Effects of metal and acidic sites on the reaction by-products of butyl acetate oxidation over palladium-based catalysts

Catalytic oxidation is widely used in pollution control technology to remove volatile organic compounds. In this study, Pd/ZSM-5 catalysts with different Pd contents and acidic sites were prepared via the impregnation method. All the catalysts were characterized by means of N2 adsorption- desorption, X-ray fluorescence （XRF）, HE temperature programmed reduction （H2-TPR）, and NH3 temperature programmed desorption （NH3-TPD）. Their catalytic performance was investigated in the oxidation of butyl acetate experiments. The by-products of the reaction were collected in thermal desorption tubes and identified by gas chromatography/mass spectrometry. It was found that the increase of Pd content slightly changed the catalytic activity of butyl acetate oxidation according to the yield of CO2 achieved at 90%, but decreased the cracking by-products, whereas the enhancement of strong acidity over Pd-based catalysts enriched the by-product species. The butyl acetate oxidation process involves a series of reaction steps including protolysis, dehydrogenation, dehydration, cracking, and isomerization. Generally, butyl acetate was cracked to acetic acid and 2- methylpropene and the latter was an intermediate of the other by-products, and the oxidation routes of typical by-products were proposed. Trace amounts of 3-methylpentane, hexane, 2-methylpentane, pentane, and 2-methylbutane originated from iso4merization and protolysis reactions.     

Carbonyl emissions from heavy-duty diesel vehicle exhaust in China and the contribution to ozone formation potential

Fifteen heavy-duty diesel vehicles were tested on chassis dynamometer by using typical heavy duty driving cycle and fuel economy cycle. The air from the exhaust was sampled by 2,4- dinitrophenyhydrazine cartridge and 23 carbonyl compounds were analyzed by high performance liquid chromatography. The average emission factor of carbonyls was 97.2 mg/km, higher than that of light-duty diesel vehicles and gasoline-powered vehicles. Formaldehyde, acetaldehyde, acetone and propionaidehyde were the species with the highest emission factors. Main influencing factors for carbonyl emissions were vehicle type, average speed and regulated emission standard, and the impact of vehicle loading was not evident in this study. National emission of carbonyls from diesel vehicles exhaust was calculated for China, 2011, based on both vehicle miles traveled and fuel consumption. Carbonyl emission of diesel vehicle was estimated to be 45.8 Gg, and was comparable to gasolinepowered vehicles （58.4 Gg）. The emissions of formaldehyde, acetaldehyde and acetone were 12.6, 6.9, 3.8 Gg, respectively. The ozone formation potential of carbonyls from diesel vehicles exhaust was 537 mg O3/km, higher than 497 mg O3/km of none-methane hydrocarbons emitted from diesel vehicles.     

南昌市移动源排放清单研究

根据收集的南昌市移动源活动水平数据,采用合适的估算方法、排放因子和GIS技术,建立了南昌市2007—2014年移动源排放清单,并对2014年移动源清单进行了空间化处理与分析,空间分辨率为1 km×1 km.结果表明,2007—2014年南昌市移动源共向大气排放CO、HC、NO_x、PM_(2.5)、PM_(10)、SO_2分别为18.26×10~4、5.07×10~4、18.46×10~4、0.99×10~4、1.08×10~4、3.31×10~4t.其中,2014年移动源向大气中排放的这6种污染物总量分别为2.14×10~4、0.76×10~4、1.97×10~4、0.08×10~4、0.09×10~4、0.55×10~4t.道路移动源中,汽油小型客车是CO、HC和SO_2最大的贡献源,排放量分别占机动车排放总量的55.1%、78.5%和56.1%;柴油重型货车是NO_x、PM_(2.5)和PM_(10)排放贡献率最大的车型,分别占43.2%、40%和40%.非道路移动源中,小型拖拉机对CO、HC、NO_x、PM_(2.5)和PM_(10)的贡献率均较大,分别占非道路移动源排放总量的29.9%、26.9%、23.4%、29.5%和29.8%;SO_2排放主要来源于船舶,占非道路移动源SO_2排放总量的45.1%.高污染排放集中的区域,主要是青山湖区、西湖区和东湖区.     

生物基质对煤渣改良地下渗滤系统脱氮效果的影响

地下渗滤系统(SWIS)对硝化、反硝化过程调控不灵活,导致其对氮的去除效果不够理想。组建了两套SWIS装置(1#装置:65～80cm段没有生物基质;2~#装置:65～80cm段添加生物基质),对沿程氮素、硝化和反硝化作用强度及氮还原酶活性进行分析。结果表明,两套装置均表现为硝化反应主要发生在20～60cm段,反硝化反应主要发生在60～80cm段。2~#装置的反硝化作用明显强于1#装置,因此其TN去除率高于1~#装置。硝化作用强度随深度增加而递减,反硝化作用强度随深度增加而递增。硝酸盐还原酶(NAR)活性随深度的增加而逐渐减弱,亚硝酸盐还原酶(NIR)活性随深度的增加先减弱后又增强。主要原因是2~#装置中添加了干化污泥作为生物基质,为反硝化作用补充了碳源,增强了脱氮能力。     

Study on the denitrification performance of FexLayOz/activated coke for NH3-SCR and the effect of CO escaped from activated coke at mid-high temperature on catalytic activity

Currently, activated coke is widely used in the removal of multiple pollutants from industrial flue gas. In this paper, a series of novel Fe_xLa_yO_z/AC catalysts was prepared by the incipient wetness impregnation for NH₃-SCR denitrification reaction. The introduction of Fe-La bimetal oxides significantly improved the denitrification performance of activated coke at mid-high temperature, and 4% Fe_0.3La_0.7O_1.5/AC exhibited a superior NO_x conversion efficiency of 90.1% at 400 °C. The catalysts were further characterized by BET, SEM, XRD, Raman, EPR, XPS, FTIR, NH₃-TPD, H₂-TPR, et al., whose results showed that the perovskite-type oxide of LaFeO₃ and oxygen vacancies were produced on the catalysts’ surfaces during roasting. Fe-La doping enhanced the amount of acid sites (mainly Lewis and other stronger acid sites) and the content of multifarious oxygen species, which were beneficial for NO_x removal at mid-high temperature. Moreover, it was investigated that the effect of released CO from activated coke at mid-high temperature on the NO_x removal through the lifetime test, in which it was found that a large amount of CO produced by pyrolysis of activated coke could promote the NO_x removal, and long-term escaping of CO on the activated coke carrier did not have a significant negative impact on catalytic performance. The results of the TG-IR test showed that volatile matter is released from the activated coke while TG results showed that the weight loss rate of 4% Fe_0.3La_0.7O_1.5/AC only was 0.0015~0.007%/min at 300–400 °C. Hence, 4% Fe_0.3La_0.7O_1.5/AC had excellent thermal stability and denitrification performance to be continuously used at mid-high temperature. Finally, the mechanisms were proposed on the basis of experiments and characterization results.

     

铁屑去除酸法地浸采铀地下水中硝酸盐的试验研究

在酸法地浸采铀过程中,硝酸及硝酸盐的广泛使用使硝酸盐在地下不断累积并扩散到地下水中,这给矿区地下水造成了一定程度的污染.本试验以铁屑为还原剂,对该地下水中NO3--N的去除进行了批试验和动态试验研究.试验结果表明,铁屑可有效去除地下水中的NO3--N,其去除率随pH值的降低而逐渐升高;溶液中共存的Ca2 、Mg2 对NO3--N的去除影响不大,而SO42-、HCO3-的存在可明显降低NO3--N去除率;铁屑最佳投加量为120 g/L,铁炭最佳体积比为1∶1;二级柱可以明显提高柱子的稳定运行时间,在55 h内NO3--N去除率可保持在93%以上,去除效果较好.     

敏捷网络集成方法在区域应急预案编制中的应用

为解决区域性突发事件应急管理预案的一致性及时效性问题,提出了区域应急组织分层网络集成重构的分级动态预案编制管理方法.结合区域性生物恐怖袭击事件应急管理案例分析,试图提高应急预案编制的实际可操作性.     

好氧硝化颗粒污泥膜生物反应器性能和膜污染研究

实验研究了好氧硝化颗粒污泥膜生物反应器AGMBR的处理性能,并将其与活性污泥膜生物反应器ASMBR进行对比,考察了颗粒污泥在减缓膜污染中所起的作用.好氧硝化颗粒污泥膜生物反应器AGMBR连续稳定运行102 d,系统具有良好的去除有机物和同时硝化反硝化能力,在进水COD和NH+4-N浓度分别为500和200 mg/L时,COD、NH+4-N和TN的去除率分别稳定在86%、94%和45%以上.颗粒污泥有效减缓了膜污染,延长了膜清洗的周期,AGMBR中的膜污染以膜孔堵塞为主,占总阻力的64.81%;滤饼层的阻力为2.1×1012m-1,远小于ASMBR中的16.07×10"m-1;膜清洗周期是相同条件下ASMBR的2.43倍以上;而且AGMBR内不断有新颗粒生成,维持了AGMBR系统性能和运行的稳定.     

对苯二甲酸生产废水回用实验研究

采用高级氧化工艺对对苯二甲酸生产废水进行处理,系统考察了氧化剂投加量、废水pH等对处理效果的影响,得出了最佳工艺条件。经过处理的PTA废水,水质达到了车间用水的要求。本方法具有处理效果好、操作简单和环境友好等优点。     

塔山水库蓝藻暴发的成因及控制

简述了塔山水库蓝藻暴发的过程及成因。指出 ,由于水库的营养物质增多、水质恶化 ,在不利的水文、气象 (高温、光照充足、微风 )等条件下 ,导致蓝藻暴发。提出了相应的控制对策