[C2OHMIM]+Cl－离子液体-水体系中纳米TiO2的合成及光催化性能

 采用[C₂OHMIM]⁺Cl^-离子液体 水体系混合加热法制备了纳米 TiO₂光催化剂,应用 XRD、SEM 和 UV-Vis 手段对其进行了表征,考察了体系中[C₂OHMIM]⁺Cl^-质量分数、反应时间和反应温度对所制备的纳米 TiO2的颗粒结构、形貌及光催化活性的影响。结果表明,由此法得到的 TiO₂均为金红石相,由纳米晶小颗粒堆积起来的球形颗粒组成。当[C₂OHMIM]⁺Cl^-质量分数为66.6%、反应温度150℃、反应时间24 h 时,制备所得 TiO₂的光催化活性好,对罗丹明B的降解率高达96%。     

Pd/Al2O3-TiO2催化剂的制备条件

 以含K₂O的Al₂O₃-TiO₂复合物为催化剂载体,考察了浸渍液pH值、浸渍液浓度、浸渍时间和焙烧温度对Pd/Al₂O₃-TiO₂催化剂颗粒的蛋壳厚度、Pd粒子粒径等的影响。采用BET、TEM等方法对所制备的催化剂进行了表征,选择较佳制备条件的Pd/Al₂O₃-TiO₂催化剂进行了C₄馏分选择加氢活性评价。结果表明,随着浸渍液pH值的减小,催化剂颗粒的蛋壳厚度增加;浸渍溶液的浓度越高,浸渍时间越长,越有利于金属在催化剂内层的分布;浸渍液的pH值并不会影响Pd/Al₂O₃-TiO₂催化剂Pd粒子最终的大小。催化剂焙烧温度越高,Pd粒子的平均直径越大,Pd的分散度越小。在反应温度40℃、压力1.5 MPa、体积空速8.0 h^-1、氢/炔摩尔比2.5的条件下,较佳制备条件的Pd/Al₂O₃-TiO₂催化剂催化C₄馏分加氢的炔烃转化率73%、丁二烯选择性85%、丁二烯损失率2.5%。     

负载型 Co/BiVO4催化剂的制备及其光催化脱氮性能

 采用水热法制备 BiVO₄,再采用浸渍水热法和浸渍焙烧法制备负载型 Co/BiVO₄。考察了 Co 负载量、焙烧温度和焙烧时间对 Co/BiVO₄晶体结构的影响,并采用X射线衍射、紫外-可见吸收光谱、热重-差热分析等方法对 BiVO₄和 Co/BiVO₄进行表征。将 Co/BiVO₄催化剂用于可见光催化模拟油脱除有机碱性氮,考察催化剂制备条件对 Co/BiVO₄光催化脱氮活性的影响。结果表明,在 Co 负载量为5%、400℃下焙烧1 h 的浸渍焙烧法得到的 Co/BiVO₄催化剂的光催化脱氮活性最高,含吡啶氮模拟油的光催化脱氮率达到83.59%。     

ZrO2对Cu/Al2O3-ZrO2催化剂糠醛选择加氢活性的影响

 采用共沉淀法制备了Al₂O₃-ZrO₂复合氧化物,并以它为载体,浸渍法制备Cu 质量分数为24%的负载型Cu 基催化剂。运用X射线衍射(XRD)、H₂程序升温还原(H₂-TPR)、X射线能谱(XPS)对载体和催化剂进行表征,并考察了ZrO₂对Cu/Al₂O₃-ZrO₂催化剂糠醛选择加氢活性的影响。结果表明,载体中ZrO₂质量分数20%的Cu/Al₂O₃-ZrO₂催化剂对糠醛的选择加氢活性最高。与Cu/Al₂O₃催化剂相比,添加ZrO₂可以提高Cu/Al₂O₃-ZrO₂催化剂加氢活性,并有效提高较高反应温度下的糠醇选择性。     

Fe3O4纳米封堵剂的制备、表征及封堵性能

通过热分解法制备了Fe₃O₄纳米封堵剂,利用傅里叶转换红外光谱（FT-IR）仪、X-射线衍射（XRD）仪、透射电镜对所制备的Fe₃O₄纳米粒子进行了结构表征,考察了Fe₃O₄在不同盐度NaCl溶液中稳定性及超声时间对Fe₃O₄纳米粒子在不同盐度NaCl溶液中分散稳定性的影响,并进行了人造泥饼模拟封堵实验。实验结果表明,Fe₃O₄纳米封堵剂最佳反应温度为200℃,最佳反应时间为2 h。FT-IR分析表明聚乙二醇修饰在纳米粒子表面,XRD分析表明所制备的Fe₃O₄纳米粒子属于立方晶相,TEM分析表明所制备的Fe₃O₄纳米粒子粒径在9.5 nm左右。超声0.5 h后的所制备的Fe₃O₄纳米粒子的耐盐分散性能最好。人造泥饼模拟实验结果表明,加入100 mL 质量分数为3%的Fe₃O₄纳米粒子水分散液,3.5 MPa压力下,7200 s后的滤失量只有11.3 mL,说明该纳米封堵剂堵水效果显著,是一种性能优异的纳米封堵材料。     

硫酸铝法制备的ZrO2-Al2O3的孔结构和表面性质

 在NaAlO₂-Al₂(SO₄)₃法制备拟薄水铝石成胶过程中加入氧氯化锆, 得到ZrO₂-Al₂O₃样品。采用XRD、BET、SEM、Py-IR、NH₃-TPD方法对ZrO₂-Al₂O₃样品进行了表征。结果表明,ZrO₂质量分数小于5.6%时, ZrO₂-Al₂O₃样品的晶相为γ-Al₂O₃,当ZrO₂质量分数大于5.6%时,出现了t-ZrO₂的晶相;随着ZrO₂含量的增加_,样品的比表面积逐渐减小;ZrO₂质量分数从0增至6.6%,孔容从1.12cm³/g到1.17cm³/g,变化不大,随ZrO₂质量分数的增加,孔容开始下降;平均孔径随着ZrO₂质量分数的增加而逐渐增加,ZrO₂质量分数达到7.4%以后,随着ZrO₂质量分数的增加,孔径减小。ZrO₂的加入对γ-Al₂O₃的孔型结构没有影响。ZrO₂-Al₂O₃样品主要以L酸为主,有少量的B酸;随着ZrO₂含量的增加,总酸量略有增加,其中弱酸比例降低,而强酸和中强酸的比例提高。     

MoO3-WO3/TiO2-SiO2催化剂对正庚烷异构化的催化性能

 采用溶胶-凝胶法制备了TiO₂-SiO₂复合氧化物载体,浸渍法制备了MoO₃-WO₃/TiO₂-SiO₂催化剂,通过XRD、BET表征了催化剂的物化性质,并在连续流动固定床反应器上考察了MoO₃-WO₃/TiO₂-SiO₂催化正庚烷临氢异构化反应性能,讨论了催化剂制备条件和反应条件对其正庚烷异构化催化性能的影响。结果表明,当 w(MoO₃)=5%、w(WO₃)=15%、w(TiO₂)=80%、w(SiO₂)=20%、焙烧温度773 K、还原温度723 K、反应温度553 K、还原时间6 h 时,MoO₃-WO₃/TiO₂-SiO₂催化剂对正庚烷异构化反应表现出最高催化活性,此时正庚烷转化率可达23.12%, 异庚烷选择性可达77.32%。     

MoO3/Al2O3介孔催化剂在柴油氧化脱硫中的应用

 通过溶胶-凝胶法,以硝酸铝为铝源、蔗糖为模板剂、氨水为沉淀剂,制备了介孔 Al₂O₃,并以其为载体,等体积浸渍法制备了MoO₃/Al₂O₃介孔催化剂。采用 N₂吸附-脱附及X射线衍射对介孔 Al₂O₃和 MoO₃/Al₂O₃催化剂进行了表征。将 MoO₃/Al₂O₃催化剂用于柴油催化氧化脱硫,以 H₂O₂为氧化剂,探讨了 MoO₃负载量以及 H₂O₂用量对其催化柴油氧化脱硫的影响。结果表明,自制的 Al₂O₃载体为具有介孔结构的 γ-Al₂O₃,其比表面积、孔容、平均孔径分别为304.3 m²/g、 0.467 cm³/g 和6.14 nm。MoO₃负载量为20%(质量分数)、H₂O₂与柴油中硫的摩尔比为12、氧化温度为60℃时,柴油的氧化脱硫效果较佳,脱硫率为68.4%。     

复合SiO2-WO3催化剂的制备、表征及氧化脱除苯并噻吩性能

 采用溶胶-凝胶法制备了SiO₂-WO₃催化剂,并采用XRD、FT-IR、BET、TG-DTA等方法对催化剂进行表征。以苯并噻吩(BT)为模型化合物,H₂O₂为氧化剂,考察了催化剂的活性元素、制备方法、n(W)/n(Si)和焙烧温度对其催化氧化脱硫活性的影响。结果表明,W的引入降低了SiO₂的比表面积,SiO₂-WO₃催化剂中W的主物相为WO₃。在以W为活性组元,且n(W)/n(Si)为0.1时,500℃焙烧得到的SiO₂-0.1WO₃催化剂具有最好的催化脱硫活性。在模拟油20 mL、催化剂SiO₂-0.1WO₃用量0.04 g、n(H₂O₂)/n(S)为15.9、乙腈/模拟油体积比0.3、65℃反应60 min的条件下,苯并噻吩模拟油脱硫率可达99.3%。     

Co掺杂对CuO/ CeO2-Co3O4优先氧化CO催化性能的影响

采用共沉淀-浸渍法制备了一系列不同Ce/Co物质的量比的CeO₂-Co₃O₄载体和CuO负载量(质量分数)为7% 的CuO/CeO₂-Co₃O₄催化剂,考察了它们在富氢气氛中对CO的优先氧化性能。采用BET、XRD、H₂-TPR等对催化剂进行了表征。测试结果表明:Ce/(Co+Ce)物质的量比为0.9时,CuO/ CeO₂-Co₃O₄催化剂活性最好。少量的Co掺杂有利于提高催化剂的比表面积和铜物种在载体上的分散,少量的Co进入了CeO₂的晶格,增强了钴铈相互作用,进而提高了载体的氧化还原性能。      

A novel La3+–Zn2+–Al3+–MoO42− layered double hydroxides photocatalyst for the decomposition of dibenzothiophene in diesel oil

A new type of photocatalyst, La³⁺-Zn²⁺-Al³⁺-MoO₄^2? layered double hydroxide (LDH) (La:Zn:Al = 1:7:2), was prepared by a complexing agent-assisted homogeneous precipitation technique. The LDHs were used as catalysts for the desulfurization of diesel oil under UV irradiation. As revealed by the results, the catalyst showed superior desulfurization efficiency and recycling performance. Under UV irradiation, the desulfurization efficiency was 84% in 60 min. In La³⁺–Zn²⁺–Al³⁺–MoO₄^2? LDHs, the introduction of MoO₄^2? increased the interlayer space for promoting the adsorption of dibenzothiophene, and MoO₄^2? might act as the active sites for the oxidation of dibenzothiophene, resulting in the high desulfurization efficiency.     

Surface Properties and Reactivity of Iron-Doped Titanium Oxides Catalysts in Oxidative Dehydrogenation of Ethylbenzene with CO2

Abstract

The effect of Fe³⁺ doping level on the surface properties and catalytic performance of a series of iron-doped titanium oxide catalysts (1–7 mol% Fe³⁺) prepared using an acid-catalyzed sol-gel method was investigated in oxidative dehydrogenation of ethylbenzene with CO₂. The characterization of catalysts was carried out by means of x-ray powder diffraction (XRD), temperature programmed reduction (TPR), and the method of Brunauer, Emmett, and Teller (BET). It was found that the capacity of isolated Fe³⁺ centers in titania matrix is responsible for the catalytic performance; the catalysts exhibit the best activity at the loading level of Fe³⁺, about 3 mol%. In addition, it was shown that the appropriate pore size of the catalysts ranges from 5 nm to 25 nm; the selectivity to styrene increases with an increase in the specific surface area of the appropriate pores.     

Design of Catalyst Support for Deep Hydrodesulfurization of Gas Oil

Abstract

Alumina-silica (Al₂O₃-SiO₂) composite supports were examined to find the optimum state of support (i.e., composition and morphology). SiO₂ content in the Al₂O₃-SiO₂ support induced a shift of the main peak to higher frequency ascribed to an increased amount of Mo₈O₂₆ ^4?. A 75 wt% Al₂O₃-25 wt% SiO₂ support had homogeneously dispersed alumina particles of smaller size with high crystallinity. Hydrodesulfurization (HDS) of straight-run gas oil and its conventionally hydrotreated straight-run gas oil was performed over NiMo sulfides supported on Al₂O₃-SiO₂ composites. The high crystallinity of NMASA2-27 may be related to the high HDS and hydrogenation activity of NiMo sulfides due to its moderate interaction with the alumina surface.     

Effects of low-salinity water coupled with silica nanoparticles on wettability alteration of dolomite at reservoir temperature

Wettability alteration in porous media is one of the mechanisms for enhancing oil recovery through injecting low-salinity water into carbonate reservoirs, in which active ions can remove the carboxylic oil component from the rock surface, altering the rock's wettability toward a water-wet condition. This study investigated the concomitant effects of low-salinity water and hydrophilic SiO₂ nanoparticles on oil-wet dolomite rock. Results revealed that low-salinity water coupled with hydrophilic nano-SiO₂ in oil-wet dolomite rock remarkably affected the wettability alteration of the rock, showing that the simultaneous presence of ions in water and hydrophilic nano-SiO₂ led to considerable wettability alteration compared with using just low-salinity water.     

Pt/SO42-/ZrO2-Al2O3在正己烷异构化反应中的催化行为

采用连续流动的固定床微反装置考察了Pt/SO24-/ZrO2-Al2O3(PSZA)在正己烷异构化反应中的催化行为。采用NH3-TPD、H2-TPR及TG表征了催化剂的酸性、还原性能及硫物种含量。结果表明,PSZA的初始异构化催化活性几乎不受反应温度的影响,而稳定性则与反应温度密切相关。低温下反应,催化剂在短时间内迅速失活,而提高反应温度可大大提高PSZA的反应稳定性。PSZA具有良好的再生性能,与新鲜催化剂相比,多次再生后的催化剂异构化催化活性基本没有变化。PSZA在低温下的快速失活与其催化活性中心产生的机理有关,而与其硫损失或硫物种的还原无关。在异构化反应过程中,催化剂通过氢溢流可产生强酸活性中心,并在反应过程中不断被消耗;在高温下通过氢溢流不断产生新的强酸中心,使催化活性保持稳定;而低温下氢溢流难以发生,消耗的强酸活性中心不能及时补充,使催化活性下降。     

硫化行为对Ni2P/SBA-15催化剂结构和加氢脱硫性能的影响

以介孔分子筛SBA-15为载体、硝酸镍为镍源、磷酸氢二铵为磷源,等体积浸渍法制备了Ni2P/SBA-15催化剂前驱体,然后在H2流中程序升温还原,得到Ni2P/SBA-15催化剂,再用CS2溶液对催化剂进行了硫化处理,制备出了硫化态xCS2-Ni2P/SBA-15催化剂。采用XRD、N2吸附-脱附、XPS对催化剂的结构进行了表征,对催化剂的二苯并噻吩加氢脱硫活性进行了评价,考察了硫化条件对催化剂结构和二苯并噻吩加氢脱硫催化活性的影响。结果表明,xCS2-Ni2P/SBA-15催化剂的物相有Ni2P、Ni12P5、Ni3S2,催化剂的比表面积随硫化溶液中CS2质量分数的增加有一定程度的增加,催化剂表面的Ni以Niδ+和Ni 2+形式存在,P以Pδ-和P5+形式存在。采用5%CS2硫化溶液硫化的催化剂对二苯并噻吩加氢脱硫具有最高的催化活性,380℃时二苯并噻吩的转化率可达99.3%。硫化过程形成的Ni3S2活性物相对二苯并噻吩的转化和直接脱硫都有利。     

Production of Lubricating Base Oil Using a Moist SiO2/γ-Al2 O3 Catalyst

Abstract

The catalyst SiO₂/γ-Al₂ O₃ treated by micro-wetness air to produce lubricating base oil was studied in this article. The satisfactory reaction temperature, the treatment temperature, and the proper content of active composition was researched. Under the best reaction conditions with a reaction temperature of 170°C, a reaction pressure at 6.0 Mpa, the volume velocity at 0.5 h^?1. The polymerization of α-olefin was performed at a microreactor and produced lubricating base oil with the kinetic viscosity at 38.19 mm² · s^?1, the bromine number at 5.78 g(Br) · (100 g)^?1, and the pour point at ?43.0°C. Then the structure of the catalyst was determined by Brunauer, Emmett and Teller (BET) technology. The result shows that when the optimal micro-wetness air was 45°C, the reaction temperature was 800°C, and the amount of active composition was 12%, and the catalyst has high catalytic activity and wide market prospect.     

Conditions for nonhydrodewaxing reaction of hydrocracking tail oil

Hydrocracking tail oil is used in hydrogenation modification in the hydrocracking process and is an ideal material to produce lube-based oil. Through investigating the effect of operation conditions on properties of dewaxing products under atmospheric pressure, the optimum operation conditions are that reaction temperature is 360°C, volume space velocity is 1.0 h^?1, and distillation temperature is 140°C. Under the optimum condition, the yield of liquid products is higher, and the flash point, pour point, and viscosity of white oil are stable and meet the factory product requirements. Especially, properties of alkane and white oil change little when reaction time is 20 h, which indicates that HZSM-5/Al₂O₃ has better stability. When HZSM-5 molecular sieve catalyst was loaded by pseudo-boehmite, HZSM-5/Al₂O₃ catalyst activity and stability improved and became more beneficial to nonhydrodewaxing reaction of hydrocracking tail oil.     

Dibenzothiophene Hydrodesulfurization Activity of MoS2 Supported in Sol–Gel ZrO2–TiO2 Mixed Oxides

Abstract

In this work, we report the effect of support composition on the properties of MoS₂ impregnated in sol–gel ZrO₂–TiO₂ mixed oxides as dibenzothiophene hydrodesulfurization catalyst. The supports calcined at 500°C were characterized by N₂ physisorption and X-ray diffraction (electronic radial distribution function). The oxidic impregnated materials (2.8 Mo atoms/nm²) were sulfided at 400°C under a H₂S/H₂ stream. The sample impregnated on the equimolar support showed the highest activity per mass of catalysts whereas the one with TiO₂ carrier was superior in a per mass of Mo basis. Marked differences in products selectivity were observed by TiO₂ addition in the supports. The hydrodesulfurization route to partially hydrogenated compounds was favored over the mixed oxides-supported catalysts meanwhile the direct desulfurization (to biphenyl) was promoted on the ZrO₂-supported solid. It is suggested that among other properties the dispersion and morphology of the MoS₂ phase could influence that behavior.     

Magnetically Recyclable Cufe2o4 Nanoparticles as an Efficient and Reusable Catalyst for the Green Synthesis of 2,4,6,8,10,12-Hexabenzyl-2,4,6,8,10,12-hexaazaisowurtzitane as CL-20 Explosive Precursor

Magnetic nanoparticles of copper ferrite (CuFe₂O₄ MNPs) have been simply prepared and applied as an efficient recyclable and reusable catalyst for the green synthesis of 2,4,6,8,10,12-hexabenzyl-2,4,6,8,10,12-hexaazatetracyclo[5.5.0.0^5,9.0^3,11]dodecane (HBIW). The structure of the synthesized pure HBIW (recrystallization from ethanol) was confirmed by using various spectral techniques like infrared (IR), ¹H-NMR, ¹³C-NMR and some of its physical properties. The prepared catalyst was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), and Fourier transform infrared (FTIR). In addition, CuFe₂O₄ MNPs could be reused up to seven runs without any significant loss of activity. Finally, the remarkable advantages of this method are the simple experimental procedure, shorter reaction times, simple workup, and green aspects by avoiding toxic catalysts and high yield of product.