CO还原NO海泡石铜族金属催化剂的研究

以改性海泡石为载体,负载IB族金属(Cu,Ag,Au),制备CO还原NO的催化剂.用正交实验确定载体海泡石的改性条件.研究考察该催化剂在有氧条件下的催化还原性能,并用XRD、TGA、H2 TPR、BET等对该催化剂进行表征.研究发现,在有氧条件下,IB族金属(Cu,Ag,Au)催化剂中,Cu 海泡石对CO还原NO反应的催化活性最好;Cu负载量为5%、灼烧温度为400℃的催化剂表现出较高的活性;Cu 海泡石催化剂中加入Ce和Sm可以改善催化剂的性能.在实验条件基本相同的情况下,Cu 海泡石的催化活性好于Cu ZSM 5催化剂.     

外源NO介导Cu~(2+)胁迫下番茄幼苗活性氧与内源NO代谢的研究

采用营养液培养方法,研究Cu~(2+)胁迫下外源一氧化氮(nitric oxide,NO)介导的番茄幼苗活性氧及NO代谢途径。结果表明:在Cu~(2+)胁迫下,番茄叶片和根系氧自由基含量增加,NO释放量以及硝酸还原酶(nitrate reductase,NR)和一氧化氮合酶(nitric oxide synthase,NOS)活性降低。外源NO能提高Cu~(2+)胁迫下番茄叶片NR和NOS活性,促进NO的产生,根系NOS活性及NO产量也同时上升。外源NO使精氨酸含量显著增加,而Hb(牛血红蛋白,NO清除剂)可部分抵消NO的促进作用,使Cu~(2+)+SNP+Hb处理下番茄精氨酸含量显著下降。可见,外源NO的加入可通过酶促和非酶促途径促进Cu~(2+)胁迫下NO的合成,介导NO信号调控网络,调节内源NO、精氮酸和活性氧代谢途径,从而缓解过多Cu~(2+)引起的氧化伤害。     

Sublethal concentrations of azinphos-methyl induce biochemical and morphological alterations in Rhinella arenarum embryos

Considering that amphibians are good sentinels of environmental conditions, Rhinella arenarum embryos were used to investigate the effects of sublethal concentrations of the organophosphorus insecticide azinphos-methyl, focusing on its anticholinesterasic or pro-oxidant actions and its possible connection with the appearance of morphological alterations. Early amphibian embryos exposed to azinphos-methyl displayed a protective response through glutathione S-transferase induction, along with superoxide dismutase inhibition. At intermediate embryonic stages, embryos exposed to azinphos-methyl displayed superoxide dismutase inhibition and morphological alterations, although cholinesterase activity was not altered, suggesting that molecular targets other than cholinesterase were involved in the development of morphological alterations. At the end of embryonic development, decreases in reduced glutathione and cholinesterase inhibition were observed, along with a significant increase in the number of malformed embryos. The connection between biochemical alterations and the appearance of malformations was not evident in R. arenarum embryos. However, increased glutathione S-transferase and decreased superoxide dismutase activities could be considered as early markers of exposure to azinphos-methyl. The results obtained demonstrate that sublethal concentrations of azinphos-methyl are a serious threat to toad embryos in their natural habitats because biochemical and morphological alterations could impair their ability to deal with environmental stresses.     

大气PM_（2.5）在线监测仪对SO_4~（2-）、NO_3~-和NH_4~＋的测定评价

通过两套大气细颗粒物（PM2.5）水溶性离子在线监测仪与蜂巢式固气分离器膜采样系统作对比,评估了在线监测仪器对主要水溶性组分SO24-、NO3-和NH4＋的测定结果.美国URG公司生产的在线连续监测分析系统（AIM URG-9000B）对NH4＋和NO3-的监测结果较好,但对SO24-的测定结果存在明显高估,其原因是AIM的平板溶蚀器系统无法完全去除大气中高浓度SO2,从而对SO24-的测定结果有干扰.为解决这一问题,进行了一系列实验,结果表明采用两个溶蚀器串联并用5 mmol.L-1H2O2＋5 mmol.L-1NaOH混合溶液作吸收液时,高浓度的SO2（甚至达到260μg.m-3）可以被完全吸收而对SO24-的测定结果不产生影响.由荷兰能源研究所（ECN）、Metrohm和Applikon共同研制的在线气体组分及气溶胶监测系统（MARGA,ADI2080）对NH4＋和SO24-的监测结果较好,可以满足实验要求;但NO3-的测定结果偏高,其准确性需作进一步评估.新型监测仪器在不同大气环境中投入使用前需进行对比测试,以确定其准确性和精确性.     

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.      

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。     

细叶蜈蚣草对悬沙胁迫的生理生态学研究

研究了悬沙对细叶蜈蚣草(Egeria nojas)营养生殖、叶绿素、抗氧化酶(超氧化物歧化酶和过氧化氢酶)等影响。实验结果表明:悬沙处理96h后,各组细叶蜈蚣草断枝均能发芽,其发芽率均在60%以上,悬沙浓度<4.0g/L时,断枝新芽生长较好,悬沙浓度>6.0g/L时,新芽生长受到影响;各组细叶蜈蚣草叶片的叶绿素a和叶绿素b以及总叶绿素含量均相差不大,叶绿素a/b值都在2.50以上,属于正常范围,变化幅度不大;各试验组中细叶蜈蚣草SOD和CAT相差不大,相对比较稳定,受到影响较小。因此,细叶蜈蚣草对悬沙胁迫具有较好的抗逆性,是一种在含沙量较高水体的生态修复实践中具有良好应用前景的水生植物。     

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.