甲醇水蒸汽重整制氢Au/TiO2催化剂

采用沉积-沉淀法制备了一系列Au/TiO2催化剂,考察了Au负载量、焙烧温度以及助剂等因素对甲醇水蒸汽重整制氢反应催化性能的影响;并利用XRD, TEM对催化剂进行了表征. 结果表明,制备条件对催化性能有明显影响;Au负载量为5%(w)时所得催化剂活性较好;助剂NiO可使催化剂催化甲醇水重整的催化活性明显提高;100℃烘干未焙烧制得的催化剂活性最好;TEM结果显示,NiO的加入使载体TiO2颗粒分散度提高,Au粒粒度变小.     

Pt/TiO_2光催化制氢的初步研究

对无氧条件下Pt/TiO_2光催化重整甲醇制氢的基本步骤进行简化,在同一体系中进行了光催化剂的合成和光催化制氢的两步反应。基于正交设计法对该复杂体系进行了分析,得到Pt载量、甲醇/水体积、灯距、前反应时间这4种影响因素的3个不同水平对放氢速率的影响。确定了最佳实验条件为Pt载量0.5％(mol)、甲醇/水体积比5:1、灯距12 cm、前反应时间3h。分析结果表明,Pt载量对放氢速率的影响最大。实验获得的最高放氢速率为5.84 ml·h~(-1)·g~(-1)。     

Au/La2O3/TiO2催化甲醇水蒸汽重整制氢

用沉积-沉淀法制备了Au/La2O3/TiO2催化剂,考察了制备条件和反应条件对催化剂活性的影响,并利用X射线衍射(XRD)、透射电子显微镜(TEM)等测试手段对催化剂进行了表征. 结果表明La2O3的加入可使催化剂催化甲醇水重整的催化活性明显提高,且明显降低产物气体中CO和CH4的含量,使氢气选择性明显增加. 当nH2O/nCH3OH=1.0、液体进料空速WHSV=3.42 h-1、反应温度为275℃时,Au/La2O3/TiO2催化剂催化甲醇水蒸汽重整制氢反应的效果最佳.     

Pt/TiO2上的污染物降解耦合光解水制氢研究

以三乙胺和乙醚为目标污染物,研究了Pt/TiO₂上光催化分解水产氢和污染物同时降解的光催化反应。研究了作为电子给体的污染物浓度对光解水制氢反应的影响,污染物本身的降解规律符合Langmuir-Hinshelwood准一级动力学方程。使用拉曼光谱仪和紫外-可见光分光光度计对降解产物浓度进行了表征,讨论了可能的降解反应机理。     

二甲醚水蒸气重整制氢复合催化体系研究进展

1二甲醚与甲醇重整制氢的比较优势近年来,为应对日益严峻的能源危机和环境污染,氢作为一种绿色能源受到世界各国的广泛关注。氢燃烧只产生水,具有能量密度高、无污染等优点,但其运输和储存尚存在问题。甲醇重整制氢能有效地解决氢的运输和储存等问题,技术也非常成熟,但甲醇的毒性较大,一旦泄漏将对人体和环境造成很大的影响,而且需要修建重整制氢的基础设施。     

非贵金属M/TiO2催化剂上甲烷和二氧化碳光催化干重整制氢

以TiO2为载体,通过正交设计,采用浸渍法制备了Ni、Co和Cu等非贵金属负载型催化剂,进行CH4和CO2光催化干重整制氢活性评价,并采用TPR、XRD、FT-IR和BET对催化剂的氧化还原性、晶体结构和织构特征进行表征.结果表明,在600℃焙烧的9％Ni/TiO2催化剂上于750℃反应40 min,CH4转化率和H2...     

二甲醚水蒸汽重整制氢反应平衡组成模拟计算

对比了二甲醚水蒸汽重整过程中由外部供热和燃烧反应尾气供热两种方式下的热效率,并对体系进行了热力学分析,模拟考察了反应温度、压力、原料组成等因素对体系平衡组成的影响,探讨了二甲醚转化率、氢气和一氧化碳等产物的变化情况.分析发现,反应器温度在200 ℃,压力为0.1 MPa时可以获得最佳的原料转化率.研究认为二甲醚水蒸气重整制氢的副产物甲烷可显著降低氢气的含量,一氧化碳在高温、低水/二甲醚进料比的情况下产生.催化剂应具有选择性催化功能,同时应具有低温高活性.     

二甲醚在Pt系催化剂上的电氧化行为初探

本实验用化学浸渍-还原法,甲醛为还原剂制备直接二甲醚燃料电池阳极催化剂。用循环伏安法和稳态极化法,采用粉末微电极技术,研究二甲醚在自制Pt／C、PtSn／C和PtRu／C催化剂上的氧化行为。研究结果显示,二甲醚在PtRu／C上有较佳的反应活性。在PtRu／C催化剂上考察温度对于二甲醚电氧化的催化活性的影响,得出温度的升高有利于二甲醚电氧化的进行。     

Pt/Al_2O_3与Pt/MgO-Al_2O_3催化剂制备及其催化氢能载体甲基环己烷脱氢反应性能

以碱共沉淀法制备Mg-Al水滑石,然后采用浸渍法负载活性组分Pt,经焙烧、氢气还原得到Pt/Al_2O_3与Pt/Mg O-Al_2O_3催化剂,采用XRD、N2吸附-脱附、FT-IR、H2-TPR和Py-IR等分析Mg O的加入对Pt/Al_2O_3催化剂结构性能的影响,并在甲基环己烷连续脱氢反应中对比两种催化剂活性。结果表明,Pt/Mg O-Al_2O_3催化剂比表面积小于Pt/Al_2O_3催化剂,且表面基本无酸性活性中心,但表现出与Pt/Al_2O_3催化剂相同的脱氢活性。在Pt负载质量分数2%、催化剂用量0.5 g、甲基环己烷0.1 m L·min-1纯样进料和325℃反应10 h后,原料平均转化率79.9%,脱氢产物只有甲苯,对应的产氢速率192.8 mmol·(g-metal·min)-1,表现出优良的脱氢活性。     

Hydrogen production from partial oxidation and reforming of DME

Hydrogen production from partial oxidation and reforming of dimethyl ether (DME) was investigated with a fixed bed continuous-flow reactor. H₂ yield of over 90% was obtained with 100% DME conversion at 700 °C over Pt/Al₂O₃+Ni–MgO dual catalyst bed, while keeping CH₄ yield at low level. Such results indicated that partial oxidation and reforming of DME to produce hydrogen at high temperature is possible and effective.     

空气气氛下RuO2/ZSM-5催化醇的部分氧化反应

通过原位反应法制备了RuO₂/ZSM-5催化剂，并用XRD、XPS和TEM对合成的催化剂进行了表征，结果表明，RuO₂主要以20 nm左右的微晶分散在载体中，原位反应引入钌物种，没有改变载体ZSM-5的结构，大部分钌为四价。催化试验表明，在以空气为氧化剂的温和条件下，RuO₂/ZSM-5不仅可有效地催化芳香醇和带烯丙基的醇类（激活醇）氧化生成醛酮，而且对一些非激活醇也有较好的催化效果。     

M/γ-Al2O3催化剂对煤油水重整制氢的影响

以γ-Al₂O₃为载体,采用等体积分步浸渍法制备了以Ni为活性组分,La、Ce、Fe、Cr、Co为助剂的催化剂M/γ-Al₂O₃,在固定床管式反应器中研究了M/γ-Al₂O₃催化剂的性能,考察了反应温度、水碳比和空速对氢产率的影响,并对催化剂进行XRD、SEM和BET表征。结果表明,NiLaCeFeCrCo/γ-Al₂O₃催化剂具有较好的催化性能,在反应温度700 ℃、水碳物质的量比10和空速6 min^-1的条件下,氢产率达到27.335 mol·mol^-1,并在300 min内表现出较好的活性,平均氢产率为21.966 mol·mol^-1。     

H2 production through steam reforming of ethanol over Pt/ZrO2, Pt/CeO2 and Pt/CeZrO2 catalysts

The effect of the support nature and metal dispersion on the performance of Pt catalysts during steam reforming of ethanol was studied. H₂ and CO production was facilitated over Pt/CeO₂ and Pt/CeZrO₂, whereas the acetaldehyde and ethene formation was favored on Pt/ZrO₂. According to the reaction mechanism, determined by temperature-programmed desorption (TPD) and Diffuse Reflectance Infrared Spectroscopy (DRIFTS) analysis, some reaction pathways are favored depending on the support nature, which can explain the differences observed on the resulting product distribution.     

H2气氛中TiOx的形成及其对Ni/TiO2催化剂顺酐液相加氢性能的影响

采用等体积浸渍法制备了Ni/TiO₂催化剂,利用N₂物理吸附、H₂-TPR、XRD、H₂-TPD及CO-TPSR等表征手段研究H₂气氛中随着热处理温度升高,Ni/TiO₂催化剂结构和织构变化规律,并考察催化剂的顺酐液相加氢性能。研究表明,随着热处理温度的升高,催化剂C-C键加氢活性逐渐增高,而CO加氢活性先增高后降低。产生这一现象的原因与TiO_x物种随H₂气氛中热处理温度的升高而逐渐增多有关。     

Effects of microwaves on selective oxidation of toluene to benzoic acid over a V2O5/TiO2 system

Two series of catalysts, V₂O₅/TiO₂ and modified V₂O₅/TiO₂, were prepared with a conventional impregnation method. They were tested in the selective oxidation of toluene to benzoic acid under microwave irradiation. The reaction conditions were optimized over V₂O₅/TiO₂. It was found that in the microwave catalytic process the optimum reactor bed temperature of the titled reaction decreases to 500 K (600 K in the conventional process). The modification of V₂O₅/TiO₂ with MoO₃, WO₃, Nb₂O₅ or Ta₂O₅, which has no negative influence on the reaction in the conventional catalytic process, can greatly promote the catalytic activities in the microwave process, leading to a high yield of benzoic acid (41%). The effects of microwave electromagnetic field on the catalysts are discussed.     

Catalytic oxidation of naphthalene using a Pt/Al2O3 catalyst

Polycylic aromatic hydrocarbons (PAHs) are listed as carcinogenic and mutagenic priority pollutants, belonging to the environmental endocrine disrupters. Most PAHs in the environment stem from the atmospheric deposition and diesel emission. Consequently, the elimination of PAHs in the off-gases is one of the priority and emerging challenges. Catalytic oxidation has been widely used in the destruction of organic compounds due to its high efficiency (or conversion of reactants), its economic benefits and good applicability.

This study investigates the application of the catalytic oxidation using Pt/γ-Al₂O₃ catalysts to decompose PAHs and taking naphthalene (the simplest and least toxic PAH) as a target compound. It studies the relationships between conversion, operating parameters and relevant factors such as treatment temperatures, catalyst sizes and space velocities. Also, a related reaction kinetic expression is proposed to provide a simplified expression of the relevant kinetic parameters.

The results indicate that the Pt/γ-Al₂O₃ catalyst used accelerates the reaction rate of the decomposition of naphthalene and decreases the reaction temperature. A high conversion (over 95%) can be achieved at a moderate reaction temperature of 480 K and space velocity below 35,000 h⁻¹. Non-catalytic (thermal) oxidation achieves the same conversion at a temperature beyond 1000 K. The results also indicate that Rideal–Eley mechanism and Arrhenius equation can be reasonably applied to describe the data by using the pseudo-first-order reaction kinetic equation with activation energy of 149.97 kJ/mol and frequency factor equal to 3.26 × 10¹⁷ s⁻¹.     

TiO2-SiO2 and V2O5/TiO2-SiO2 catalyst: Physico-chemical characteristics and catalytic behavior in selective catalytic reduction of NO by NH3

TiO₂-SiO₂ with various compositions prepared by the coprecipitation method and vanadia loaded on TiO₂-SiO₂ were investigated with respect to their physico-chemical characteristics and catalytic behavior in SCR of NO by NH₃ and in the undesired oxidation of SO₂ to SO₃, using BET, XRD, XPS, NH₃-TPD, acidity measurement by the titration method and activity test. TiO₂-SiO₂, compared with pure TiO₂, exhibits a remarkably stronger acidity, a higher BET surface area, a lower crystallinity of anatase titania and results in allowing a good thermal stability and a higher vanadia dispersion on the support up to high loadings of 15 wt% V₂O₅. The SCR activity and N₂ selectivity are found to be more excellent over vanadia loaded on TiO₂-SiO₂ with 10–20 mol% of SiO₂ than over that on pure TiO₂, and this is considered to be associated with highly dispersed vanadia on the supports and large amounts of NH₃ adsorbed on the catalysts. With increasing SiO₂ content, the remarkable activity decrease in the oxidation of SO₂ to SO₃, favorable for industrial SCR catalysts, was also observed, strongly depending on the existence of vanadium species of the oxidation state close to V⁴⁺ on TiO₂-SiO₂, while V⁵⁺ exists on TiO₂, according to XPS. It is concluded that vanadia loaded on Ti-rich TiO₂-SiO₂ with low SiO₂ content is suitable as SCR catalysts for sulfur-containing exhaust gases due to showing not only the excellent de-NO_x activity but also the low SO₂ oxidation performance.