Preparation of Cu-BiVO4 and Its Photocatalytic Properties for Desulfurization of Model Oil

A photocatalyst Cu-BiVO4 was synthesized by the hydrothermal method and was characterized by XRD, UV-vis DRS, and N2 adsorption-desorption measurement. The catalytic activity of the Cu-BiVO4 samples was studied on desulfurization of thiophene dissolved in n-octane, which was used as a model light oil, via photocatalytic oxidation reaction under illumination by visible light. The catalyst characterization results indicated that the loading of Cu on the catalyst did not change the crystal phase of BiVO4, and the crystallinity of the Cu-BiVO4 sample was found to be better at pH=7. The Cu-BiVO4 samples presented a significant bathochromic shift of the absorption band in the visible region, and the absorption intensity increased for the composite catalyst. The desulfurization experiments showed that the Cu-BiVO4 sample prepared at a pH value of 7 had a better catalytic activity. Under proper operating conditions, the desulfurization rate of the model compound achieved by Cu-BiVO4 sample prepared at pH=7 could reach as high as 90%.     

埃洛石纳米管负载氮掺杂二氧化钛的制备及其太阳光光催化性能

The N-doped TiO2-loaded halloysite nanotubes(N-Ti O2/HNTs) nanocomposites were prepared by using chemical vapor deposition method which was realized in autoclave. The photocatalytic activity of nanocomposites was evaluated by virtue of the decomposition of formaldehyde gas under solar-light irradiation. The XRD patterns verified that the anatase structured TiO2 was deposited on HNTs. The TEM images showed that the surface of HNTs was covered with nanosized TiO2 with a particle size of ca. 20 nm. The UV-vis spectra indicated that the N-Ti O2/HNTs presented a significant absorption band in the visible region between 400 nm and 600 nm. Under solar-light irradiation, the highest degradation rate of formaldehyde gas attained 90% after 100 min of solar-light irradiation. The combination of the photocatalytic property of TiO2 and the unique structure of halloysite would assert a promising perspective in degradation of organic pollutants.     

高效三相光催化剂BiVO4@C3N4@GO的制备及性能研究

NBiVO4, BiVO4@C3N4 and BiVO4@C3N4@GO composite photocatalysts were synthesized, and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive spectrometer(EDS), transmission electron microscopy (TEM), ultraviolet-visible diffuse reflectance spectroscopy (UV-vis DRS), Fourier Transform Infrared Spectroscopy(FT-IR), and Brunauer-Emmett-Teller (BET) surface area techniques. The photocatalytic activity was evaluated for the degradation of the methylene blue (MB) under visible light irradiation and BiVO4@C3N4@GO ternary composite outperformed the binary composites, BiVO4@C3N4 and BiVO4. Then the effects of catalyst dosage, initial pH, and initial methylene blue concentration on degradation process were investigated systematically. The improvement of visible-light photocatalytic degradation performance was attributed to the enhanced visible light absorption, larger surface area, higher adsorption ability, and prolonged lifetime of photo-generated electron-hole pairs. The recycle experiments results showed that the BiVO4@C3N4@GO composite have excellent photo-stability for MB photocatalytic degradation.     

Catalytic Conversion of Bioethanol to Ethylene

Dehydration of bioethanol to ethylene has been investigated on supported cerium-containing catalysts and with additives of lanthanum. It was established that the modification of the 3% Ce/γ-Al2O3 catalyst by lanthanum increases catalyst dispersion, thereby increasing yield of the main product ethylene. The highest yield of ethylene is observed on the CeLa/γ/-A12O3 catalyst under optimal conditions （space velocity： 6,000 hl, bioethanol concentration： 21.7 g/m3 and T = 400℃）.     

硫掺杂g-C3N4多孔纳米片的制备及其光催化降解性能研究

Abstract: In this study, sulfur-doped porous g-C3N4 nanosheets (CN-T-U 1.75) have been synthesized successfully by one-step calcination using urea and thiourea as the precursors. CN-T-U 1.75 exhibited excellent photocatalytic performance for Rhodamine B (RhB) degradation under visible light irradiation, with the kinetic reaction rate constant of 0.01838 min-1. Analysis of the characterization results showed that CN-T-U 1.75 had a larger specific surface area, and the doping caused a change in the energy band structure. Moreover, the catalytic mechanism analysis shows it could produce two oxidation groups of ?O2- and ?OH to degrade pollutants synergistically.     

Preparation and Characterization of Zeolite Beta with Low SiO_2/Al_2O_3 Ratio

Zeolite beta with a low SiO2/Al2O3 ratio was synthesized by a novel two-step process.The synthesized sample was characterized with XRD,SEM,FTIR,and N2 adsorption-desorption and solid-state MAS NMR.The results showed that aluminium species were inserted into the framework of zeolite beta.The BET surface area,volume,and particle size of the zeolite beta sample decreased with decreasing SiO2/Al2O3 ratio.Our process was proved an efficient route to synthesize zeolite beta with a low SiO2/Al2O3 ratio.     

粘结剂对HZSM-5芳构化催化剂的性能影响研究

The effect of different binders on light hydrocarbon aromatization performance of the HZSM-5 catalyst was investigated.Physicochemical properties of the catalysts,such as the specific surface area,pore volume and acidity,etc.,were characterized to correlate with their aromatization performance data.The results showed that the pore structure of Al2O3 could significantly affect the catalyst performance.As the accessible pore diameter of the catalyst increased from 8.0 nm to 9.0 nm,the light aromatics yield increased by 2.7 percentage points,while the operating time of the catalyst nearly doubled.In addition,catalysts prepared with SiO2 and aluminum phosphate was more active and stable than that prepared with Al2O3,of which the light aromatics yield enhanced 6-8 percentage points and the run length,or seivice eife run length nearly doubled.     

Effect of Mixed Oxide Support for Ni/ZnO in Reactive Adsorption Desulfurization

The effect of mixed oxide support on the performance of Ni/ZnO in the reactive adsorption desulfurization(RADS) reaction was investigated in a fixed bed reactor by using thiophene as the sulfur-containing compound in the model gasoline. A series of oxide supports for Ni/ZnO were synthesized by the co-precipitation method and characterized by XRD, N_2-adsorption, TPR and NH_3-TPD techniques. It was found that the desulfurization capacity of Ni/ZnO was enhanced greatly when active components were supported on the proper mixed oxide. Ni/ZnO supported on oxides exhibited much higher desulfurization efficiency and sulfur adsorption capacity than the unsupported Ni/ZnO and the synthesized Ni/ZnO-SA adsorbent exhibited the highest efficiency for thiophene removal. The higher desulfurization activity and sulfur capacity of Ni/ZnO supported on SiO_2-Al_2O_3 with small particle size, high specific surface area and large pore volume could promote the high dispersion of active metal phase and the transfer of sulfur to ZnO with lower mass transfer resistance. γ-Al_2O_3 species could weaken the interaction of active phases and SiO_2 as well as could increase greatly the amount of weak acids. Therefore, these oxides could impose a great influence on the structure and chemical properties of the catalyst.     

Selective Oxidation of PM over Li Doped Potassium Titanate Catalysts

K2Ti2O5 and LixK2-xTi2O5 samples with varying K contents (x=0.125, 0.15, 0.3), targeted on removal of two main environmental pollutants: PM and NOx, were synthesized by the solid state method using TiO2, KNO3 and LiOH·H2O as starting materials and were characterized by X-ray diffractometry, scanning electron microscopy, and BET. The catalytic activity of titanate catalysts on PM oxidation was evaluated using the temperature programmed oxidation (TPO) method. The test results showed that the perovskite structure of K2Ti2O5 was still retained after doping a small amount of Li, and the catalytic performance of LixK2-xTi2O5 had been improved significantly compared with that of K2Ti2O5. Li0.15K1.85Ti2O5 catalyst had the highest catalytic activity with an ignition temperature of 210 ℃ and a peak temperature of 290 ℃. The catalytic activity of both K2Ti2O5 and LixK2-xTi2O5 under intimate contact was higher than that under loose contact. When the exhaust gas flow rate was around 100 mL/min, the catalyst samples showed a highest activity. The Li doped K2Ti2O5 could be an excellent candidate for PM oxidation due to its high oxidation activity, water stability, resistance to sulfur poisoning and economical advantages.     

Reverse Microemulsion Synthesis and Characterization of Pd-Ag Bimetallic Alloy Catalysts Supported on Al2O3 for Acetylene Hydrogenation

Pd-Ag bimetallic alloy nanoparticles were synthesized by the reverse microemulsion method,and then deposited on Al2O3 to form the supported catalyst.The nanoparticles of Pd-Ag and Pd-Ag/Al2O3 samples were characterized by UV/Vis,HRTEM,EDX,XRD,and XPS.The test results indicated that Pd-Ag bimetallic alloy nanoparticles with a size of about 2 nm and a face-centered cubic(fcc) structure were formed in the measured area of microemulsion.The growth of nanoparticles was effectively limited within the droplet of micoremulsion.TEM image exhibited that the Pd-Ag alloy nanoparticles were well-dispersed on the Al2O3 support.The catalytic performance of various catalysts for selective hydrogenation of acetylene showed that a higher acetylene conversion and selectivity to ethylene upon acetylene hydrogenation was achieved on a nano-sized Pd-Ag bimetallic catalyst with a Pd/Ag alloy supported molar ratio of 1:1.5.     

NiO/Ca_2Fe_2O_5催化剂可见光下催化分解水制氢

用溶胶-凝胶方法制备了Ca2Fe2O5,采用浸渍法负载NiO制备了NiO/Ca2Fe2O5催化剂。采用X射线衍射、X射线光电子能谱和紫外-可见光漫反射光谱对催化剂进行了表征。Ca2Fe2O5和NiO/Ca2Fe2O5催化剂对可见光有良好的响应。考察了NiO/Ca2Fe2O5催化剂在可见光下分解水的光催化活性。实验结果表明,负载的NiO可以使光生电子和空穴得到较好的分离;溶液的初始pH对NiO/Ca2Fe2O5催化剂的光催化活性影响显著;NiO/Ca2Fe2O5催化剂光催化分解纯水的氢气生成速率为0.048μmol/(g.h),分解0.272mol/LNaHCO3溶液的氢气生成速率为84.857μmol/(g.h),NaHCO3中的HCO3-促进了光生电子和空穴的分离,从而提高了催化剂的光催化活性。     

Cu-Bi纳米粉体催化剂的表征及其可见光光催化降解甲基橙的研究

以Cu(NO3)2.3H2O,B i(NO3)3.5H2O,CO(NH2)2为原料、聚乙二醇为分散剂,采用均匀共沉淀法制备了Cu-B i纳米粉体催化剂,用X射线粉末衍射、傅里叶变换红外光谱、透射电镜、能量色散法、示差扫描-热重分析和紫外-可见漫反射光谱法对Cu-B i纳米粉体催化剂的组成、粒径大小、表面形貌和光学吸收性能进行了表征,并以甲基橙为目标降解物,考察了所制备的Cu-B i纳米粉体催化剂在可见光下的光催化性能。实验结果表明,Cu-B i为类球形纳米粉体,粒度均匀,粒径约为50nm;在可见光下Cu-B i纳米粉体催化剂对甲基橙具有良好的光催化降解性能,辐照时间4h,甲基橙的脱色率可达80%以上。     

La_2O_3／TiO_2／SO_4~(2-)纳米光催化剂的制备和性能

采用溶胶-凝胶-浸渍法制备了La2O3／TiO2／SO42-纳米光催化剂。采用X射线衍射和BET比表面积测试法对纳米光催化剂的晶型和比表面积进行了表征。以甲基橙溶液为光催化降解反应模型化合物,考察了纳米光催化剂的催化活性。实验结果表明,La2O3的掺杂使TiO2的粒径减小,比表面积增大,La2O3的最佳掺杂量(相对于TiO2的摩尔分数)为1．00％,La2O3／ TiO2(x(La2O3)=1．00％)为纳米光催化剂时,甲基橙的脱色率达到75．8％(光照60min);SO42-的负载也使TiO2的粒径减小, 比表面积增大,浸渍液H2SO4的浓度对纳米光催化剂的催化活性有一定的影响,H2SO4的最佳浓度为0．4 mol／L,TiO2／SO42- (c(H2SO4)=0．4 mol／L)为纳米光催化剂时,甲基橙的脱色率达到83．2％(光照60 min);掺杂La2O3和负载SO42-使TiO2纳米光催化剂的催化活性显著提高,La2O3／TiO2／SO42-(x(La2O3)=1．00％,c(H2SO4)=0．4mol／L)为纳米光催化剂时,甲基橙的脱色率达到91．7％(光照60min)。     

碳纳米管@球形氮化碳核壳结构光催化剂的构筑及其性能

以二氰二胺和三聚氯氰为原料,以碳纳米管 (CNT)为核,采用溶剂热法成功制备了一系列不同CNT质量的可见光响应的碳纳米管@球形氮化碳 (CNT@CNMS) 核壳结构催化剂。采用X射线衍射光谱（XRD）、傅里叶变换红外（FT-IR）、透射电子显微镜（TEM）、紫外可见光谱(UV-vis)、X射线光电子能谱(XPS)、电化学阻抗（EIS）和光致发光光谱（PL）等分析方法对催化剂进行了表征。通过电化学表征计算出CNMS的价带与导带位置。结果表明,CNMS均匀的生长到管状CNT表面,形成CNT@CNMS核壳结构;制备的CNT@CNMS核壳催化剂比表面积增大,且可见光吸收性能明显增强。光催化性能试验表明,当CNT质量为20 mg时,制备的催化剂性能最高,反应120 min,4 - 硝基苯酚的降解率高达54.44%,其降解效果明显高于CNMS。该研究对于采用溶剂热法制备核壳结构基氮化碳催化剂治理油田废水中酚类污染物提供了理论基础。     

掺杂型光催化剂Ag-BiVO_4的制备及其光催化降解含酚废水的研究

研究了掺杂型可见光催化剂Ag-BiVO4的制备及其光催化氧化降解含酚废水的工艺条件。采用水热法制备了Ag-BiVO4,并对其进行X射线衍射、紫外-可见漫反射等手段表征;以含酚废水为降解目标,考察了催化剂前驱体的pH值、催化剂用量和空气流量等工艺条件对降解率的影响,研究了Ag-BiVO4催化剂光催化氧化苯酚的性能。结果表明,Ag的掺杂延伸了BiVO4的可见光吸收范围,吸收边带明显红移,能隙禁带宽窄于纯BiVO4,而Ag的掺杂没有改变BiVO4的晶相,在中性条件下制备的Ag-BiVO4催化剂晶型较完整,可见光催化活性最高。在空气通入量为200mL/min、Ag-BiVO4(pH=7)催化剂加入量为0.5mg/L时,400W金卤灯照射150min,对含酚废水的去除率可达93%。     

AgBr@Ag_3PO_4的制备及其可见光催化降解盐酸莫西沙星的性能

以Ag3PO4为前体,采用超声辅助原位离子交换法制备了AgBr@Ag3PO4光催化剂,并利用XRD,SEM,UV-Vis等方法对其进行了表征。以盐酸莫西沙星(MX)模拟自然水体中的抗菌药物残留,考察了该催化剂在可见光下的光催化性能,探讨了溶液pH、催化剂用量、MX初始浓度及催化剂循环使用次数对AgBr@Ag3PO4光催化性能及降解动力学的影响。研究了AgBr@Ag3PO4在可见光下的光催化反应机理。实验结果表明,AgBr和Ag3PO4形成了简单的物理复合物;AgBr@Ag3PO4对MX具有很强的可见光催化降解活性;在溶液pH=11、MX初始浓度20μmol/L、ρ(AgBr@Ag3PO4)=1.0 g/L的条件下,MX在可见光下照射15 min后,降解率达到97.5%;催化机理研究表明,空穴和.OH是该光催化反应中主要的氧化性物质。     

掺杂改性废催化裂化平衡剂的光催化脱氮性能研究

采用磁搅拌法制备了锶掺杂改性废催化裂化平衡剂,利用XRD、DRS、XPS和SEM等手段对其进行表征,并以模拟含氮油品为目标降解物,在可见光下评价其光催化脱氮性能。结果表明,锶掺杂废催化裂化平衡剂对模拟油品中的吡啶表现出良好的可见光脱氮效果。当Sr掺杂浓度为0.5mol/L,催化剂用量为0.05g,焙烧温度为400℃,焙烧时间5h,在可见光下光照2.5h,对质量浓度为100 ug/g的模拟油品的脱氮率可达92.0%。     

碘掺杂g-C3N4光催化剂的制备及催化性能

采用热聚合法,以尿素为前驱体,碘化氨为掺杂剂,制备出不同碘离子掺杂量的可见光催化剂石墨相氮化碳（g C3N4）。对碘掺杂g C3N4催化剂（Ix C3N4）进行X射线衍射（XRD）、扫描电镜（SEM）、透射电镜（TEM）、傅里叶变换红外光谱（FT IR）、X光电子能谱（XPS）、紫外 可见漫反射（UV Vis）、N2吸附、电子荧光光谱（PL）、电化学阻抗（EIS）等表征,分析了催化剂的形貌、结构、光学和电学性能。以4 硝基苯酚为目标污染物进行光催化降解实验,选取最佳碘掺杂量的I002 C3N4催化剂进行重复性实验。结果表明,碘离子的引入没有改变g C3N4的原始形貌和结构,掺杂后的样品拓宽了g C3N4对可见光的吸收范围,降低了光生电子 空穴对的复合率;掺杂最佳碘离子量的催化剂I002 C3N4在2 h内对4 硝基苯酚的降解率达到84%,重复4次实验后,降解率仍能达到80%。     

水滑石类化合物-氧化铈催化剂的制备及其光降解甲基橙的性能研究

采用共沉淀法制备了LDHs-CeO2(LDHs为水滑石类化合物)催化剂,并将其用于光催化降解甲基橙溶液,考察了催化剂的原料配比、反应时间、甲基橙初始含量、甲基橙溶液的pH和催化剂用量对甲基橙降解率的影响;同时采用FTIR,XRD,SEM,TEM,EDS,TG等方法对催化剂进行了表征。实验结果表明,n(Mg)∶n(Al)∶n(Ce)=2∶1∶0.50的LDHs-CeO2催化剂活性最高,用该催化剂光催化降解甲基橙溶液的适宜条件为:250 mL甲基橙溶液,甲基橙初始质量浓度40 mg/L,pH=5,反应时间80 min(暗处静置20 min,光照时间60 min),催化剂用量0.3 g;在此条件下,甲基橙降解率达到98.69%。表征结果显示,LDHs-CeO2晶相单一,晶体结构一致,结晶度好,属于六方晶系,形貌为规则的片状结构,分散性较好。