它特征尺寸给定条件下 ,中心电极存在一个最佳直径 ,使得NO的去除效果最为理想 .     

脉冲放电烟气脱除尘与除SO_2和NO_X的研究

对脉冲放电烟气除尘与脱除ＳＯ２和ＮＯＸ进行实验研究与分析的结果表明，烟气中的飞灰对ＳＯ２和ＮＯＸ吸附脱除２％～５％，吸附脱除量随着飞灰浓度和烟气含量的增加而增大。在单位体积烟气注入能量为４Ｗｈ／Ｎｍ３和烟气在反应器中停留时间小于３秒，飞灰与水蒸气的协同作用使ＳＯ２和ＮＯＸ脱除率分别达到２３％和３３％。同时，脉冲放电使反应器对飞灰具有良好的协同作用，收集效率为９７％。     

Review on the NO removal from flue gas by oxidation methods

Due to the increasingly strict emission standards of NOx on various industries, many traditional flue gas treatment methods have been gradually improved. Except for selective catalytic reduction (SCR) and selective non-catalytic reduction (SNCR) methods to remove NOx from flue gas, theoxidation method is paying more attention to NOx removal now because of the potential to simultaneously remove multiple pollutants from flue gas. This paper summarizes the efficiency, reaction conditions, effect factors, and reaction mechanism of NO oxidation from the aspects of liquid-phase oxidation, gas-phase oxidation, plasma technology, and catalytic oxidation. The effects of free radicals and active components of catalysts on NO oxidation and the combination of various oxidation methods are discussed in detail. The advantages and disadvantages of different oxidation methods are summarized, and the suggestions for future research on NO oxidation are put forward at the end. The review on the NO removal by oxidation methods can provide new ideas for future studies on the NO removal from flue gas.     

燃煤流化床钙基脱硫剂对NO转变率的影响及机理

在φ150mm×1000mm流化床试验台上,温度区间840℃～960℃,研究了钙基脱硫剂品种、粒径和Ca/S比对NO转变率的影响.阐述了钙基脱硫剂使NO转变率增加机理试验发现,同等质量钙基脱硫剂使NO增加的次序为氧化钙、石灰石、方解石;Ca/S比越大,NO转变率越高;粒径为1～2mm时NO转变率最大,2～3mm时次之,0.2～1mm时最小.加入脱硫剂降低了HCl、HF、SO₂的浓度,导致O、H、HO₂浓度升高,CO的氧化反应加速,在床料、燃料灰催化作用下CO与NO的反应减慢,最终导致NO浓度升高.     

Benzene conversion by manganese dioxide assisted silent discharge plasma

Non-thermal plasma technologies have shown their promising potential specially for the low concentration of volatile organic compound control in indoor air in recent years. But it is also high energy consuming. So, to improve the energy efficiency, adding catalysts which enhance the plasma chemical reactions to plasma reactors may be a good selection. Therefore, in this study the manganese dioxide assisted silent discharge plasma was developed for benzene conversion at a relatively high energy efficiency. The results show that MnO₂ could promote complete oxidation of benzene with O₂ and O₃ produced in the plasma discharge zone. The energy efficiency of benzene conversion with MnO₂ was two folds as much as that without catalysts. It was also found that the site of MnO₂ in the reactor and the energy density had effects on benzene conversion. While the energy density was lower than 48 J/L, benzene conversion decreased with the increase in the distance between MnO₂ bed and the plasma discharge zone. Whereas when the energy density was higher than 104 J/L, benzene conversion had an optimal value that was governed by the distance between MnO₂ bed and the plasma discharge zone. The mechanism of benzene oxidation in plasma discharges and over MnO₂ is discussed in detail. __________ Translated from China Environmental Science, 2006, 26(6): 703–707 [译自: 中国环境科学]     

N-TiO2/PSF中空纤维复合膜光催化烟气脱硝研究

采用溶胶-凝胶法以聚砜(PSF)中空纤维膜为载体制备了N-Ti O2/PSF中空纤维复合膜催化剂,考察其光催化烟气脱硝性能.紫外光催化的NO去除效率可达63%,去除负荷可达213.6 g·m-3·h-1.采用紫外-可见光谱(UV-Vis)、X-射线光电子能谱(XPS)和傅里叶变换红外光谱(FTIR)表征了N-Ti O2/PSF中空纤维复合膜催化剂.UV-Vis光谱分析表明,掺杂N改性的Ti O2复合膜光催化层在紫外和可见光波段的吸收性能都有极大的改善.XPS证明了O—Ti—N键能的存在.N-Ti O2/PSF中空纤维膜光催化处理NO的作用机制为NO气体通过中空纤维膜传质到NTi O2催化膜,光催化产生羟基自由基和超氧负离子,NO气体被羟基自由基和超氧负离子氧化成易处理的NO2和HNO3.     

典型酸碱条件下NO2-对剩余污泥水解产酸的影响

控制温度35℃,在典型pH值条件下(酸性5.0,碱性9.0)对比研究了NO2-对剩余污泥水解酸化性能的影响.结果表明:投加亚硝酸盐促进了剩余污泥的水解,提高了总可溶性COD(SCOD)产量,且随着时间的进行,酸性时比碱性时水解程度更高,到第28d时,总SCOD浓度由高到低依次为B1(pH=5且加NO2-),B2(pH=9且加NO2-),B4(pH=9且未加NO2-),B3(pH=5且未加NO2-);B1,B2,B3和B4中总挥发性脂肪酸(TVFAs)最高浓度分别为4476,4303,1350和2921mg/L,表明亚硝酸盐同样增强了污泥的酸化程度,并且酸性条件时促进作用更大.除此之外,酸性且投加NO2-的条件可以有效减少氨氮的释放.     

以MnOx/TiO2作为催化剂的低温SCR反应过程中还原剂NH3的作用

研究了在以MnOx/TiO2作为催化剂的低温SCR反应过程中,还原剂NH3所起的作用.当系统中NH3浓度较低时,增加气相中NH3的浓度可以大幅度提高NO的去除率.但当系统中NH3浓度较高时,NO去除率基本不随NH3浓度变化而变化.并且瞬态研究中,NH3对NO去除率的影响较为复杂.为了探明NH3在SCR反应中的作用,用原位傅立叶红外检测了各个反应历程中NH3在催化剂表面形成的基团变化及其活性特征.结果表明,在SCR反应过程中,在催化剂表面形成的配位态的NH3是参与反应的主要物质.并且在催化剂表面,此种NH3会与NO生成的硝酸盐形成竞争吸附,当催化剂活性点首先被硝酸盐占领时,将会影响配位态NH3的生成,从而在一定程度上降低了NO的转化率.     

脉冲电晕放电协同烟气脱硫脱硝试验研究

脉冲电晕放电对PM2.5具有一定的凝并作用,与直流静电除尘器相结合可以提高燃煤电厂烟气中粉尘的脱除效率.基于脉冲电晕放电还可以将烟气中的NO、SO2氧化成NO2、SO3等易吸收的物质成分,与传统的液相吸收洗涤技术相结合可提高NO、SO2的脱除效率.文中进行了脉冲电晕放电协同烟气脱硫脱硝的试验研究,研究了影响NO、SO2转化效率的主要因素.实验结果表明,提高脉冲峰值电压、脉冲频率、脉冲放电电极数目.延长停留时间.降低气体初始浓度有助于提高NO、SO2的转化效率;增加空气湿度可以显著提高SO2的转化效率.在本试验中,当NO、SO2初始浓度为150×10-6左右时,其相应的转化效率可以分别达到70%、90%.     

Cu-ZSM-5对燃气烟气中NO的吸附特性

由于燃气烟气中水含量高,从预处理条件、H₂O含量和O₂含量方面考察Cu-ZSM-5分子筛吸附NO的影响.实验结果表明：在5%O₂,无水条件下,Cu-ZSM-5（Si/Al=25）吸附效果最好,穿透吸附量为0.8371mmol/g;通过FT-IR验证NTP预处理能够有效去除Cu-ZSM-5分子筛中H₂O,并保留-OH吸附位;H₂O的存在能够明显抑制Cu-ZSM-5的吸附能力,在烟气含8%H₂O的条件下,Cu-ZSM-5穿透吸附量下降至0.09566mmol/g,相比之下,混合吸附剂CMS/La-Cu-ZSM-5=1/9穿透吸附量可达0.1889mmol/g;O₂的存在可以有效促进NO吸附,但在10% O₂时出现了氧抑制现象;通过TPD和FT-IR分析,Cu-ZSM-5吸附物种以NO₂,NO,-NO₃为主,而在8% H₂O条件下,-NO₃含量较少.     

半焦负载钙和铁催化还原NO的研究

用浸渍法制备负载Ca和Fe的褐煤半焦,采用程序升温和恒温法在石英固定床反应器上于常压反应条件下研究了NO-半焦催化还原反应.研究发现,Ca和Fe对半焦还原NO的反应具有催化作用,其中Fe的催化作用强于Ca;热处理温度升高,Ca的催化作用降低,但热处理温度的变化基本不影响Fe的催化活性;CO和O₂气氛可以促进NO的还原,温度升高CO和O₂的促进作用减小.     

基于卫星数据研究兰州市NO2时空分布特征以及冬季NOx排放通量

搭载在EOS AURA卫星上的OMI探测器由于其较高时空分辨率在大气痕量气体(O3,NO2,SO2)探测中得到广泛应用.利用2010~2012年OMI NO2柱浓度数据产品重构了兰州市以及周边地区NO2柱浓度分布,分析了其时空变化特征,并利用西南风场下NO2空间分布特征采用拟合方法研究了NOx冬季排放通量以及寿命.研究表明,NO2柱浓度空间分布呈现以兰州市为中心,浓度向四周扩散的特征;兰州市NO2柱浓度的年变化特征为12月达到最大浓度,8月达到最小浓度;2010~2012年NO2寿命分别为10.6,9.9,9.1h,NOx冬季排放通量分别为175.3, 183.7,179.9mol/s.其排放通量与兰州环境公报提供的氮氧化物排放通量数量级之间具有较好的一致性,说明利用卫星数据估算兰州的NOx通量方法的有效性.     

Seasonal variability of ambient NH3, NO, NO2 and SO2 over Delhi

We present the diurnal and seasonal variability of ambient NH3, NO, NO2 and SO2 over Delhi, India. Ambient NH3, NO and NO2 were measured continuously during winter, summer and autumn seasons using NH3- and NOx-analyzer, which operates by chemiluminescence method with a higher estimation e ciency (> 90%) than the chemical trap method (reproducibility 4.7%). Prominent diurnal, day-to-day and seasonal variations of ambient mixing ratio of NH3, NO, NO2 and SO2 were observed during the study period. Seasonal variation with higher mixing ratio in winter was observed for all measured trace gases except NO. Day-night variation of all measured trace gases observed was higher in winter in comparison with summer. Late morning increase in NO2 mixing ratio might be attributed to conversion of NO to NO2 with the interaction of O3.     

Simultaneous removal of NO and SO2 from dry gas stream using non-thermal plasma

In order to investigate the feasibility of sequential removal NO and SO_2 using non-thermal plasma and adsorbent simultaneously,the removal of NO and SO_2 from dry gas stream(NO/SO_2/N_2/O_2)with very little O_2 using non-thermal plasma was investigated using a coaxial dielectric barrier discharge.Comparative experiments were carried out in the dry gas stream with and without Ar respectively at O_2 concentration of 0.1%.The results showed that NO could be removed remarkably and it would be enhanced in the presence of Ar in the dry gas stream.It seems that SO_2 could not be removed unless there is Ar in the dry gas stream.The mechanism of removal of NO and SO_2 in the dry gas stream was discussed.     

高压脉冲等离子体催化还原NO的研究

用离子交换法制备Co-ZSM-5催化剂,考察了有氧条件下,在甲烷选择还原NO的反应中,高压脉冲等离子体的加入对Co-ZSM-5活性的影响。发现在一定温度范围内,高压脉冲等离子体与Co-ZSM-5之间存在协同效应。在此基础上,初步探讨了高压脉冲等离子体活化CH4催化还原净化NO的反应机理。