负载型Pt模型催化剂中Pt纳米粒子的形貌对CO氧化活性的影响

采用简单的化学还原法制备了具有不同形貌特征的Pt纳米粒子,并利用浸渍法将其负载到SiO2上,得到了粒子分散均一的负载型Pt催化剂,考察了其催化CO氧化反应性能.X射线荧光分析、X射线光电子能谱、红外光谱和透射电镜结果表明,Pt/SiO2模型催化剂上CO氧化活性的不同来源于Pt纳米粒子不同晶面的贡献,即Pt纳米粒子的晶型...     

Pt负载复合氧化物催化剂的CO催化发光性能

采用非晶态络合物法制备了La0.9Cu0.1MnO3和LaCoO3钙钛矿催化剂, 并利用固定化溶胶工艺合成了Pt纳米粒子负载的Pt/La0.9Cu0.1MnO3和Pt/LaCoO3复合催化剂. 通过透射电镜(TEM)、X射线衍射(XRD)和X射线光电子能谱(XPS)等手段对催化剂的微观结构、形貌及Pt的价态进行了研究; 考察了催化剂的CO催化氧化发光性能. 结果表明, 若La0.9Cu0.1MnO3催化剂表面上负载的Pt纳米颗粒形成团聚, 则在其CO催化氧化发光谱中出现发光峰分裂的现象, 而在Pt纳米颗粒分散较好的Pt/LaCoO3体系中却没有出现这一情况. 因此可以利用CO催化发光谱来初步判断贵金属纳米颗粒在载体表面的分散状态.     

组合型Pt/TiO_2催化剂用于低温催化甲苯完全氧化

将均匀分布的纳米Pt粒子直接吸附到TiO2载体上,即制得了组合型Pt/TiO2催化剂(Pt/TiO2-AS).与浸渍法制备的Pt/TiO2催化剂(Pt/TiO2-WI)比较,Pt/TiO2-AS催化剂在催化甲苯完全氧化反应中表现出了很好的催化性能,甲苯转化率为100%时的反应温度低至150°C,而且即使在较高甲苯浓度和较高气体空速下,该催化剂也能保持较好的催化性能.通过X射线衍射(XRD)、N2吸附-脱附(BET)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、氢气程序升温还原(H2-TPR)及傅里叶变换红外(FTIR)光谱等对两种Pt/TiO2催化剂的结构和表面性能进行了表征.结果表明组合型Pt/TiO2-AS催化剂粒径小(2.5 nm),活性组分主要以Pt0形式存在且分布在载体表面,而且载体表面Ti―O键活化使催化剂具有较强的催化氧化能力.另外,活性中心的价态变化(Pt0→Ptδ+)是导致Pt/TiO2-AS催化剂失活的主要原因.     

石墨烯氢氧化钴复合催化剂的一步合成及其对酸性橙的催化降解(英文)

用一步合成自组装法制备出了氢氧化钴与还原氧化石墨烯(Co(OH)2/rGO)的复合催化剂,并将其用于水中染料的催化降解实验.通过X射线衍射(XRD),激光拉曼(Raman)光谱,透射电镜(TEM),X射线能量色散谱(EDS)以及X射线光电子能谱(XPS)等一系列分析手段对催化剂的结构形貌进行了详细的表征,表征结果证实氢氧化钴很好地附着在还原石墨烯的表面.最后初步考察了催化剂催化单过硫酸钾(PMS)降解酸性橙(AO7)的性能.结果表明,催化剂显示出了高效的催化性能,酸性橙的色度可在12 min内完全去除,总有机碳(TOC)实验也表明染料降解的同时也可获得较高的矿化度.循环稳定性实验表明在进行到第三次实验时,催化剂仍能保持高的催化活性,将酸性橙在16 min内降解完毕.     

Pt-TiO2/CeO2-MnO2复合催化剂光热降解气相苯

 用溶胶-凝胶法制备Ce-Mn储氧材料,并于该储氧材料上分别负载光催化剂TiO2 和贵金属Pt制备出Pt-TiO2/CeO2-MnO2复合催化剂. 用X射线衍射、 X射线能谱分析、程序升温还原和漫反射紫外-可见光谱等技术对复合催化剂进行了表征,并以光热催化降解气相苯评价了复合催化剂的活性. 结果表明, Mn分别进入到TiO2和CeO2的晶格中形成固溶体; Pt均匀分散在复合催化剂表面; Ce-Mn储氧材料在250 ℃下具有较好的储氧性能; 复合催化剂对紫外及可见光的吸收较强; 1.6%Pt-40%TiO2/CeO2-MnO2复合催化剂的活性较高,光热催化10 h时,苯降解率可达94.5%.     

CNT表面修饰对Pt/CNT在邻氯硝基苯加氢反应中催化性能的影响

用乙二醇还原法制备了碳纳米管(CNT)负载的铂催化剂(Pt/CNT).考察了CNT化学修饰与物理修饰对催化剂的影响.CNT化学修饰采用H2SO4-HNO3氧化法,物理修饰采用十二烷基硫酸钠(SDS)吸附法.用X射线衍射、透射电子显微镜、电感耦合等离子发射光谱、H2程序升温脱附、傅里叶变换红外光谱和元素分析对Pt/CNT催化剂进行了表征,并以邻氯硝基苯选择加氢为探针反应考察了Pt/CNT的催化性能.结果表明,化学修饰与物理修饰都能在CNT表面引入一定数量的活性位,有助于促进Pt异相成核,提高Pt的分散性,进而提高催化剂的活性.SDS在一定浓度下可形成特定结构的胶束,导致形成特定形貌的Pt纳米粒子.     

丙烷脱氢反应中焙烧温度和反应气氛对 Pt-Sn/SAPO-34 催化性能的影响

 在不同的焙烧温度下制备了 Pt-Sn/SAPO-34 催化剂, 并使用 X 射线衍射、N2 吸附、X 射线荧光光谱、O2 脉冲烧炭、H2 程序升温还原和透射电镜等手段对催化剂进行了表征. 在微型反应器中评价了 Pt-Sn/SAPO-34 催化剂对丙烷脱氢制丙烯反应的催化性能, 考察了焙烧温度和反应气氛对催化剂性能的影响. 结果表明, 焙烧温度为 500 oC 时, 催化剂具有最佳的反应活性. 当焙烧温度高于 500 oC 时, 催化剂出现不希望的表面变化, 例如活性 Pt 位点的聚集、Pt 的团聚、Sn 的流失等. 当反应温度为 595 oC 时, Pt-Sn/SAPO-34 催化性能稳定, 且能够保持表面金属状态.     

Pt/BiOCl纳米片的制备、表征及其光催化性能

采用光化学沉积法制备了一系列不同Pt含量的新型Pt/BiOCl纳米片光催化剂,运用N2物理吸附-脱附、X射线粉末衍射、扫描电镜、透射电镜、X射线光电子能谱、光致发光光谱、紫外-可见漫反射光谱等手段对Pt/BiOCl进行了表征,并以λ=254nm的紫外灯和钨灯为光源,考察了Pt含量对Pt/BiOCl光催化降解酸性橙II活性的影响.结果表明,沉积的Pt对BiOCl样品比表面积的影响不大,但可有效增强催化剂对可见光的吸收能力,显著抑制光生电子与空穴的复合.当Pt含量为1%~2%时,能大幅度提高紫外光下BiOCl催化降解染料的活性,并产生可见光活性.这是由于Pt/BiOCl具有一定的可见光吸收能力,产生了Pt纳米粒子的等离子体光催化作用.     

氮铂共掺杂纳米二氧化钛的制备及表征

采用溶胶-凝胶法制备了氮掺杂纳米TiO2(N-TiO2),并用光分解沉积法在N-TiO2表面负载上微量金属Pt形成铂-氮共掺杂纳米TiO2(Pt/N-TiO2).通过X射线衍射、光电子谱、紫外-可见吸收、扫描电镜和光电流测试对催化剂进行了表征.结果表明:Pt和N共掺杂对TiO2的晶型和形貌影响不大,但其吸收边带较纳米TiO2约红移20nm,Pt/N-TiO2电极在可见光区的光电流约为纳米TiO2电极的4倍.     

过渡金属修饰对Pt/M-DMSN催化剂丙烷脱氢性能的影响

以两步法制备了一系列过渡金属(M=Fe, Co, Ni, Cu, Zn)修饰的树枝状介孔二氧化硅纳米粒子(DMSN)负载铂(Pt/M-DMSN)催化剂, 并对该系列催化剂进行了丙烷催化脱氢性能评价. X射线衍射(XRD)、 透射电子显微镜(TEM)、 紫外-可见漫反射光谱(UV-Vis DRS)和氢气程序升温还原(H₂-TPR)表征结果表明, 不同过渡金属在DMSN载体表面分散状态不同,且与Pt的相互作用程度不同. 其中Zn-DMSN载体最有利于Pt的分散, 且反应后催化剂上积碳含量最低; Pt/Fe-DMSN催化剂中Pt与载体的相互作用力较强. 通过活性评价结果可知, Pt/Fe-DMSN催化剂表现出最优的丙烷催化脱氢性能, 丙烷初始转化率为44.2%, 反应6 h后丙烷转化率仍可达36.5%.     

One-Pot Synthesis of Nitrogen-Doped TiO2 with Supported Copper Nanocrystalline for Photocatalytic Environment Purification under Household White LED Lamp

Developing efficient and cheap photocatalysts that are sensitive to indoor light is promising for the practical application of photocatalysis technology. Here, N-doped TiO₂ photocatalyst with loaded Cu crystalline cocatalyst is synthesized by a simple one-pot method. The structure is confirmed by transmission electron microscopy and X-ray photoelectron spectroscopy analysis, which exhibit that Cu metal nanocrystalline is uniformly deposited on the surface of N-doped TiO₂ material. UV-Vis absorption spectra illustrate that the modified samples possess favorable visible light absorption properties and suppressed-electron hole separation. The as-fabricated Cu-loaded N-TiO₂ materials show high activity in photocatalytic decomposing isopropanol and inactivating E. coli under the irradiation of a household white LED lamp. The developed synthetic strategy and photocatalytic materials reported here are promising for indoor environment purification.     

Plasmon-resonance-enhanced visible-light photocatalytic activity of Ag quantum dots/TiO2 microspheres for methyl orange degradation

We successfully prepared Ag quantum dots modified TiO₂ microspheres by facile solvothermal and calcination method. The as-prepared Ag quantum dots/TiO₂ microspheres were characterized by scanning electron microscope, transmission electron microscope, X-ray diffraction, X-ray photoelectron spectroscopy and UV-vis diffuse reflectance spectroscopy. The Ag quantum dots/TiO₂ photocatalyst showed excellent visible light absorption and efficient photocatalytic activity for methyl orange degradation. And the sample with the molar ratio of 0.05 (Ag to Ti) showed the best visible light photocatalytic activity for methyl orange degradation, mainly because of the surface plasmon resonance (SPR) effects of Ag quantum dots to generate electron and hole pairs for enhanced visible light photocatalysis. Finally, possible visible light photocatalytic mechanism of Ag quantum dots/TiO₂ microspheres for methyl orange degradation was proposed in detail.     

Modification of the Optical and Electronic Properties of TiO<Subscript>2</Subscript> By N Anion-Doping for Augmentation of the Visible Light Assisted Photocatalytic Performance

In this work, a nitrogen-doped anatase TiO₂ nanocrystal is prepared by a modified sol-gel preparation method using the nonionic surfactant (polyoxyethylene sorbitan monooleate) as a structural controller and a soft template. The as-prepared samples are characterized by X-ray diffraction, Raman spectroscopy, UVVis diffuse reflectance spectroscopy, and X-ray photoelectron spectroscopy techniques. Then the photocatalytic activity of these samples is assessed by the photocatalytic oxidation of phenol under visible light irradiation. The phenol concentration is measured using a UV-Vis spectrometer. Experimental results show that N-doping leads to an excellent visible light photocatalytic activity of the TiO₂ nanocatalyst. Furthermore, the formation energy and electronic structure of pure and N-doped anatase TiO₂ are described by density functional theory (DFT) calculations. It is found that N-doping narrowed the band gap of bare TiO₂, which leads to an excellent visible light photocatalytic activity of N–TiO₂ nanocatalysts. Therefore, the prepared N–TiO₂ photocatalyst is expected to find the use in organic pollutant degradation under solar light illumination.     

Effect of nitrogen-doping temperature on the structure and photocatalytic activity of the B,N-doped TiO2

B,N-TiO₂ photocatalysts were synthesized by boron doping firstly and subsequently nitrogen doping in NH₃ at variable temperatures. The effects of the nitrogen doping temperature on the structure and photocatalytic activity of the B,N-codoped TiO₂ were investigated. The as-prepared samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), UV-vis diffuse reflectance spectrum (DRS), electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS). The photocatalytic activity was evaluated with photocatalytic degradation of methyl orange dye (MO) under visible light and UV-visible light irradiation. The results suggested that the boron and nitrogen can be incorporated into the TiO₂ lattice either interstitially or substitutionally or both, while the Ti-O-B-N structure plays a vital role in photocatalytic activity in visible light region. The optimal nitrogen doping temperature is 550 °C. Higher temperature may form many oxygen vacancies and Ti³⁺ species, resulting in the decrease of photocatalytic activity in visible light.     

Enhancement of visible-light photocatalytic activity of Cu-doped TiO<Subscript>2</Subscript> nanoparticles

Bare TiO₂ and Cu-doped TiO₂ nanoparticles with different nominal doping amounts of Cu ranging from of 0.5 to 5.0 mol% were synthesized using the modified sol–gel method. The samples were physically characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, Brunauer–Emmett–Teller-specific surface area, UV–Vis diffuse reflectance spectroscopy, zeta potential, X-ray photoelectron spectroscopy, inductively coupled plasma, and photoluminescence techniques. The Cu-doped TiO₂ exhibited good photocatalytic activity in mineralization of oxalic acid and formic acid under visible light irradiation. Photomineralization of oxalic and formic acids under visible light irradiation revealed greatly enhanced photoactivity exhibited by the 2.0 mol% Cu-doped TiO₂ photocatalyst compared to bare TiO₂ . The enhanced photocatalytic performance arises from copper ion doping in the TiO₂ structure, leading to an extended photoresponsive range, enhanced photogenerated charge separation, and transportation efficiency.     

Preparation and photocatalytic antibacterial property of nitrogen doped TiO2 nanoparticles

Nitrogen doped TiO₂ (N-TiO₂) nanoparticles with about 30 nm in size were produced by a sol–gel method and characterized respectively by UV–vis, X-ray diffraction (XRD), Transmission electron microscopy, X-ray photoelectron spectroscopy (XPS). Their photocatalytic antibacterial properties were evaluated by the antibacterial ratio against Escherichia coli in dark and under simulated sunlight respectively. The XRD pattern showed that the doped nano-TiO₂ was mainly composed of anatase phase. The XPS spectra of the N-TiO₂ sample indicated that TiO₂ was doped by nitrogen atom. The nitrogen doping created a new N 2p state slightly above the valence band top consists of O 2p state, and this pushes up the valence band top and decreased the band gap. Which leaded to the absorption edge was red-shifted to the visible light region of UV–vis spectra of nitrogen doped nano-TiO₂ comparing with pure nano-TiO₂. The antibacterial percentage of N-TiO₂ against E. coli reached to 90 % under simulated sunlight for 2 h, which was much better than that in dark, also than that of pure nano-TiO₂. The photo-catalytic antibacterial activity was activated under visible light. The structure and integrity of cell wall and cell membrane were destructed, and even caused the bacteria death.     

Pt deposited TiO2 catalyst fabricated by thermal decomposition of titanium complex for solar hydrogen production

C, N codoped TiO₂ catalyst has been synthesized by thermal decomposition of a novel water-soluble titanium complex. The structure, morphology, and optical properties of the synthesized TiO₂ catalyst were characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, and UV–vis diffuse reflectance spectroscopy. The photocatalytic activity of the Pt deposited TiO₂ catalysts synthesized at different temperatures was evaluated by means of hydrogen evolution reaction under both UV–vis and visible light irradiation. The investigation results reveal that the photocatalytic H₂ evolution rate strongly depended on the crystalline grain size as well as specific surface area of the synthesized catalyst. Our studies successfully demonstrate a simple method for the synthesis of visible-light responsive Pt deposited TiO₂ catalyst for solar hydrogen production.     

钯氮共掺杂TiO2的制备与表征及其可见光催化活性

在空气气氛和N₂中热处理表面均匀分散有尿素和氯化钯的纳米管钛酸,制备了两个系列Pd/N共掺杂的TiO₂光催化剂,并对所得样品进行了X射线衍射、透射电镜、X射线光电子能谱、紫外-可见漫反射光谱、荧光光谱和电子自旋共振等表征.结果表明,焙烧气氛对样品的形貌、晶体结构、光谱吸收、生成的氧空位浓度和可见光光催化性能的影响很大,其中在空气气氛中制备的样品光催化性能优于在N₂中制备的样品.在可见光(λ≥420nm)照射下,以丙烯为模型污染物考察了样品的光催化活性,发现在空气中400℃下焙烧的样品具有最佳的可见光催化活性.另外,讨论了Pd/N共掺杂TiO₂光催化剂具有可见光响应的机理,认为掺杂的Pd/N元素和制备过程中生成的氧空位是影响可见光催化性能的重要因素.     

Synthesis and characterization of substitutional and interstitial nitrogen-doped titanium dioxides with visible light photocatalytic activity

Both substitutional and interstitial nitrogen-doped titanium dioxides (N-TiO₂) were prepared. Their surface states were clarified by XPS spectra of N 1s, O 1s and Ti 2p. The results of photocatalysis show that both substitutional and interstitial N impurities greatly enhance the photoactivity of TiO₂ in visible light. Moreover, the visible light activity of interstitial N-doped TiO₂ is higher than that of substitutional N-doped TiO₂. The microwave synthesis presented in this paper is a promising and practical method to produce interstitial nitrogen-doped photocatalysts with high visible light activity.     

三维有序结构In掺杂TiO_2薄膜的可见光催化活性

采用自组装生长聚苯乙烯胶体模板和溶胶-凝胶法,制备出三维(3D)有序结构In掺杂TiO2(IO-TiO2-In)薄膜可见光催化剂.光催化实验证明,IO-TiO2-In薄膜降解甲醛的可见光活性是TiO2和三维有序结构TiO2(IOTiO2)薄膜的5倍.利用X射线电子衍射(XRD)谱、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)和紫外-可见(UV-Vis)漫反射吸收光谱确定了催化剂的晶相结构、表面微结构和能带结构.结果表明,IO-TiO2-In薄膜具有锐钛矿型三维有序结构,与TiO2相比,增加了比表面积,提高光的利用率;掺入的In离子在薄膜表面形成In2O3和O-In-Clx(x=1,2)物种,既增强可见光的吸收,又有效地促进了光生载流子的分离,提高了光生载流子在固/气界面参加光催化反应的利用率,使催化剂的可见光催化活性显著提高.