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.     

Pd/activated carbon sorbents for mid-temperature capture of mercury from coal-derived fuel gas

Higher concentrations of Hg can be emitted from coal pyrolysis or gasification than from coal combustion, especially elemental Hg. Highly efficient Hg removal technology from coal-derived fuel gas is thus of great importance. Based on the very excellent Hg removal ability of Pd and the high adsorption abilities of activated carbon（AC） for H2 S and Hg, a series of Pd/AC sorbents was prepared by using pore volume impregnation, and their performance in capturing Hg and H2 S from coal-derived fuel gas was investigated using a laboratory-scale fixed-bed reactor. The effects of loading amount, reaction temperature and reaction atmosphere on Hg removal from coal-derived fuel gas were studied. The sorbents were characterized by N2 adsorption, X-ray diffraction（XRD） and X-ray photoelectron spectroscopy（XPS）. The results indicated that the efficiency of Hg removal increased with the increasing of Pd loading amount, but the effective utilization rate of the active component Pd decreased significantly at the same time. High temperature had a negative influence on the Hg removal. The efficiency of Hg removal in the N2-H2S-H2-CO-Hg atmosphere（simulated coal gas） was higher than that in N2-H2S-Hg and N2-Hg atmospheres, which showed that H2 and CO, with their reducing capacity, could benefit promote the removal of Hg. The XPS results suggested that there were two different ways of capturing Hg over sorbents in N2-H2S-Hg and N2-Hg atmospheres.     

Fenton试剂氧化法处理印染废水实验研究

通过将Fenton法应用于印染废水的处理,研究pH值、温度、反应时间、Fe2+投加量以及H2O2投加量对Fenton试剂处理印染废水的影响,同时确定Fenton法处理印染废水的最适反应条件。实验结果表明:(1)最适反应条件,即pH值、温度、反应时间、Fe2+投加量、H2O2投加量分别为3,50℃,45 min,70 mg/L,2.5 mL/L,此时COD的去除率最高,为66.60%。(2)pH值为3时,下列因素对COD的去除率影响程度大小依次为H2O2投加量Fe2+投加量反应时间反应温度。     

V2O5/TiO2催化剂脱除NO的研究

采用了等体积浸渍法制备二氧化钛负载钒氧化物催化剂（V2O5/TiO2）,研究了V2O5负载量、反应温度、烟气流量、氨氮比以及运行时间各因素对NH3选择性催化还原NO反应（SCR）效率的影响.研究结果表明：经过500℃温度下煅烧,烟气流量为200ml/min,负载量为7wt％的V2O5/TiO2催化剂,在400℃温度下反应,NO脱除率可达70.5％.     

浙江省污水污泥处理处置状况的调查

通过对丽水、宁波、衢州、诸暨等浙江省境内十几个地区的污水处理厂的调查发现:目前浙江省内的污水处理工艺中,A2/O、A/O、氧化沟三种工艺占了近50%的份额。而SBR因其方法特点正在受到越来越多的重视。在污泥处理工艺中,填埋占了最大的一部分,有近70%的污水处理厂将产生的污泥进行填埋处理。目前,污泥处理技术单一,需要继续探寻污泥的减量和资源化技术,为日益增多的污泥探寻出路。     

UASB+接触氧化法处理CMC废水

CMC废水属于高盐分高有机物废水,废水COD为50 000~80 000 mg/L,含盐量为13%左右,不适合直接生化处理。本文采用CMC废水和循环冷却水按一定比例混合后一起处理,混合后的废水采用UASB+接触氧化法的处理工艺处理。工程运行表明:稀释后的CMC废水中的盐分稳定在1.4%以内,该处理工艺能够确保出水达到《污水综合排放标准》(GB8978-1996)中三级排放标准。     

SBR法处理低C/N污水的工程应用——以某基地污水处理站改造工程为例

低C/N污水的生化处理过程中,由于碳源不足,不能满足硝化和反硝化的要求,造成出水NH3-N超标。采用SBR工艺对某基地污水处理站厌氧处理后的低C/N污水进行改造,处理后出水COD去除率达到97%以上,NH3-N去除率达到93%以上。     

电化学氧化PFOA阳极材料筛选及其机制研究

全氟辛酸(PFOA)具有环境持久性及内分泌干扰性,传统的生物降解及高级氧化法对PFOA的去除效果微弱.本研究采用电化学氧化法降解PFOA,选取BDD(掺硼金刚石电极)、Pt、Ti、Ti/RuO2、Ti/RuO2-IrO2、Ti/In2O3、Ti/SnO2-Sb2O5-IrO2、Ti/SnO2-Sb2O5-RhO2、Ti/SnO2-Sb2O5、Ti/SnO2-Sb2O5-CeO2和Ti/SnO2-Sb2O5-Bi2O3这11种阳极材料为备选电极.采用线性扫描伏安法测试析氧电位(OEP),评价11种电极对PFOA的降解效果和脱氟效果,并采用超声-电化学协同方法间接证明PFOA分子在电极表面的直接电子转移是降解反应的第一步.Ti/SnO2-Sb2O5-Bi2O3、Ti/SnO2-Sb2O5-CeO2、Ti/SnO2-Sb2O5和BDD对PFOA有较好的电氧化效果,降解率分别是89.8%、89.8%、93.3%和98.0%.Pt、Ti/SnO2-Sb2O5-RhO2、Ti/SnO2-Sb2O5-IrO2和Ti/In2O3对PFOA的电氧化效果微弱,降解率分别是2.1%、2.3%、12.5%和3.1%.而Ti、Ti/RuO2和Ti/RuO2-IrO2对PFOA没有电氧化能力.PFOA分子经过电极表面的直接电化学氧化发生脱羧反应,后经过逐步脱掉CF2单元的循环生成短链的全氟羧酸类化合物C6F13COO-、C5F11COO-、C4F9COO-和C3F7COO-.     

汉江上游金水河流域氮湿沉降

汉江上游金水河流域是南水北调工程的重要水源涵养区,但是氮污染已成为该流域水质的主要威胁因素.该研究对汉江的金水河流域开展了为期1 a(2012-02~2013-02)的氮湿沉降观测,并利用氮输出模型估算了氮湿沉降对河流氮负荷的贡献量.结果表明雨水中总氮(DTN)的浓度在0.24~2.89 mg·L-1之间,铵态氮(NH+4-N)、硝态氮(NO-3N)及有机氮(DON)分别占42.8%、13.3%和43.9%;雨水氮浓度随降雨量增大而变小,明显受到降雨的稀释作用.流域内氮湿沉降主要来自人类活动,沉降负荷在4.97~7.00 kg·(hm2·a)-1之间,受降雨量的主要影响,上游地区的氮湿沉降负荷>下游地区>中游地区,春夏两季约占全年氮湿沉降的81%.流域氮湿沉降对河流氮负荷贡献量约为34 000~46 000 kg,只占流域氮肥贡献量的5.05%~6.78%,远小于流域内农业活动化肥氮的贡献量,不是河流氮的主要来源.     

羟基磷灰石-四氧化三铁-沸石复合材料制备及去除水中刚果红研究

采用可溶性磷酸盐、钙离子、二价铁离子、三价铁离子和天然沸石等材料制备了羟基磷灰石-四氧化三铁-沸石(HAPFe3O4-沸石)复合材料,对该复合材料进行了表征,并考察了该复合材料对水中刚果红的吸附作用.结果表明,HAP-Fe3O4-沸石复合材料对水中的刚果红具备良好的吸附能力.当pH由3增加到4或由7增加到11时,HAP-Fe3O4-沸石复合材料对水中刚果红的去除能力下降;当pH由4增加到7时,对刚果红的吸附能力基本保持不变.HAP-Fe3O4-沸石复合材料对水中刚果红的去除率随吸附剂投加量的增加而增加,而对水中刚果红的单位吸附量则随吸附剂投加量的增加而降低.HAP-Fe3O4-沸石复合材料对水中刚果红的吸附动力学过程可以较好地采用准二级动力学模型加以描述,对刚果红的吸附平衡数据可以采用Langmuir和Freundlich等温吸附模型加以描述.根据Langmuir模型确定的最大吸附容量为117 mg·g-1.(pH 7和303 K).HAP-Fe3O4-沸石复合材料对水中刚果红的吸附是自发吸热并伴随熵增加的过程.当pH为7时,HAP-Fe3O4-沸石复合材料吸附水中刚果红的主要机制包括表面配位作用、氢键作用以及路易斯酸碱反应.采用热再生的方法可以使吸附刚果红后的HAP-Fe3O4-沸石复合材料得到再生,热再生后的复合材料可以循环使用并且对水中刚果红的吸附性能良好.X射线衍射分析结果表明HAP-Fe3O4-沸石复合材料含Fe3O4,磁滞回线结果表明HAP-Fe3O4-沸石复合材料具备较高的磁饱和强度,复合材料吸附刚果红后可以很容易地通过外加磁场的作用快速地与水溶液分离.结果表明,HAP-Fe3O4-沸石复合材料适合作为一种吸附剂去除废水中的刚果红.