“三明治”PbS纳米晶/rGO复合材料的制备及其对NH_3的室温气敏性能研究

采用一步溶液法制备"三明治"PbS纳米晶/rGO复合材料,通过X射线衍射仪和场发射扫描电子显微镜对样品的晶体结构和表面形貌进行表征,并制作旁热式气敏元器件,测试其气敏特性。研究结果表明在PbS纳米晶/rGO复合材料中,PbS纳米晶均匀负载在rGO片层上,且复合材料存在类似"三明治"的三维结构。该复合材料在室温下对NH_3具有良好检测能力,对1000 ppm NH_3的灵敏度达到3.45,与纯PbS纳米晶及rGO相比,气敏性能得到显著提升,其最低检测极限为1 ppm,且具有良好的氨气选择性。对"三明治"PbS纳米晶/rGO复合材料气敏机理进行分析认为,rGO加入起到载流子传输层的作用,三维结构增加气体扩散速度及吸附面积。三明治状PbS纳米晶/rGO复合材料因其特殊结构及优异的气敏性能,有望在气敏领域得到广泛应用。     

铜掺杂对Fe/β催化剂NH_3-SCR催化性能的影响

制备了一系列Cu掺杂量不同的Fe/β(40)催化剂,并采用ICP-AES、XRD、H2-TPR、UV-vis和XPS等表征技术分析了催化剂的物化性质.结果表明,适量的铜掺杂能大大提高Fe/β(40)催化剂的低温活性,拓宽其活性温度窗口,但过量的Cu掺杂会降低催化剂的N2选择性.Cu掺杂质量比为1.27%Cu-2%Fe/β(40)的催化剂具有最佳的SCR性能,这与催化剂中存在较多离子交换位的Fe~(3+)和Cu~(2+)物种有关,而存在较多的CuO物种会促进氨高温氧化,使催化剂的N2选择性降低且高温窗口变窄.高温水热条件下Cu的存在可能使Cu、Fe物种更容易发生迁移和团聚,导致Cu-Fe/β(40)催化剂的水热稳定性明显变差.     

PbO-PbI2复合物膜转化的CH3NH3PbI3钙钛矿薄膜及其光电特性

有机-无机卤化物钙钛矿是一类优异的光电材料. 在过去四年内, 基于有机-无机卤化物钙钛矿的光电器件实现了超过15%的光电转换效率. 而有机-无机卤化物钙钛矿材料的可控制备是保证其在光电器件中应用的基础. 本文采用新的沉积方法在玻璃衬底表面制备了一种典型的有机-无机卤化物钙钛矿CH₃NH₃PbI₃薄膜. 其制备过程是: 采用超声辅助的连续离子吸附与反应法在玻璃衬底表面沉积PbO-PbI₂复合物膜, 之后与CH3NH3I蒸汽在110 ℃环境下反应, 将PbO-PbI₂复合物膜转化成CH₃NH₃PbI₃钙钛矿薄膜. 对CH₃NH₃PbI₃薄膜的微观结构, 结晶性及其光电性能等进行了表征. 结果表明, CH₃NH₃PbI₃薄膜呈晶态, 具有典型的钙钛矿晶体结构. 薄膜表面形貌均匀, 晶粒尺寸超过400 nm. 在可见光范围, CH₃NH₃PbI₃薄膜透过率低于10%, 能带宽度为1.58eV. 电学性能研究表明CH₃NH₃PbI₃薄膜表面电阻率高达1000 MΩ. 高表面电阻率表明CH₃NH₃PbI₃薄膜具有一定的介电性能, 其介电常数(ε_r)在100 Hz时达到155. 本研究提出了一种制备高质量CH₃NH₃PbI₃钙钛矿薄膜的新方法, 所得CH₃NH₃PbI₃薄膜可望在光、电及光电器件中得到应用.     

Interactions of Cationic Surfactant Cetyl-trimethyl ammonium bromide with Ammonium nitrate: Surface and Thermodynamic Studies

The study of interactions between surfactant and salt in aqueous solutions has attracted significant interest in recent years because of their widespread applications and relatively complex behavior. This work reports the systematic study of surface phenomenon and self-aggregation behavior of cationic surfactant cetyltrimethyl ammonium bromide (CTAB) with ammonium nitrate (NH\begin{document}$ _4 $\end{document}NO\begin{document}$ _3 $\end{document}) salt. Surface and thermodynamic properties of cationic surfactant CTAB with NH\begin{document}$ _4 $\end{document}NO\begin{document}$ _3 $\end{document} were investigated at different temperatures using different techniques such as conductometry and surface tensiometery. The surface tension measurement was carried out to find out the critical micelle concentration, free energy of adsorption, free energy of micellization, minimum area per molecule, and surface excess concentration. The study reveals that the process of micellization is spontaneous and exothermic in nature. Conductance measurement was carried out to determine critical micelle concentration, degree of ionization and degree of counter ion binding. Addition of NH\begin{document}$ _4 $\end{document}NO\begin{document}$ _3 $\end{document} to the surfactant solutions increase the values of degree of ionization and degree of counter ion binding, although it lowers the values of critical micelle concentration showing that the process of micellization is more favorable and spontaneous. The study is very helpful to develop better understanding about interaction between electrolyte and surfactant, which are used in many applications and in different processes (e.g., pharmaceutical, industrial foaming, drug solubilization, oil recovery, and medium for metal nanoparticle formation).     

THF-FER沸石的系列研究IV.固体酸性及C5烯烃骨架异构化催化性能

在四氢呋喃(THF)-Na2O-SiO2-Al2O3-H2O体系中水热合成的THF-FER沸石,经酸交换／焙烧或焙烧／酸交换处理可制得H-FER-1和H-FER-2两种H型沸石．红外光谱及NH3-TPD等实验结果表明,两者的强酸位主要是对烯烃骨架异构化反应有贡献的Bronsted酸位．1073K／10h的高温水蒸汽处理会导致沸石骨架脱铝,但并未产生过多的末端硅羟基．两者比较,H-FER-1沸石的结构缺陷较少,Bronsted酸位较多,骨架更完美．由THF-FER沸石制备的H-FER催化剂,对C5正构烯烃骨架异构化反应显示了优良的催化活性、选择性及稳定性．     

氧/硫杂卟啉内氢迁移反应的理论研究

采用B3LYP/6-31G**方法在Gaussian 03程序下, 对氧杂卟啉(OPH), 硫杂卟啉(SPH)的结构和能量进行优化, 并寻找与内氢迁移反应相关的过渡态构型. 计算结果表明, 由于分子内氢键的存在, 氧或硫杂化均会使卟吩内氢迁移正负反应速率明显降低.     

硝酸铵对SO2在大气颗粒物表面气-粒转化影响的模拟研究

利用流动态的原位傅里叶变换红外漫反射光谱(DRIFTS)对含硝酸铵气溶胶(以α-Fe₂O₃为主模拟气溶胶)与SO₂的非均相反应进行了研究, 比较了硝酸铵与其它金属氧化物(CaO, MgO, α-Al₂O₃和SiO₂)与SO₂反应的情况.实验结果表明, 硝酸铵和α-Fe₂O₃混合颗粒物比硝酸铵和其它金属氧化物混合颗粒与SO₂反应的吸附系数高, 表明α-Fe₂O₃比其它金属氧化物催化能力变强.利用BET面积作为反应活性表面积, 发现含有6％(质量分数)NH₄NO₃的α-Fe₂O₃混合颗粒物与SO₂反应具有最高的比表面积吸附系数(γ_BET=2.42×10^-9), 比纯氧化铁的反应高了近1.8倍.而纯NH₄NO₃颗粒与SO₂不发生反应, 表明少量硝酸铵的存在在一定程度上提高了SO₂在气溶胶颗粒物表面转化成硫酸盐的能力. 本文还讨论了含硝酸铵气溶胶与SO₂的反应机制及其对大气环境的影响.     

Performance and Kinetics Studies on Selective Catalytic Reduction of NOx with NH3 over MnOx-WO3/TiO2 Catalyst

The catalytic activities of MnOx-WO3/TiO2 for selective catalytic reduction(SCR) of NO with NH3 were investigated in a wide range of temperature and reaction condition.It yielded a NOx conversion of 80.3%-99.6% and a N2 product selectivity of 100%-98.7% during 100 °C to 350 °C at gas hourly space velocity(GHSV)=18900 h-1.In the presence of 0.01% SO2 and 6% H2O at 120 °C,the NOx conversion can maintain 98.5%.At 300 °C and with 0.07% SO2 in reactant stream,the NOx conversion stabilized at 99% as high as the commercial V-W/TiO2 catalyst's level.The steady-state kinetics study shows that O2 played a promoting role.In the presence of less than 1.5% O2,NOx conversion can increase sharply with the increase of O2 concentration.The reaction order was zero with respect to NH3 and first with respect to NO with excess O2 and H2O.The kinetics active energy(Ea) of Mn-W/TiO2 was calculated to be 6.24 kJ/mol according to the kinetic experiment at various temperatures,much lower than those of other catalysts reported in the literature.Mn-W/TiO2 is an excellent catalyst for SCR of NO with NH3 by now.     

ZnSe晶体气相生长输运剂Zn(NH4)3Cl5的热分解行为及动力学

晶体生长;非等温动力学;ZnSe晶体气相生长输运剂Zn(NH4)3Cl5的热分解行为及动力学     

Influence of cationic substitution on lattice constants and optical characterization in solution grown mixed crystals of potassium‐ ammonium zinc chloride

Mixed crystals of potassium‐ammonium zinc chloride in different concentrations were grown from aqueous solution employing the techniques of slow cooling and controlled evaporation. Powder x‐ray diffraction studies were carried out on the grown crystals. The comparison between lattice parameters a, b and c are experimentally determined and calculated by Vegad's law. The concentration of K⁺ ions in the crystals was measured by the atomic absorption technique. The crystal morphology changed considerably by increasing K⁺ concentration. The optical absorption coefficient (α) indicated strong influence changing concentration. The optical energy gap was found to decrease with increasing K⁺ concentration. (© 2006 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)