SO2对MnOx/PG催化剂低温脱硝的影响机理研究

采用等体积浸渍法制备了锰氧化物负载凹凸棒石(MnO_x/PG)低温SCR催化剂,通过SO₂暂态响应、程序升温表面反应(TPSR)等实验技术研究了烟气中SO₂对催化剂SCR脱硝活性的影响行为.采用程序升温脱附(TPD)、BET比表面及孔径分布测定、XPS等表征技术对催化剂硫中毒的机理及化学本质进行了深入分析.结果表明,低温下烟气中SO₂对MnO_x/PG催化剂的SCR脱硝活性存在显著的抑制作用,催化剂中毒主要由烟气中SO₂的催化氧化引起.一方面SO₂氧化为SO₃后与NH₃及H₂O竞争反应形成复杂的硫酸铵盐堵塞催化剂孔道,另一方面与活性组分MnO₂结合形成MnSO₄使得部分活性组分形态发生变迁.其中硫酸铵盐的形成可通过适当的热处理得以去除,而MnSO₄则不可恢复,但催化剂SCR活性却显著增加,表明MnSO₄的形成不是催化剂失活的主要因素.吸附态的硫可显著增加催化剂表面酸性,因此对SCR活性有促进作用.催化剂失活主要机理为:由气相SO₂的连续氧化并与NH₃相结合形成硫酸铵盐,并且在低温下难以分解,以致堵塞催化剂活性中心.     

季铵型树脂的合成及其对水中溴酸根及前驱物溴离子的吸附性能与机制

水中的溴离子(Br^-)和溴酸根离子(BrO₃^-)由于难挥发、易溶解、稳定性好而难以除去,因此,制备了一种对较低浓度的Br^-和BrO₃^-都有良好吸附去除效果的季铵碱树脂(Quaternary ammonium base resin,QABR)并表征了其物化结构.同时,考察了初始浓度、QABR投加量、溶液pH、离子强度、吸附接触时间和吸附温度等因素对QABR吸附Br^-和BrO₃^-性能的影响.结果表明,在0.05～4.00 mmol·L^-1浓度范围内,在298 K、pH=7.0时QABR对Br^-和BrO₃^-的吸附能力最佳,其最大吸附量分别为1.78 mmol·g^-1和1.65 mmol·g^-1;QABR对Br^-和BrO₃     

MnOx同步除锰氨氮滤池的快速启动及污染物去除机制

通过将MnO_x负载于石英砂表面形成MnO_x滤料,并以此构筑滤池,开展动态试验,考察了滤池的启动周期、污染物去除效率及影响因素;同时通过表征MnO_x结构变化和灭活滤料表面微生物等方法探究了MnO_x滤池的污染物去除机制.结果表明:运行第1d滤池出水锰即可达标,运行至第9d,滤池启动完成,可实现对水中锰和氨氮的同步有效去除.滤池可稳定同步去除锰和氨氮的最大平均浓度分别为1.4和1.6mg/L,滤速为6m/h,且通过提升水中溶解氧含量可进一步增强滤池对锰和氨氮的去除效果.SEM、EDS和XRD分析结果表明,滤池运行过程中, MnO_x由相对密实的颗粒堆积形态逐步发展为多孔的一体化海绵状结构,其组成由ramsdellite和birnessite型MnO₂,逐步发展为buserite和birnessite型MnO₂,但元素组成相对较为稳定.结合滤料表面的微生物灭活实验,认为滤池稳定运行阶段,MnO_x对锰的去除主要为非生物作用,...     

进水亚硝氮限制下Anammox去除氨氮研究

利用UASB反应器分别在降低进水亚硝氮/氨氮比（R）和停供亚硝氮条件下研究了Anammox体系运行特性.发现随着进水亚硝氮减少,亚硝氮与氨氮去除摩尔比减小,发生氨氮超量去除现象,即使进水无亚硝氮时也可去除氨氮.当R为1：2时,氨氮超量去除量达最大,均值为57.2mg/L;长期停供亚硝氮条件下氨氮能够稳定去除,平均去除量为45.6mg/L.停供亚硝氮后Anammox体系中微生物群落多样性增加,AnAOB、氨氧化菌和反硝化菌相对丰度均增加.其中AnAOB相对丰度从9.44%增长到13.26%;氨氧化菌相对丰度从3.29%增长到7.3%;反硝化菌相对丰度由0.54%增加到3.14%.研究表明,溶解氧是氨氮超量去除量的限制性因素,氨氮超量去除的途径包括：好氧氨氧化、厌氧氨氧化与部分内碳源反硝化.在微量溶解氧作用下,主要是氨氧化菌与厌氧氨氧化菌协同实现了氮的去除.     

磷钼酸铵-聚乙烯醇复合材料的制备及其对水中Cs+的吸附性能研究

利用磷钼酸铵、聚乙烯醇和正硅酸四乙酯合成一种新型复合材料（AMP-PVA）,运用扫描电镜（SEM）、傅里叶红外光谱（FTIR）、X射线衍射（XRD）、X射线光电子能谱（XPS）和热重分析仪（TG-DSC）等对AMP-PVA进行结构和形貌表征.同时,探究了不同初始浓度、pH、时间等因素对AMP-PVA特异性吸附Cs⁺性能的影响,并结合等温吸附曲线、吸附动力学等对AMP-PVA的吸附机制进行探讨.结果表明,AMP-PVA可在pH=2~11范围内使用,耐酸性能良好,且在35 ℃、pH=7.7、初始Cs⁺浓度为200 mg·L^-1的条件下达到最大吸附量109.56 mg·g^-1;吸附过程以自发的、吸热的、可持续的化学吸附为主,符合Freundlich等温吸附模型和准二级动力学模型,并伴随着内扩散和Boyd模型的特征;AMP-PVA主要作用机制为Cs⁺与AMP中的NH₄⁺发生离子交换.     

Application of an aerosol electrical mobility spectrum analyzer: Charged-particle polarity ratio measurement in the Antarctic and Arctic regions

An aerosol electrical mobility spectrum analyzer (AEMSA), developed at Hanyang University, was employed to investigate the particle charge characteristics in the Antarctic and Arctic regions. The particle charge characteristics in these areas were compared with the charging state in Ansan, South Korea, located in the midlatitude, where artificial factors, such as human activity, urbanization, and traffic, might result in a higher total concentration. Furthermore, in Ansan, South Korea, the charged-particle polarity ratio was very stable and was close to 1. However, notably different particle charge characteristics were obtained in the Antarctic and Arctic regions. The imbalance between the numbers of positively and negatively charged particles was evident, resulting in more positive charges on the atmospheric particles. On average, the positively charged particle concentrations in the Antarctic and Arctic areas were 1.4 and 2.8 times higher, respectively, compared with the negatively charged particles. The developed AEMSA system and the findings of this study provide useful information on the characteristics of atmospheric aerosols in the Antarctic and Arctic regions and can be further utilized to study particle formation mechanisms.     

土壤铵氮在热活化过硫酸盐氧化过程中的转化

采用来自江苏和河北, 具有不同土壤有机质含量和NH₄⁺浓度的土壤样本, 系统地研究了NH₄⁺在热活化过硫酸盐(PS)氧化过程中的转化和归趋, 考察了反应时间、PS浓度和外加NH₄⁺对硝基副产物生成的影响.结果表明, 土壤中的NH₄⁺能够转化成3-硝基酚、4-硝基酚、2-羟基-5-硝基苯甲酸、4-羟基-3-硝基苯甲酸、2, 4-二硝基酚等副产物, 它们的生成量随着反应的进行先增加后降低.增大PS浓度可促进硝基副产物的生成.当PS浓度为30mmol/kg, 反应12h后一硝基酚和一硝基羟基苯甲酸的生成量达到最大.然而随着PS浓度进一步增大, 硝基副产物发生降解.硫酸根自由基(SO₄·^-)在硝化过程中起到了关键作用, 它能将NH₄⁺氧化生成氨基自由基(·NH₂), 随后经过一系列自由基链式反应生成二氧化氮自由基(NO₂·).同时, SO₄·^-进攻土壤有机质中的酚结构单元, 使其氧化生成苯氧自由基, 苯氧自由基进一步与NO₂·结合生成硝基副产物.天然有机质(NOM)在环境中无处不在, NH₄⁺在环境中也普遍存在, PS用于土壤和地下水污染修复时生成硝基副产物很可能是一个普遍现象.     

Silica-quaternary ammonium “Fixed-Quat” nanofilm coated fiberglass mesh for water disinfection and harmful algal blooms control

Intensification of pollution loading worldwide has promoted an escalation of different types of disease-causing microorganisms, such as harmful algal blooms(HABs), instigating detrimental impacts on the quality of receiving surface waters. Formation of unwanted disinfection by-products(DBPs) resulting from conventional disinfection technologies reveals the need for the development of new sustainable alternatives. Quaternary Ammonium Compounds(QACs) are cationic surfactants widely known for their effective biocidal properties at the ppm level. In this study, a novel silica-based antimicrobial nanofilm was developed using a composite of silica-modified QAC(Fixed-Quat) and applied to a fiberglass mesh as an active surface via sol–gel technique. The synthesized Fixed-Quat nanocoating was found to be effective against E. coli with an inactivation rate of 1.3 × 10~(-3) log reduction/cm min. The Fixed-Quat coated fiberglass mesh also demonstrated successful control of Microcystis aeruginosa with more than 99% inactivation after 10 hr of exposure.The developed antimicrobial mesh was also evaluated with wild-type microalgal species collected in a water body experiencing HABs, obtaining a 97% removal efficiency. Overall,the silica-functionalized Fixed-Quat nanocoating showed promising antimicrobial properties for water disinfection and HABs control, while decreasing concerns related to DBPs formation and the possible release of toxic nanomaterials into the environment.     

Aerosol optical properties and the mixing state of black carbon at a background mountainous site in Eastern China

In-situ measurements of aerosol optical properties were conducted at Mt. Huang from September 23 to October 28, 2012. Low averages of 82.2, 10.9, and 14.1 Mm~(-1) for scattering coefficient(σ_(sp, neph, 550)), hemispheric backscattering coefficient(σ_(hbsp, neph, 550)), and absorption coefficient(σ_(ap, 550)), respectively, were obtained. Atmospheric aging process resulted in the increase of σap, 550 but the decrease of the single scattering albedo(ω_(550)) at constant aerosol concentration. However, the proportion of non-light-absorbing components(non-BCs) was getting higher during the aging process, resulting in the increase of aerosol diameter, which also contributed to relatively higher σ_(sp, neph, 550) and ω_(550). Diurnal cycles of σ_(sp, neph, 550) and σ_(ap, 550) with high values in the morning and low values in the afternoon were observed closely related to the development of the planetary boundary layer and the mountain-valley breeze. BC mixing state, represented by the volume fraction of externally mixed BC to total BC(r), was retrieved by using the modified Mie model.The results showed r reduced from about 70% to 50% when the externally mixed non-BCs were considered. The periodical change and different diurnal patterns of r were due to the atmospheric aging and different air sources under different synoptic systems. Local biomass burning emissions were also one of the influencing factors on r. Aerosol radiative forcing for different mixing state were evaluated by a "two-layer-single-wavelength" model,showing the cooling effect of aerosols weakened with BC mixing state changing from external to core-shell mixture.     

厌氧氨氧化污泥群体感应信号分子检测及影响研究

厌氧氨氧化作为一种新型的脱氮工艺具有很好的应用前景,但厌氧氨氧化污泥富集培养困难.本研究以处理垃圾渗滤液的污泥作为接种污泥,在升流式厌氧污泥反应器(UASB)中启动厌氧氨氧化过程;检测驯化成功的厌氧氨氧化污泥中是否存在群体感应信号分子;并通过添加外源信号分子(cis-11-Methyl-2-dodecenoic acid,DSF和N-acyl-homoserine lactone,AHL),探究信号分子对厌氧氨氧化污泥附着生长能力的影响.结果表明,UASB反应器在运行150 d后,总氮去除率达到80%,菌群结构中厌氧氨氧化菌所占比例超过了20%,成功启动厌氧氨氧化工艺,且厌氧氨氧化污泥中存在低浓度的AHLs信号分子;人为添加3-碳位置取代基为羰基的AHLs(3-oxo-C6-HSL、3-oxo-C8-HSL、3-oxo-C10-HSL和3-oxo-C12-HSL)信号分子均能促进厌氧氨氧化污泥附着生长,而3-碳位置无取代基的AHLs中只有C12-HSL和C6-HSL存在积极影响,C8-HSL、C10-HSL和DSF信号分子对厌氧氨氧化污泥的附着生长能力并没有促进作用.