Selective reduction of NO by photo-SCR with ammonia in an annular fixed-film photoreactor

Gaseous NO was photocatalytically reduced at room temperature by photo-assisted selective catalytic reduction (photo-SCR) with ammonia over TiO₂ in this study. NO reduction efficiency and N₂ selectivity were determined from gases composition at the outlet stream of photoreactor. Effect of operating conditions, e.g. light intensity and inlet concentrations of ammonia and oxygen, on the NO reduction efficiency and N₂ selectivity were discussed to determine the feasible operating condition for photocatalytic reduction of NO. Experimental results showed that selective catalytic reduction of NO with ammonia over TiO₂ in the presence of oxygen was a spontaneous reaction in dark. The photoirradiation on the TiO₂ surface caused remarkable photocatalytic reduction of NO to form N₂, NO₂, and N₂O under 254 nm UV illuminations, while almost 90% of N₂ selectivity was achieved in this study. The ammonia and oxygen molecules played the roles of reductant and oxidant for NO reduction and active sites regeneration, respectively. The reduction of NO was found to be increased with the increase of inlet ammonia and oxygen concentrations until specific concentrations because of the limited active sites on the surface of TiO₂. The kinetic model proposed in this study can be used to reasonably describe the reaction mechanism of photo-SCR.     

2006─2010年环保重点城市主要污染物浓度变化特征

利用2006─2010年全国环保重点城市的空气质量日报数据,分析了大气ρ(SO2)、ρ(NO2)和ρ(PM10)的变化特征. 结果表明:从年际变化看,ρ(SO2)和ρ(PM10)呈下降趋势,ρ(NO2)变化不显著.从季节变化看,ρ(SO2)、ρ(NO2)和ρ(PM10)均呈冬季高、夏季低的特征.从浓度谱分布看,全国大气中ρ(SO2)、ρ(NO2)和ρ(PM10)分别集中在0～0.150、0～0.100和0～0.250 mg/m3范围内,ρ(SO2)和ρ(PM10)谱峰区间逐渐向低浓度范围偏移,高浓度事件逐渐减少,表明SO2和PM10污染得到较明显的控制,而ρ(NO2)谱峰变化不大.从浓度变化看,山西ρ(SO2)、ρ(NO2)和ρ(PM10)下降最明显,年变化率分别为-11.2、-3.6和-14.2 μg/m3;青海ρ(SO2)、山东ρ(NO2)和ρ(PM10)的上升趋势最明显,年变化率分别为4.4、2.7和4.5 μg/m3.      

利用SCIAMACHY遥感资料研究我国NO2柱浓度及其时空分布

利用SCIAMACHYENVISAT 2003—2009年月均观测数据,结合1∶4 000 000行政区划图,得到了近7 a来我国城市级别NO₂柱浓度的时空分布和变化趋势,并采用Seasonal Mann-Kendall非参数检验方法对各城市的变化趋势进行了显著性分析. 结果表明:我国NO₂分布东高西低,NO₂柱浓度高值区主要分布在京津冀及环渤海区域、长江三角洲北部及广东省等地区. 近7 a来我国北部和中部地区的NO₂增长趋势显著,NO₂柱浓度平均值最高和增速最快的前20个城市主要分布在江苏、山东和安徽等省的二级城市郊县和小城市. 与统计年鉴工业废气排放数据的比较表明,工业废气排放与NO₂柱浓度及其时空分布具有较好的一致性. 这种新的NO₂污染格局应该引起重视并采取有针对性的污染监管措施.      

NO在分子筛ZSM-5催化剂上催化氧化动力学研究

研究了常温下NO在疏水型高硅分子筛ZSM-5上的氧化反应. 结果发现,NO在分子筛ZSM-5表面氧化的同时,伴随着明显的吸附过程,待吸附饱和后释放出NO2.相比于活性炭,高硅分子筛ZSM-5上NO氧化受水汽影响较小,303K饱和湿气下,NO稳态转化率只比干气下降低6%.在排除内、外扩散影响的条件下,于等温积分反应器中研究了稳定阶段NO氧化的本征动力学,根据不同温度下X~W/FA0及NO分压数据,计算了反应速率,建立简化的动力学模型并获得了反应速率方程,结果表明其拟合复相关系数较高.     

南充市城市空气质量变化及达标分析

为了掌握南充市近年来城市空气质量变化及其达标情况,对南充市城区2008～2012年SO2、NO2和PM10的质量浓度数据进行统计分析,并计算各个站点的空气污染指数和空气质量指数。结果表明,3种污染物浓度值都有明显的下降趋势,S02浓度在0．002～0．052mg／m^3之间变化;N02浓度值从0．042mg／m^3下降到0．029mg／m^3;PM10浓度在0．060～0．063mg／m^3之间波动。南充市空气质量冬季较差,夏季较好。在5个监测点中,炼油厂空气质量最差,优良率为92．9％（85．1％）;高坪空气质量最好,优良率为99．1％（98．3％）。相关性分析表明,南充市空气污染源主要是工业燃煤和机动车尾气。     

水体中氨氮污染来源及其控制——富营养化的思考

本文从营养学的角度,叙述氮源对水体富营养化的产生和危害,并从生态系统中物质循环分析氨氮的多方来源,根据其不同来源提出相应的控制措施。     

上海市机动车发展的大气环境容量

研究了上海市机动车和固定源排放对环境中NOx 浓度的贡献率 ,采用ADMS Urban空气质量模型从环境容量角度提出上海市机动车发展的总量控制目标 .2 0 0 2年上海全市NOx 排放总量为 39 7× 10 4t/a ,其中中心城区机动车NOx 排放分担率81% ,浓度贡献率为 86 % .为实现 0 0 8mg/m3 年平均浓度容量控制目标 ,上海市机动车NOx 排放总量应控制在 3 5× 10 4t/a以下     

Phylogenetic diversity of NO reductases,new tools for nor monitoring,and insights into N2O production in natural and engineered environments

● 548 representative nor genes were collected to create complete phylogenetic trees. ● The distribution of nor and nod genes were detected in 18 different phyla. ● The most conserved amino acids in NOR were located adjacent to the active site. ● nor-universal and Clade-specific primers were designed, suggested, and tested. Nitric oxide reductases (NORs) have a central role in denitrification, detoxification of nitric oxide (NO) in host-pathogen interactions, and NO-mediated cell-cell signaling. In this study, we focus on the phylogeny and detection of qNOR and cNOR genes because of their nucleotide sequence similarity and evolutionary relatedness to cytochrome oxidases, their key role in denitrification, and their abundance in natural, agricultural, and wastewater ecosystems. We also include nitric oxide dismutase (NOD) due to its similarity to qNOR. Using 548 nor sequences from publicly accessible databases and sequenced isolates from N₂O-producing bioreactors, we constructed phylogenetic trees for 289 qnor/nod genes and 259 cnorB genes. These trees contain evidence of horizontal gene transfer and gene duplication, with 13.4% of the sequenced strains containing two or more nor genes. By aligning amino acid sequences for qnor + cnor, qnor, and cnor, we identified four highly conserved regions for NOR and NOD, including two highly conserved histidine residues at the active site for qNOR and cNOR. Extending this approach, we identified conserved sequences for: 1) all nor (nor-universal); 2) all qnor (qnor-universal) and all cnor (cnor-universal); 3) qnor of Comamonadaceae; 4) Clade-specific sequences; and 5) nod of Candidatus Methylomirabilis oxyfera. Examples of primer performance were confirmed experimentally.     

利用LUR模型模拟天津市大气污染物浓度的空间分布

针对传统监测方法无法满足对大气污染物空间分布高分辨率的要求,以Arcgis为平台,利用LUR模型模拟天津市PM10和NO2年均浓度的空间分布.选取的回归变量为1~4km半径缓冲区内的道路总长度、不同土地利用类型的面积、人口密度、风向指数及距海距离,选取3个监测点的监测数据对方程进行了验证.结果表明,对PM10年均浓度影响最大的因素是缓冲区为1km的道路总长度(R2为0.560),而对NO2年均浓度影响最大的因素是人口密度(R2为0.414).多元线性回归方程计算结果显示,PM10和NO2的R2分别达到0.946和0.691;如果考虑风向的影响,R2可分别提高到0.980和0.849.对天津市中心城区建立5km′5km网格嵌套,根据多元线性回归方程计算每个网格交点的污染物浓度模拟值.通过kriging插值得到2种污染物在天津市中心城区的空间模拟分布图.PM10年均浓度分布以研究区中心最高,向四周逐渐降低;NO2的年均浓度以研究区中心最低,向四周逐渐升高.模拟结果与实际情况相符.     

疏水型H-ZSM-5分子筛上NO氧化反应的研究

针对NO低温氧化催化剂的抗水汽性差的问题,以疏水型高硅H-ZSM-5分子筛为NO氧化催化剂,在温度为10~90℃、NO进口浓度为0.05%~0.08%,及相对湿度为0~100%条件下,考察了NO的氧化反应.结果表明,H-ZSM-5分子筛的硅铝比由50提高至300时,湿气条件(水汽含量1.18%)下,NO氧化率由20%升高至56%;干气下,低温有利于NO氧化;湿气下(水汽含量1.18%),NO氧化率随着温度的升高先增加后减少,最佳反应温度为20℃,与NOx工业废气的排放温度相近.200h的稳定性试验结果显示,在30℃、NO进口浓度0.08%、空时0.5s、保持相对湿度为50%或100%时,NO氧化率可维持在60%和50%,催化剂具有良好的稳定性.