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.     

酸雨与镧对大豆幼苗生长的复合伤害效应研究

为探索酸雨与稀土镧对大豆幼苗生长的复合影响及其内在机制,以重要油粮作物大豆(Glycine max)为材料,研究在模拟酸雨pH分别为3.0、3.5、4.5与稀土镧La(Ⅲ)浓度分别为60、100和300mg·L-1处理下大豆幼苗生长及光合作用的变化.结果表明,相对单一酸雨与镧处理,酸雨与La(Ⅲ)复合处理组中大豆幼苗的生长受抑制程度增大,两者呈协同效应,且pH越低,La(Ⅲ)浓度越高,抑制效应越明显.光合参数的变化规律与生长指标近同,相同处理组各光合参数的降幅不一致,其中最大荧光(Fv/Fm)和叶绿素含量(Chl)的降幅范围分别为9.53%～22.75%和9.14%～24.53%,较净光合速率Pn(22.78%～84.7%)、希尔(Hill)反应速率(15.52%～73.38%)和Mg2+-ATPase活性(14.51%～71.54%)小,表明各光合参数对2个胁迫因子的敏感程度存在差异.进一步相关性分析发现,Pn变化主要受Hill反应速率与Mg2+-ATPase活性的影响,而Chl、Fv/Fm次之.表明酸雨与La(Ⅲ)对植物光合过程各环节的作用机制不同,光合作用受阻是影响植物生长的重要因素之一.     

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.     

两种新型涂铁改性砂的过滤性能及反冲洗条件研究

以两种新型涂铁改性石英砂(纳米氧化铁改性砂,Nano-OCS;氧化铁改性砂,IOCS)及普通石英砂(RQS)为研究对象,考察了两种新型改性砂对沉后水腐殖酸及浊度的直接过滤效果,对其反冲洗条件进行优化研究,并对3种滤料的过滤效果进行了比较.结果表明,1滤层厚度为45 cm时,最佳滤速为6 m·h-1;3种滤料对腐殖酸和浊度的直接过滤效果依次为:Nano-OCSIOCSRQS,其中两种涂铁砂对腐殖酸的去除率分别为71.70%和61.61%;2Nano-OCS和IOCS滤柱的反冲洗流程分4步,对应的流程及最佳操作条件为:首先,用0.5 mol·L-1NaOH的溶液浸泡,气冲强度13 L·s-1·m-2,气冲时间6 min;然后,用0.075 mol·L-1的NaOH溶液与空气同时反冲洗,NaOH溶液冲洗强度为8 L·s-1·m-2,气冲强度13 L·s-1·m-2,冲洗时间3 min;接着用0.015 mol·L-1的FeCl3溶液与空气同时反冲洗,FeCl3溶液冲洗强度为8 L·s-1·m-2,气冲强度13L·s-1·m-2,冲洗时间2 min;最后,用清水冲洗,冲洗强度8 L·s-1·m-2,冲洗时间4 min.两种涂铁砂反冲洗前后表面形态结构更加复杂、粗糙度增加,对腐殖酸去除率进一步提高.3当滤层厚度由45 cm增加到80 cm时,Nano-OCS对腐殖酸直接过滤的最高去除率由74.6%提高至80.3%,平均去除率由57.9%提高至68.5%.