胶州湾及邻近海域表层海水中一氧化氮浓度分布及其影响因素探讨

2011年2～3月利用化学发光法对胶州湾及邻近海域表层海水中一氧化氮(NO)浓度进行了监测.结合水文、化学和生物等要素的同步观测资料,对该海域NO浓度分布及其影响因素进行了探讨.结果表明,胶州湾内表层海水中NO浓度为0.080～0.493 nmol.L-1,平均值为(0.292±0.146)nmol.L-1,胶州湾外NO浓度为未检出～0.435 nmol.L-1,平均值为(0.160±0.130)nmol.L-1.总体来说,胶州湾表层海水中NO浓度呈现出自湾内向湾外递降的分布趋势,陆地径流和人为活动可能对NO浓度的分布造成一定程度的影响.胶州湾及邻近海域表层海水中NO浓度比开阔大洋高1个数量级.周日变化研究表明,NO浓度具有一定的变化特征,最大值出现在15:00,这可能主要受光照的影响.影响NO浓度分布的因素比较复杂,可能主要受亚硝酸盐、光强和pH等因素的影响.结果表明,2011年春季胶州湾及邻近海域表层海水是大气NO的源,通量约为1.09×10-15 mol.(cm2.s)-1.     

Effects of long-term amendment of organic manure and nitrogen fertilizer on nitrous oxide emission in a sandy loam soil

To understand the effects of long-term amendment of organic manure and N fertilizer on N2O emission in the North China Plain, a laboratory incubation at different temperatures and soil moistures were carried out using soils treated with organic manure （OM）, half organic manure plus half fertilizer N （HOM）, fertilizer NPK （NPK）, fertilizer NP （NP）, fertilizer NK （NK）, fertilizer PK （NK） and control （CK） since 1989. Cumulative N2O emission in OM soil during the 17 d incubation period was slightly higher than in NPK soil under optimum nitrification conditions （25℃ and 60% water-filled pore space, WFPS）, but more than twice under the optimum denitrification conditions （35℃ and 90% WFPS）. N2O produced by denitrification was 2.1-2.3 times greater than that by nitrification in OM and HOM soils, but only 1.5 times greater in NPK and NP soils. These results implied that the long-term amendment of organic manure could significantly increase the N2O emission via denitrification in OM soil as compared to NPK soil. This is quite different from field measurement between OM soil and NPK soil. Substantial inhibition of the formation of anaerobic environment for denitrification in field might result in no marked difference in N2O emission between OM and NPK soils. This is due in part to more rapid oxygen diffusion in coarse textured soils than consumption by aerobic microbes until WFPS was 75% and to low easily decomposed organic C of organic manure. This finding suggested that addition of organic manure in the tested sandy loam might be a good management option since it seldom caused a burst of N2O emission but sequestered atmospheric C and maintained efficiently applied N in soil.     

Kinetics of selective catalytic reduction of NO by NH3 on Fe-Mo/ZSM-5 catalyst

The catalyst of Fe-Mo/ZSM-5 has been found to be more active than Fe-ZSM-5 and Mo/ZSM-5 separately for selective catalytic reduction (SCR) of nitric oxide (NO) with NH3. The kinetics of the SCR reaction in the presence of O2 was studied in this work. The results show that the observed reaction orders were 0.74-0.99, 0.01-0.13, and 0 for NO, O2 and NH3, respectively, at 350-450℃. And the apparent activation energy of the SCR was 65 kJ/mol on the Fe-Mo/ZSM-5 catalyst. The SCR mechanism was also deduced. Adsorbed NO species can react directly with adsorbed ammonia species on the active sites to form N2 and H2O. Gaseous O2 might serve as a reoxidizing agent for the active sites that have undergone reduction in the SCR process. It is also important to note that a certain amount of NO was decomposed directly over the Fe-Mo/ZSM-5 catalyst in the absence of NH3.     

Effect of C/N ratio, aeration rate and moisture content on ammonia and greenhouse gas emission during the composting

Gaseous emission (N₂O, CH₄ and NH₃) from composting can be an important source of anthropogenic greenhouse gas and air pollution. A laboratory scale orthogonal experiment was conducted to estimate the effects of C/N ratio, aeration rate and initial moisture content on gaseous emission during the composting of pig faeces from Chinese Ganqinfen system. The results showed that about 23.9% to 45.6% of total organic carbon (TOC) was lost in the form of CO₂ and 0.8% to 7.5% of TOC emitted as CH₄. Most of the nitrogen was lost in the form of NH₃, which account for 9.6% to 32.4% of initial nitrogen. N₂O was also an important way of nitrogen losses and 1.5% to 7.3% of initial total nitrogen was lost as it. Statistic analysis showed that the aeration rate is the most important factor which could affect the NH₃ (p = 0.0189), CH₄ (p = 0.0113) and N₂O (p = 0.0493) emissions significantly. Higher aeration rates reduce the CH₄ emission but increase the NH₃ and N₂O losses. C/N ratio could affect the NH₃ (p = 0.0442) and CH₄ (p = 0.0246) emissions significantly, but not the N₂O. Lower C/N ratio caused higher NH₃ and CH₄ emissions. The initial moisture content can not influence the gaseous emission significantly. Most treatments were matured after 37 days, except a trial with high moisture content and a low C/N ratio.     

La-Co-Fe-Cu/HZSM-5在尾气碳颗粒燃烧中的催化性能

采用柠檬酸络合低温浸渍法制备分子筛负载钙钛矿型复合氧化物催化剂。采用XRD、SEM和H2-TPR等手段对催化剂性能进行表征,并在微型固定床反应器中对催化剂进行活性评价。结果表明,在钙钛矿型复合氧化物中进行B位离子掺杂,可以改善催化活性,碳颗粒燃烧温度降低。在20%LaCoO3/HZSM-5催化剂中用铁离子部分取代钴离子可以改善碳颗粒的燃烧性能,取代量增加碳颗粒燃烧温度降低,但是生成CO2的选择性也降低,以20%LaCo0.2Fe0.8O3/HZSM-5为催化剂,Tig、Tm和Tf分别为256℃、399℃和403℃,但生成CO2的选择性只有72.5%。在20%LaCo1-xFexO3/HZSM-5中的钙钛矿型复合氧化物B位离子中加入铜离子后,在碳颗粒燃烧反应中生成CO2的选择性得到明显改善,Sco2提高10个单位以上。以20%LaCo0.2Fe0.6Cu0.2O3/HZSM-5为催化剂,在碳颗粒燃烧反应中生成CO2的选择性可以达到94.7%,Tig、Tm和Tf分别为242℃、427℃和445℃。     

燃煤电厂烟气氮氧化物排放控制技术发展现状

在广泛查阅文献的基础上,对近年来国内外已成功应用和正在研究开发的一些主要的燃煤烟气氮氧化物控制技术进行了介绍。结合我国目前脱硝行业整体水平和国家环保政策要求,对我国脱硝行业技术研发方向提出了建议。     

快速高效去除微囊藻的GO/QPEI复合纳米材料

本研究合成了一种新型高效的去除铜绿微囊藻(Microcystis aeruginosa)的氧化石墨烯/季铵盐聚乙烯亚胺(GO/QPEI)纳米复合材料.GO/QPEI在pH为4~10的条件下都具有高效去除M.aeruginosa的能力,其去除能力在2 min内可达96%以上.GO/QPEI对微囊藻的吸附更符合Freundlich方程,最大吸附量为5.58×1011cells·mg-1.吸附动力学表明GO/QPEI的假二级吸附反应.GO纳米片和QPEI的协同效应是其高效去除微囊藻的主要机制.     

Mo-modified Pd/Al2O3 catalysts for benzene catalytic combustion

Mo-modified Pd/Al2O3catalysts were prepared by an impregnation method and tested for the catalytic combustion of benzene. The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction（XRD）, X-ray photoelectron spectroscopy（XPS）, temperatureprogrammed desorption of NH3（NH3-TPD）, H2temperature-programmed reduction（H2-TPR）, and high-angle annular dark-field scanning transmission electron microscopy（HAADF-STEM）. The results showed that the addition of Mo effectively improved the activity and stability of the Pd/Al2O3catalyst by increasing the dispersion of Pd active components, changing the partial oxidation state of palladium and increasing the oxygen species concentration on the surface of catalyst. In the case of the Pd-Mo/Al2O3catalyst,benzene conversion of 90% was obtained at temperatures as low as 190°C, which was 45°C lower than that for similar performance with the Pd/Al2O3catalyst. Moreover, the 1.0% Pd-5% Mo/Al2O3catalyst was more active than the 2.0% Pd/Al2O3catalyst. It was concluded that Pd and Mo have a synergistic effect in benzene catalytic combustion.     

春、夏季长江口及其邻近海域溶解N2O的分布和海-气交换通量

分别于2012年3月和7月对长江口及其邻近海域进行了调查,对水体中溶解氧化亚氮(N2O)的分布及海-气交换通量进行了研究.结果表明,春季长江口及其邻近海域表层海水中溶解N2O浓度范围为9.34~49.08 nmol·L-1,平均值为(13.27±6.40)nmol·L-1.夏季表层溶解N2O浓度范围为7.27~27.81 nmol·L-1、平均值为(10.62±5.03)nmol·L-1.两航次表、底层海水中溶解N2O浓度相差不大.长江口溶解N2O浓度由近岸向外海逐渐降低,受陆源输入影响显著.溶解N2O浓度高值出现在长江口最大浑浊带附近,这主要是由于水体中较高的硝化速率造成的.温度是影响N2O分布的另一个重要因素,对溶解N2O浓度有双重作用.春季和夏季表层海水中N2O饱和度范围分别为86.9%~351.3%和111.7%~396.0%,平均值分别为(111.5±41.4)%和(155.9±68.4)%,大部分站位处于过饱和状态.利用LM86、W92和RC01公式分别计算了长江口及其邻近海域N2O的海-气交换通量,春季分别为(3.2±10.9)、(5.5±19.3)和(12.2±52.3)μmol·(m2·d)-1,夏季分别为(7.3±12.4)、(12.7±20.4)和(20.4±35.9)μmol·(m2·d)-1,初步估算出长江口及其邻近海域的年平均释放量分别为0.6×10-2Tg·a-1(LM86)、1.1×10-2Tg·a-1(W92)、2.0×10-2Tg·a-1(RC01).长江口及其邻近海域虽然只占全球海洋总面积的0.02%,但其释放的N2O占全球海洋释放量的0.06%,表明长江口及其邻近海域是产生和释放N2O的活跃区域.     

茶叶基水合氧化铁吸附水体中Pb(Ⅱ)的性能

采用原位沉积技术将水合氧化铁(HFO)负载于废弃茶叶渣表面制备了复合材料茶叶基水合氧化铁(HFO-TW),研究了HFO-TW对水溶液中Pb(Ⅱ)的吸附特性,探讨了溶液pH值、时间、共存碱土离子、温度、Pb(Ⅱ)初始浓度等因素对Pb(Ⅱ)的吸附效果的影响.结果表明酸性范围内,Pb(Ⅱ)的吸附量随溶液pH升高而增大;Pb(Ⅱ)的吸附速度较快,100 min内便可达吸附平衡,且动力学曲线较好地符合伪一级和伪二级动力学模型,拟合系数可达98.8%;在竞争离子Ca(Ⅱ)/Mg(Ⅱ)的浓度高于Pb(Ⅱ)50倍时,HFO-TW对Pb(Ⅱ)仍具有较强的吸附能力,Pb(Ⅱ)的吸附量仅分别下降12.1 mg·g-1和8.1 mg·g-1;Pb(Ⅱ)的吸附过程较好地符合Langmuir等温模型,理论最大吸附容量为89.43 mg·g-1,远高于未经改性的茶叶渣和其他生物吸附剂.所有结果均证实HFO-TW在净化实际铅污染水体中有着较为广阔的应用潜力.