Effects of synthesis methods on catalytic activities of CoOx–TiO2 for low-temperature NH3-SCR of NO

A series of cobalt doped TiO_2(Co-TiO_2) and Co Oxloaded TiO_2(Co/TiO_2) catalysts prepared by sol–gel and impregnation methods respectively were investigated on selective catalytic reduction with NH_3(NH_3-SCR) of NO. It was found that Co-TiO_2 catalyst showed more preferable catalytic activity at low temperature range. From characterization results of XRD,TEM, Raman and FT-IR, Co species were proved to be doped into TiO_2 lattice by replaced Ti atoms. After being characterized and analyzed by NH_3-TPD, PL, XPS, EPR and DRIFTS, it was found that the better NH_3-SCR activities of Co-TiO_2 catalysts, compared with Co/TiO_2 catalyst, were ascribed to the formation of more oxygen vacancies which further promoted the production of more superoxide ions(O-2). The superoxide ions were crucial for the formation of low temperature SCR reaction intermediates(NO-3) by reacting with adsorbed NO molecule. Therefore, these aspects were responsible for the higher low temperature NH_3-SCR activity of Co-TiO_2 catalysts.     

泰山顶PM2.5及其二次组分的输送路径与潜在源

为了明确泰山顶PM_2.5及其二次组分的输送路径与潜在来源,基于后向轨迹聚类方法对2015年冬季和春季抵达泰山顶的气团传输轨迹进行聚类分析,并利用PSCF（潜在源贡献因子）和CWT（浓度权重轨迹）方法分析泰山顶冬季和春季PM_2.5、SO₄2-、NO₃-和NH₄+的潜在源域.结果表明,冬季和春季来自不同方向的气团轨迹对泰山顶PM_2.5及其组分的潜在源分布的影响具有明显差异.冬季泰山顶ρ（PM_2.5）和ρ（NO₃-）平均值的最高值对应的气团轨迹来自湖北、河南、山东济宁等地区,而来自西北方向的轨迹1和轨迹2分别对应的ρ（SO₄2-）和ρ（NH₄+）平均值最高;春季影响ρ（PM_2.5）和ρ（NO₃-）的气团轨迹主要来自西南方向的河南、安徽北部、山东聊城等地区,而源自蒙古国途经内蒙古、山西、河南北部和山东聊城的气团轨迹对ρ（SO₄2-）和ρ（NH₄+）的贡献最大.泰山顶ρ（PM_2.5）、ρ（SO₄2-）、ρ（NO₃-）和ρ（NH₄+）的PSCF分布特征与CWT分布特征类似,WPSCF（源区分布概率）和CWT的最高计算值主要集中山东济宁、聊城以及邻近的山西省、河北省和河南省,是泰山顶大气污染物的主要潜在源域.      

石家庄秋季一次典型霾污染过程水溶性离子粒径分布特征

为研究石家庄秋季典型霾污染过程中颗粒物水溶性离子的粒径谱分布,并进一步分析其来源及形成机制,于2013年10月15日到11月14日利用惯性撞击式8级采样器(Andersen)对石家庄城区大气颗粒物进行了为期一个月的连续采样,并使用离子色谱仪对观测期间一次霾污染过程颗粒物中8种水溶性无机离子(Na~+、NH_4~+、K~+、Mg~(2+)、Ca~(2+)、Cl~-、NO_3~-、SO_4~(2-))进行了分析.结果表明,石家庄秋季颗粒物污染严重,采样期间PM10和PM2.5日均值分别达到(361.2±138.7)μg·m~(-3)和(175.6±87.2)μg·m-3,PM_(2.5)日均值达到国家环境空气质量二级标准的2.3倍.此次污染过程,优良天、轻/中度污染天和重度污染天总悬浮颗粒物中总水溶性无机离子(TWSII)浓度日均值分别为(64.4±4.6)、(109.9±22.0)和(212.9±50.1)μg·m-3,由优良天过渡到重度污染天,总水溶性无机离子中二次无机离子(SO_4~(2-)、NO_3~-和NH_4~+)的比例由44.9%上升至77.6%,此次的霾污染过程主要来源于二次无机离子的生成和积累.优良天,SO_4~(2-)、NO_3~-和NH_4~+呈现双模态分布,峰值分别出现在0.43~0.65μm和4.7~5.8μm,而在轻/中度污染天和重度污染天,逐渐转变为单模态分布,峰值出现在0.65~1.1μm,随着高湿度下液相反应的加剧,二次无机离子由凝结模态向液滴模态转移的迹象明显.Na+、Mg~(2+)和Ca~(2+)这3种离子在优良天、轻/中度污染天和重度污染天的粒径分布相似,均以粗模态形式存在,在4.7~5.8μm出现峰值;K~+、Cl~-在优良天、轻/中度污染天和重度污染天均为双峰分布,但峰值出现的粒径段有所改变.     

桂林市酸雨变化特征及来源分析

对桂林市2008~2011年共396个降水样品p H值统计表明,桂林市酸雨具有明显的季节性差异,夏季酸雨污染程度较低,冬春两季最为严重;对其中44个降水样品做离子分析,通过计算中和因子(NF)分析2008年酸雨程度低主要是NH_4~+和Ca~(2+)等碱性离子中和所致,相对酸度FA达到0.006,表明有99.4%酸性离子被中和;通过富集因子(EF)分析降水中主要离子来源,CI~-和Na~+主要为海洋来源,Ca~(2+)主要为地壳来源,K~+、SO_4~(2-)、NO_3~-主要为人为来源;最后通过Hysplit后向轨迹模拟分季节对2010年强酸雨水汽来源进行追踪,聚类,分析桂林市酸雨受区域输送的影响,确定致酸物质的3个主要源地:1东北向的江西、安徽、湖南、湖北等省份的工业集中、人口密集地区,来源于这些地区的气团春季占到19%,夏季26%,秋季19%,冬季由于盛行东北风,占到36%;2东南方向的广东省尤其珠三角地区,来源于西太平洋的气流经过此地到达桂林,春季占到19%,秋季占到33%,冬季占到36%;3西南向的南宁、柳州等本省城市,春季所有的强酸雨水汽气团都汇合到桂林的西南侧,经南宁、柳州抵达桂林,夏季直接受西南季风的控制,来自印度洋的水汽径直抵达桂林占到75%,秋季途经该地的西南向气流占到14%,冬季63%.     

湿热流域化学风化与水化学组成季节变化——以西枝江流域为例

为研究湿热中小流域岩石化学风化与化学径流组成的关系，选取硅酸盐岩为主的东江一级支流西枝江流域，分别于2011年1月和7月采集干流和支流水样品并测量其化学组成，运用图解法和正演模型对西枝江流域水化学组成进行分析和定量计算。结果表明，Na⁺和HCO₃^-为西枝江流域水体的主要阳离子和阴离子，两者分别占总阳离子和总阴离子的55%以上。硅酸盐矿物的化学风化对水体阳离子的贡献最大（45.8%），其次是人类活动和碳酸盐矿物风化的贡献（分别是24.7%和22.0%），大气输入对阳离子的贡献相对较少（7.5%）。受碳酸盐矿物风化和人类活动影响较大的支流水化学组成季节变化较大，受硅酸盐矿物化学风化影响的河流水化学组成季节变化不明显。西枝江流域硅酸盐矿物和碳酸盐矿物化学风化速率分别是8.27和56.95 t/（km²·a），二者化学风化对大气CO₂的消耗速率分别为0.80×10⁵和8.52×10⁵ mol/（km²·a）。     

电生成Fenton试剂处理染料废水

对电生成Fenton试剂处理酸性铬兰K染料废水进行了研究。采用石墨作阴、阳极,电解过程中向阴极表面通纯氧,并在废水中加入-定量的Fe2+,氧在阴极上还原生成H2O2,H2O2又产生强氧化剂·OH,进而对酸性铬兰K染料废水进行脱色降解。在槽电压为6 V、pH为2.5、电解液中FeSO4·7H2O的质量浓度为0.5 g／dm3、Na2SO4的质量浓度为20 g／dm3的条件下电解废水60 min,染料废水脱色率和COD去除率分别达74.1％和57.9％,电解废水120min后,染料废水脱色率和COD去除率分别达92.9％、71.3％。动力学研究表明,染料的降解符合一级动力学过程,速率常数k为0.02224 min-1。     

Determination of model parameters for zinc (II) ion biosorption onto powdered waste sludge (PWS) in a fed-batch system

Biosorption of zinc (II) ions onto pre-treated powdered waste sludge (PWS) was investigated using a completely mixed tank operating in fed-batch mode instead of an adsorption column. Experiments with variable feed flow rate (0.05-0.5 L h(-1)), feed Zn(II) ion concentrations (37.5-275 mg L(-1)) and amount of adsorbent (1-6 g PWS) were performed using fed-batch operation at pH 5 and room temperature (20-25 degrees C). Break-through curves describing variations of aqueous (effluent) zinc ion concentrations with time were determined for different operating conditions. Percent zinc removal from the aqueous phase decreased, but the biosorbed (solid phase) zinc ion concentration increased with increasing feed flow rate and zinc concentration. A modified Bohart-Adams equation was used to determine the biosorption capacity of PWS (q'(s)) and the rate constant (K) for zinc ion biosorption. Biosorption capacity (q'(s)=57.7 g Zn kg(-1) PWS) of PWS in fed-batch operation was found to be comparable with powdered activated carbon (PAC) in column operations. However, the adsorption rate constant (K=9.17 m(3) kg(-1) h(-1)) in fed-batch operation was an order of magnitude larger than those obtained in adsorption columns because of elimination of mass transfer limitations encountered in the column operations. Therefore, a completely mixed tank operated in fed-batch mode was proven to be more advantageous as compared to adsorption columns due to better contact between the phases yielding faster adsorption rates.     

南京市不同天气过程下颗粒物中水溶性离子分布特征及其来源解析

于2018年11月16~28日使用在线气体组分及气溶胶监测系统MARGA ADI 2080观测了南京市颗粒物中的水溶性无机离子和一些痕量气体,结合气象要素和探空数据,分析了霾、雾、清洁和降水这4类过程中污染物及水溶性离子的分布特征及其昼夜差异.结果表明,在4类过程中PM_2.5平均浓度（μg·m^-3）在26.9（降水）~96.4（霾）,而总水溶性离子浓度（μg·m^-3）在23.7（降水）~89.7（霾）.在霾和雾过程中离子浓度大小排序为NO₃^- > NH₄⁺ > SO₄^2- > Cl^- > K⁺ > Ca²⁺ > Na⁺ > Mg²⁺,而在清洁和降水过程中为NO₃^- > SO₄^2- > NH₄⁺ > Cl^- > Ca²⁺ > K⁺ > Na⁺ > Mg²⁺.水溶性离子的昼夜分布特征在4类过程中差异较大,但昼夜间SO₄^2-、NO₃^-和NH₄⁺（SNA）均呈现出在霾>雾>清洁>降水过程中的特征.由PMF源解析结果分析得到,二次源是影响霾的主导因素,二次源、海盐及燃烧源是雾过程的主要污染来源,降水过程对燃煤源和二次源的清除作用较清洁过程更明显.     

Copper(II) ions’ removal from aqueous solution using green horse-chestnut shell as a low-cost adsorbent

The adsorption of copper(II) ions from aqueous solutions by the green horse-chestnut shell was studied in a batch adsorption system. It was determined how the parameters of the adsorption process, such as time, pH, copper(II) ions concentration and sorbent dose, influence the effectiveness of copper(II) ions’ removal. The adsorption process was fast and equilibrium was established about 10?min, and near 95–97% of Cu(II) ions were removed from aqueous solution. Maximum copper(II) ions’ adsorption occurred at around pH 5. The adsorption kinetics are also described, using pseudo-first-order model and pseudo-second-order model of type 1 and 2. A comparison of the kinetics models on the overall adsorption rate showed that the adsorption system was best described by the pseudo-second-order model of type 1 (r²?=?0.999) for all initial concentrations. Another key part of this study was the use of the Freundlich model to determine the adsorption isotherm and the experimental data were in strong correspondence with this model.     

城市区域土体铁的化学行为与土体强度变异关系研究

统计了南宁市地下水中Fe的变化情况,实验研究了Fe的物理化学行为与土体强度之间的联系,并进一步研究了铁对土体强度影响的双向性.结果显示,城市区域将由于Fe的溶蚀、置换作用等使土体强度降低;城市区域CO2分压增高将促进土体中铁的溶蚀而使土体强度进一步恶化.在含水量相对较高时,铁质胶结物被溶解、迁移,土体强度降低;而在含水量相对较低时,铁质胶结物不易被溶解,而更趋向于发生沉淀反应,使土体对铁的吸附作用加强,从而使土体的强度增加.