焙烧温度对CeO_2(ZrO_2)/TiO_2选择性催化脱硝性能的影响

采用溶胶-凝胶法并以不同温度焙烧制备一系列CeO_2(ZrO_2)/TiO_2(CZT)催化剂,考察了CZT催化剂固相结构、酸量、比表面积等性能与催化活性的关系。采用XRD、BET、NH3-TPD、H2-TPR以及XPS等表征技术对催化剂进行表征。结果表明:焙烧温度为450℃时CZT催化剂具有最高的催化活性,其在240~400℃的温度窗口内活性均高于90%,且具有较好的抗水和抗硫中毒能力。随着焙烧温度的提高,催化剂表面的Ce和Zr原子进入体相晶格且Ce0.5Zr0.5O2向Ce0.75Zr0.25O2转变,导致催化剂的储释氧能力和氧化还原性能降低。另外,锐钛矿和金红石型TiO_2晶粒尺寸的增加,催化剂的有效比表面积和总酸量降低,因此CZT催化活性随着焙烧温度的提高而有所降低。换言之,大的比表面积、良好的氧化还原性能、表面Ce4+的富集以及酸性位的增多均有利于NH3-SCR活性的提高。     

β射线法与重量法监测环境空气PM_(2.5)的应用比较

重量法是测量PM_(2.5)的传统手工经典方法,而β射线法加动态加热系统联用光散射法作为自动在线监测技术的常用方法被广泛使用。将5030-SHARP型β射线法加动态加热系统联用光散射法PM_(2.5)自动监测设备监测结果与手工法测量结果进行比对、分析,结果表明:β射线法与重量法监测结果具有一致性,测量结果不存在显著性差异;β射线法与重量法相对偏差值与温度、相对湿度、风速等气象因子的相关性不明显;β射线法与重量法监测结果的差异性与PM_(2.5)质量浓度、季节等条件有关;随着PM_(2.5)质量浓度逐渐升高,β射线法与重量法相对偏差的绝对值|RD|也随之增大,不同季节的|RD|平均值差异较大,春季、冬季的|RD|平均值大于夏季、秋季。     

UV/H_2O_2对氯消毒副产物TCM、DCBM的去除影响因素研究

针对UV/H_2O_2对氯化消毒副产物三氯甲烷(TCM)和一溴二氯甲烷(DCBM)的去除效果及影响因素进行研究,结果表明UV/H_2O_2方法对TCM和DCBM去除效果的影响因素有过氧化氢(H_2O_2)投加量、紫外光照强度、反应p H值和反应物初始浓度。通过不同的反应条件得出:H_2O_2在一定投加量变化范围(10~35 mmol/L)内,随投加量的增加,TCM和DCBM的去除率均呈先上升后下降趋势,H_2O_2最佳投加量分别为25,20 mmol/L;增大紫外光照(UV)强度,TCM和DCBM的去除率均显著提高;随初始p H值的增大,去除率均呈先上升后下降趋势,p H值为7.0时,去除率达到最佳;TCM和DCBM反应初始浓度分别为150,160μg/L时,其去除率最高,在有效时间内去除率分别为95.88%、92.56%。     

Effect of MoO3 on vanadium based catalysts for the selective catalytic reduction of NOx with NH3 at low temperature

The selective catalytic reduction(SCR) activities of the MoO_3 doped V/WTi catalysts prepared by the incipient wetness impregnation method at low temperature were investigated.The results showed that the addition of MoO_3 could enhance the NO_ xconversion at low temperature and the best SCR activity was obtained when the dosage of MoO_3 reached5 wt.%. The NH3-TPD and DRIFTS experiments indicated that the addition of MoO_3 changed the type and number of acid sites on the surface of catalysts and reaction activities of acid sites were altered at the same time. The redox capacity and amount of active oxygen species got improved for V3Mo5/WTi catalyst, which could be confirmed by the H_2-TPR and transient response experiments. Water vapor inhibited the NO_xconversion at low temperature. Deposition of ammonium sulfate or bisulfate might be main reason for the loss of catalytic activity in the presence of SO_2 at low temperature. Choosing the suitable NH_3/NO ratio and elevation of reaction temperature both could weaken the influence of SO_2 on the SCR activity of the V3Mo5/WTi catalyst. Thermal treatment of the deactivated catalyst at350°C could get the low temperature activity recovered. The decrease of GHSV improved the de NO_x efficiency at low temperature and we speculated that the rational technological process and operation parameters could contribute to the application of this kind of catalysts in real industrial environment.     

TiO2–PANI/Cork composite: A new floating photocatalyst for the treatment of organic pollutants under sunlight irradiation

A novel photocatalyst based on TiO_2–PANI composite supported on small pieces of cork has been reported. It was prepared by simple impregnation method of the polyaniline(PANI)–modified TiO_2 on cork. The TiO_2–PANI/Cork catalyst shows the unique feature of floating on the water surface. The as-synthesized catalyst was characterized by X-ray diffraction(XRD),scanning electron micrograph(SEM), transmission electron microscopy(TEM), thermogravimetric analysis(TGA), Fourier transform infrared spectroscopy(FT-IR), UV–vis diffuse reflectance spectra(UV–vis DRS) and the Brunauer–Emmett–Teller(BET) surface area analysis. Characterization suggested the formation of anatase highly dispersed on the cork surface. The prepared floating photocatalyst showed high efficiency for the degradation of methyl orange dye and other organic pollutants under solar irradiation and constrained conditions, i.e., no-stirring and no-oxygenation. The TiO_2–PANI/Cork floating photocatalyst can be reused for at least four consecutive times without significant decrease of the degradation efficiency.     

In-situ synthesis of TiO2 rutile/anatase heterostructure by DC magnetron sputtering at room temperature and thickness effect of outermost rutile layer on photocatalysis

TiO_2 rutile/anatase heterostructure thin films with varying rutile thickness have been in-situ synthesized via DC magnetron sputtering with Ar gas at room temperature. The crystal texture, surface morphology, energy gap and optical properties of the films have been investigated by X-ray diffraction meter, grazing incidence X-ray diffraction meter, Raman spectroscopy, scanning electron microscopy, and UV–visible spectrophotometer, which indicates that the rutile/anatase heterostructure films are successfully fabricated. The further degradation experiments display that the photocatalytic activity can be dramatically affected by the thickness of the outmost rutile layer and the 100 nm thickness exhibits the best performance in all of the TiO_2 thin films. With the increase of the outmost rutile layer, the optical band gap of TiO_2 film displays a systematic decrease slightly. However,the change in photocatalytic activity does not coincide with that in the band gap. The photoresponse and electrochemical properties of the thin films have been characterized to understand the mechanism of the varied photocatalytic activity.     

Pd-MnO2 nanoparticles/TiO2 nanotube arrays (NTAs) photo-electrodes photo-catalytic properties and their ability of degrading Rhodamine B under visible light

Pd-MnO_2/TiO_2 nanotube arrays(NTAs) photo-electrodes were successfully fabricated via anodization and electro deposition subsequently; the obtained Pd-MnO_2/TiO_2 NTAs photo electrodes were analyzed by scanning electron microscopy(SEM), X-ray diffraction(XRD) and characterized accordingly. Moreover, the light harvesting and absorption properties were investigated via ultraviolet–visible diffuse reflectance spectrum(DRS); photo degradation efficiency was investigated via analyzing the photo catalytic degradation of Rhodamine B under visible illumination(xenon light). The performed analyses illustrated that Pd-MnO_2 codoped particles were successfully deposited onto the surface of the TiO_2 nanotube arrays;DRS results showed significant improvement in visible light absorption which was between400 and 700 nm. Finally, the photo catalytic degradation efficiency results of the designated organic pollutant(Rhodamine B) illustrated a superior photocatalytic(PC) efficiency of approximately 95% compared to the bare TiO_2 NTAs, which only exhibited a photo catalytic degradation efficiency of approximately 61%, thus it indicated the significant enhancement of the light absorption properties of fabricated photo electrodes and their yield of UOH radicals.     

深部储层中CO2沿断层泄漏量的影响因素

CGS（CO₂地质储存）是CO₂减排的重要手段之一,天然裂隙的存在则是CGS的潜在风险.CO₂地质储存过程中储层上覆盖层及其浅部含水层是防止CO₂泄漏的天然屏障,为了探究深部咸水层中CO₂沿断层的泄漏过程并获得断层渗透率及储层中超临界CO₂流体初始条件（初始饱和度、初始泄漏压力）对CO₂沿断层泄漏速率和泄漏量的影响程度,依据鄂尔多斯CO₂灌注工程示范区资料,使用多相、多组分溶质运移数值模拟软件TOUGH2建立了2D概念模型.结果表明,深部咸水层中的CO₂在压力差和浓度差的作用下沿断层发生泄漏,到达浅部含水层后开始发生侧向运移,100 a内运移了约200 m的水平距离;由于浮力的作用,CO₂集中在含水层顶板处,有效地防止了CO₂向外泄漏.影响因素分析表明,100 a内断层渗透性能为低渗、中渗和高渗条件时,CO₂累积泄漏量分别为0、1 050和3 000 t;CO₂初始饱和度分别为0.20、0.50和0.99时,CO₂累积泄漏量分别为550、1 050和1 650 t;初始泄漏压力分别为17.3、17.6和18.1 MPa时,CO₂累积泄漏量则分别为900、1 050和1 400 t.除此之外,断层渗透性、CO₂初始气体饱和度和初始泄漏压力对CO₂泄漏的影响还体现在泄漏发生时间和平均泄漏速率上.研究显示,各因素对CO₂沿断层泄漏过程的影响程度表现为断层渗透性能> CO₂初始饱和度> CO₂初始泄漏压力.      

2015年北京采暖季城市森林内外SO2浓度的时空变化特征

为探讨采暖季城市森林内外ρ(SO₂)动态变化及差异性,基于西山国家森林公园林内空气质量监测站数据,结合北京市环境保护监测中心植物园监测站的实时数据,分析2015年采暖季城市森林内外ρ(SO₂)变化和影响因素.结果表明:林内外ρ(SO₂)日变化基本呈双峰双谷型,在09:00-11:00和20:00-22:00左右达到高峰;采样期间ρ(SO₂)月变化呈不显著"V"型,最高值出现在1月,林内外分别为(25.8±9.2)和(31.7±23.4)μg/m3,最低值出现在11月,林内外分别为(19.0±5.2)和(13.0±11.2)μg/m3.林内ρ(SO₂)在1-3月低于林外,11-12月高于林外,林内ρ(SO₂)变化较林外平缓;气象条件对采暖季城市森林ρ(SO₂)变化有重要影响:降水对ρ(SO₂)消减效应明显,大风有驱散SO₂的作用,同时受风向影响;ρ(SO₂)和温度关系不显著(P=0.05,R < 0.40),但和空气相对湿度线性关系显著(α=0.05,Sig=0.00),林内受气象因素影响低于林外.研究显示,城市森林对气态污染物具有一定的缓冲、抵抗和吸收能力,因此应重视发展城市森林生态系统,充分发挥其生态效益,以提高城市大气环境质量.      

基于GIS和LUR模型的西安市PM2.5浓度空间分布模拟研究

基于地理信息系统GIS和土地利用回归LUR模型,模拟西安市PM2.5浓度空间动态分布,结果表明:与PM2.5浓度相关性最高的分别为缓冲区为2 km的水域面积、人口密度和距离水域距离,R 2分别为0.501,0.393和0.280;与PM2.5浓度相关性最低的分别为缓冲区为4 km的水域面积、未利用地面积和耕地面积,R 2分别为0.039、0.021和0.017.未考虑风速建立的LUR模型多元回归的相关系数为0.856,R 2为0.733,考虑风速的相关系数为0.892,R 2为0.796,表明风速对于污染物的分布影响较大,LUR模型模拟效果较好.模拟的PM2.5年均浓度高风险区分布于中部,中风险区分布于中西部,低风险区分布于东南部和西部.