不同Mn/Fe摩尔比对Mn-Fe复合催化剂催化氧化NO的影响

采用溶胶凝胶法制备了四种不同比例的Mn-Fe催化剂。研究了四种催化剂在100℃~400℃温度范围内的NO催化氧化活性,并采用BET、XRD和H2-TPR手段对催化剂的表征进行测试。结果表明,Mn/Fe=1:1的催化剂在低温段(100℃~300℃)活性更高,表征结果表明,Mn/Fe=1:1的催化剂的比表面积大、结晶度低、氧化还原能力强,这都是Mn/Fe=1:1的催化剂活性较高的原因。     

Role of NO in Hg oxidation over a commercial selective catalytic reduction catalyst V2O5–WO3/TiO2

Experiments were conducted in a fixed-bed reactor that contained a commercial catalyst, V₂O₅–WO₃/TiO₂, to investigate mercury oxidation in the presence of NO and O₂. Mercury oxidation was improved by NO, and the efficiency was increased by simultaneously adding NO and O₂. With NO and O₂ pretreatment at 350°C, the catalyst exhibited higher catalytic activity for Hg⁰ oxidation, whereas NO pretreatment did not exert a noticeable effect. Decreasing the reaction temperature boosted the performance of the catalyst treated with NO and O₂. Although NO promoted Hg⁰ oxidation at the very beginning, excessive NO counteracted this effect. The results show that NO plays different roles in Hg⁰ oxidation; NO in the gaseous phase may directly react with the adsorbed Hg⁰, but excessive NO hinders Hg⁰ adsorption. The adsorbed NO was converted into active nitrogen species (e.g., NO₂) with oxygen, which facilitated the adsorption and oxidation of Hg⁰. Hg⁰ was oxidized by NO mainly by the Eley–Rideal mechanism. The Hg⁰ temperature-programmed desorption experiment showed that weakly adsorbed mercury species were converted to strongly bound ones in the presence of NO and O₂.     

蜂窝式MnO_x/PG-CC催化剂的制备及低温选择性催化还原法脱硝性能

采用悬浮浆液法将凹凸棒石(PG)涂覆于堇青石蜂窝陶瓷(CC)基体上,制取PG-CC涂层载体,利用过饱和浸渍法负载MnOx制备MnOx/PG-CC催化剂应用于柴油车尾气SCR脱硝.考察了制备条件对催化剂低温SCR活性的影响,采用BET、SEM-EDS、XRD手段对催化剂的理化性质进行了分析表征,探讨了催化剂结构特性与活性间的构效关系.研究发现,堇青石基体经PG涂层后,对活性组分的一次负载量显著增加,由3%增至13%,对应的催化剂低温脱硝活性显著提高,在100℃脱硝活性由10%提高到78%.结果分析表明,堇青石基体经PG涂层后比表面积大幅度增加,可以承载更高的活性组分,且活性组分具有更好的分散性,从而使得催化剂的活性点增加;另一方面,PG涂层催化剂具有更高的表面Mn4+/Mn3+价态比,更有利于催化剂的低温选择性催化还原法(SCR)活性.活性组分Mn Ox与PG涂层之间的协同作用是导致催化剂低温SCR脱硝活性得以提升的关键因素.研究结果表明,通过对堇青石蜂窝基体进行凹凸棒石涂层后采用浸渍法负载锰氧化物,可制备出具有较高低温SCR活性的蜂窝式模块催化剂.     

电晕放电与络合催化联合同时去除烟气中SO_2、NO实验研究

采用电晕放电与液相络合催化协同同时去除烟气中SO2和NO,电压、水流量、乙二胺合钴浓度、pH、SO2和NO初始浓度以及气流量对同时去除SO2和NO效率的影响进行了实验研究.结果表明:NO去除率随着放电电压、水流量、乙二胺合钴浓度、pH的增加而增加,而随SO2和NO初始浓度、烟气流量的增大而减小;SO2去除率也随放电电压,水流量的增加而增加,随烟气流量的增加而下降,但溶液pH,SO2和NO初始浓度和乙二胺合钴浓度对其影响很小.溶液中加入Mn2+和尿素能分别增强SO2和NO的去除效果.最佳条件为:电压25 kV、水流量80 L·h-1,乙二胺合钴浓度0.02 mol·L-1,烟气流量1.0 m3·h-1、尿素浓度0.02 mol·L-1,Mn2+浓度为0.02 mol·L-1时,NO和SO2去除率分别可达68%和94%,对应能量消耗分别为22.2 g·k Wh-1和75.2 g·k Wh-1.     

Influences of pH value in deposition-precipitation synthesis process on Pt-doped TiO2 catalysts for photocatalytic oxidation of NO

This work has been undertaken to study the influences of pH value on the characteristics and activity of photocatalyst by deposition-precipitation method during its preparation process. A series of Pt-modified TiO₂ were prepared by deposition-precipitation method at different pH values as well as wet impregnation method, and characterized by XRD, XPS, TEM, UV-Vis and photoluminescence (PL). It was found that the catalysts had the highest photocatalytic activity for NO conversion when pH value was kept at around 7. And the sample prepared by deposition-precipitation method showed higher activity than that by impregnation method. This was mainly due to their high value in highly-dispersed platinum oxides (PtOx) content on the surface of the catalysts. The results from UV-Vis absorption showed that highest absorbance was obtained for Pt/TiO₂ prepared at pH values of around 7. And PL spectra results indicated that the recombination rate of photogenerated electrons and holes of the samples prepared by deposition-precipitation method was lower than that prepared by impregnation method. And in the zeta potential study, the pH values for the isoelectric point of the preparing slurry of 0.05 wt.%Pt/TiO₂ and 0.5 wt.%Pt/TiO₂ were determined to be 6.5-8.5, which further confirmed the enrichment of PtOx dopants for the catalysts repapered when pH value was around 7.     

非热等离子体强化碱液吸收脱除烟气中NO和Hg0的研究

采用正电晕放电产生非热等离子体将模拟烟气中的NO和Hg0氧化成更易吸收的NO2和Hg2+,从而强化其碱液吸收脱除,并考察放电电压及入口SO2和NO浓度对氧化和脱除效果的影响.结果表明,随着电压升高,NO和Hg0的氧化和脱除量增加.当NO浓度为134 mg/m3,放电电压为12.8kV时,吸收塔出口NO和NO2浓度分别为0和69 mg/m3.当Hg0浓度为110 μg/m3,放电电压为13.1 kV时,吸收塔出口Hg0和Hg2+浓度分别为22 μg/m3和11 μg/m3.SO2对Hg0的氧化和脱除具有一定促进效应,且这种效应随SO2浓度提高而增强,但SO2对NO的氧化和脱除影响不大.NO对Hg0氧化有明显的抑制效应,随着NO浓度提高,Hg0氧化和脱除量显著降低.当800 mg/m3 SO2、 134 mg/m3 NO和110 μg/m3 Hg0共存时,对应77 J/L的能量输入,NO和Hg0的脱除率分别为57%和31%.     

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.     

唐山市"九五"期间大气环境中SO2、NOX、TSP污染状况分析

根据唐山市大气环境污染特点，对主要污染指标SO2、NO、TSP进行了污染状况分析。结果表明，3项污染指标的平均值均超过国家环境空气质量二级标准。     

基于OMI数据的京津冀及周边地区O3生成敏感性

基于O₃生成敏感性的指示剂法,利用OMI对流层柱浓度HCHO/NO₂分析夏季O₃敏感性.O₃控制区空间分布特征分析结果表明,O₃生成受VOCs排放控制的地区主要集中在北京、太原、石家庄等城市中心及工业较发达地区,受NO_x排放控制的地区主要集中在北京北部、河北北部、河南大部分地区、山东沿海城市,其他区域为NO_x-VOCs协同控制区.分析2005~2016年间京津冀及周边地区O₃生成敏感性的年纪变化特征表明,受VOCs控制的区域面积呈现先增大后减少,受NO_x控制的区域呈先减少后增加的趋势.NO_x控制区在2011年出现“拐点”,NO_x控制区面积占研究区域面积的比例达到最低38%.2011年之后NO_x排放量下降,NO_x控制区面积逐步增大,2016年NO_x控制区占比达到65%,VOCs控制区占比降低为3%.分析2005~2016年6~9月份O₃控制区月变化特征发现,相比6~8月份,9月份VOCs控制区增加显著,这是由于6~8月份的NO_x控制区转变为NO_x-VOCs协同控制区,NO_x-VOCs协同控制区向VOCs控制区转变.     

外源脱落酸缓解二氧化硫对胡杨细胞的毒性

二氧化硫(SO_2)是一种常见的大气污染物.前期研究表明,过氧化氢(H_2O_2)和一氧化氮(NO)参与调控SO_2诱导的胡杨细胞毒性.脱落酸(ABA)是一种植物逆境激素,目前关于ABA在植物细胞响应SO_2胁迫中的具体作用并不清楚.因此,本文以胡杨愈伤细胞为材料,采用SO_2衍生物处理,研究外源ABA在植物细胞SO_2毒性缓解中的作用及相关机制.结果发现:2 mmol·L~(-1)SO_2衍生物处理胡杨细胞9 h后,细胞电解质外渗率和细胞死亡率明显增加;外源施用5μmol·L~(-1)ABA可明显缓解SO_2对胡杨细胞的毒性,降低电解质外渗率和细胞死亡率.2 mmol·L~(-1)SO_2衍生物胁迫下,与SO_2单独处理组相比,添加外源ABA能够使胡杨细胞的抗坏血酸过氧化物酶(APX)和过氧化氢酶(CAT)活性分别提高23.9%和48.0%,从而减少胞内H_2O_2水平.此外,SO_2胁迫下,外施ABA后胡杨细胞的Pe Nia1、Pe Nia2基因表达受到明显抑制,细胞硝酸还原酶(NR)活性降低24.1%,胞内NO合成减少.以上结果表明,SO_2胁迫下,外源施加ABA可有效降低胡杨细胞内H_2O_2和NO水平,从而缓解SO_2对胡杨细胞的毒性.