Na改性Pt/Al OOH对甲醛催化氧化反应活性的影响

具有晶面取向的阳极氧化Al OOH因其低温甲醛催化性能而被用于催化氧化甲醛体系。为丰富Al OOH表面羟基含量,采用Na_2CO_3为Na前体浸渍法改性载体,制备不同Na含量(0.13%、0.19%、0.30%、0.41%,质量分数)的Pt/Na_x/Al OOH催化剂。通过BET、FTIR、XPS、HRTEM等表征分析,发现加入Na后,Na/Al OOH的表面羟基更加丰富,Pt/Na_x/AlOOH催化剂的比表面积增大,拥有更小的Pt颗粒尺寸,表面Pt颗粒分散度提高,Pt0元素价态含量增加。当Na含量为0.41%时,催化剂Pt/0.41Na/AlOOH的Pt分散度高达56%。实验结果证明,Pt/0.41Na/AlOOH展现出最优的HCHO催化活性,60℃时HCHO转化率达100%。     

Pt/MnOx-FeOy催化氧化甲醛的性能研究

以MnOx-FeOy为载体,采用浸渍法负载不同质量分数的Pt,制备了一系列x％Pt/MnOx-FeOy催化剂(x=0.1％、0.3％、0.5％,质量分数),考察了Pt质量分数对催化剂催化氧化甲醛性能的影响.当Pt质量分数为0.3％时,0.3％Pt/MnOx-FeOy催化剂性能最优,在60℃可将甲醛完全转化成H2O和CO...     

Pt/MORn-H6催化剂上甲醛室温催化氧化性能

甲醛(HCHO)是室内环境中主要的空气污染物之一,严重影响室内环境空气质量。如何在室温下消除甲醛,是一个亟待解决的问题。在吸附、光催化、等离子体技术和催化氧化等甲醛去除方法中,催化氧化法可以在室温下选择性地将HCHO分解成CO_2和H_2O,因此,实验以天然丝光沸石为载体,研究了经6mol·L~(-1)硝酸处理后的系列Pt/MORn-H6在室温下完全脱除甲醛的性能。采用X射线衍射(XRD)、透射电镜图像(TEM)、X射线光电子能谱仪(XPS)等表征进行分析,结果表明,300℃焙烧的0.5%Pt/MORn-H6具有较好的催化稳定性,Pt颗粒粒径小,且催化活性较高。采用w=2.0%Na~+作为Pt/MORn-H6的添加剂时对反应活性有明显的促进作用。     

纳米氧化硅-氧化铝负载氧化物催化氧化甲醛

采用溶胶-凝胶法制备了纳米氧化硅-氧化铝材料,并利用浸渍法将氧化物负载在该纳米材料上。研究了室温环境下,纳米氧化硅-氧化铝材料负载氧化物去除甲醛的效果。结果表明了相比其他氧化物,负载MnO2的催化材料去除甲醛的效果最好;当负载量为3%左右时,效果最好。     

负载型贵金属低温催化氧化甲醛催化剂的研究

制备贵金属低温催化氧化甲醛催化剂,研究了催化剂结构特征及催化氧化甲醛机理,并考察了催化剂性能。采用沉积-沉淀法制备负载型贵金属低温催化氧化甲醛催化剂,优化组成及制备条件,采用XRD、FT-IR、H_2-TPR、拉曼等对催化剂进行表征分析。催化剂最佳制备条件:NaOH为沉淀剂,载体n(Cu)/n(Mn)摩尔比为1∶2,Pt负载量(质量分数)为1%,载体制备pH为9—10,贵金属负载pH为9.5。Pt_1/Cu_(0.5)Mn催化剂以非化学计量比Cu_(0.9)Mn_(1.8)O_4无定形态晶体特征峰存在,Pt金属在载体表面分布均匀,且贵金属与载体相互作用使催化剂表面氧缺位浓度增加,表面活性氧物种增多,催化剂在室温下表现出良好的稳定性和重复性。室温下甲醛和氧气在催化剂表面共吸附,甲醛首先被催化剂表面活性氧氧化为DOM,由于DOM很活跃,在催化剂上很快被表面氧氧化成甲酸根,甲酸根在催化剂表面氧和气相氧的共同作用下氧化生成CO,最终被完全氧化为CO_2。其中甲酸盐物种向CO转化步骤是整个反应的速控步骤。     

载体热处理温度对Pt/FeO_x催化甲醛氧化性能的影响

将Fe(OH)3以不同温度(T)热处理得到载体FeO_x-T,采用胶体沉积法制备了一系列Pt/FeO_x-T催化剂用于甲醛室温催化氧化反应。通过XRD、BET、H_2-TPR、FTIR和TEM对Pt/FeO_x-T催化剂的结构进行了表征。结果表明:热处理温度影响FeO_x载体的比表面积、氧化还原性质和Pt/FeO_x-T表面羟基的数量,以及Pt物种和FeO_x载体之间的相互作用。活性测试结果表明:以100℃热处理的FeO_x为载体,制备的Pt质量分数为1.5%的Pt/FeO_x-100催化剂具有较高的催化活性,在25℃、相对湿度(RH)55%的条件下,甲醛的转化率可达到96.2%。     

改性Pt/C催化甲醛废水的动力学研究

在气液固三相鼓泡床反应器中(65—125℃,氧分压为0.05—0.25 MPa),采用Pt/含氮活性炭催化湿式氧化处理高浓度甲醛废水(质量分数0.5%—2.5%),建立幂函数动力学模型。动力学研究表明:在排除内外扩散影响的情况下,甲醛和COD的氧化去除符合准一级动力学模型;溶解氧的反应级数分别为0.526和0.745;活化能分别为27.57 kJ/mol和35.98 kJ/mol;指前因子ln k_(10)和ln k_0分别为13.08和17.66;在125℃和氧分压为0.2 MPa下,HCHO和COD的去除率可达99%和98%。文中鼓泡床动力学研究为类似催化湿式氧化动力学研究提供重要借鉴。     

二氧化钛基催化剂催化氧化甲醛的研究进展

甲醛（HCHO）是一种主要的室内空气污染物,具有高致癌性和致突变性,催化氧化是一种理想而有效的室内消除甲醛的方法。二氧化钛作为载体负载贵金属催化剂在甲醛催化氧化反应中表现出优良的催化性能。本文综述了近年来二氧化钛基催化剂催化氧化甲醛的研究进展,主要总结了二氧化钛的吸附机理,二氧化钛晶体结构、表面形貌及微观结构、表面活性氧物种和还原性等对二氧化钛基负载贵金属催化剂催化氧化甲醛性能的影响,重点关注了催化剂的化学结构性质与甲醛氧化活性的关系,并归纳了一部分甲醛催化氧化反应机理。最后指出二氧化钛基催化剂在甲醛催化氧化反应中未来研究方向为：合理设计TiO₂各种缺陷和晶面暴露,同时提高贵金属的分散性和原子利用效率,继而进一步提高催化剂的性能;在保持催化剂高活性、高稳定性的同时,推进设计实际应用整体式催化剂的研究进程。     

超临界流体沉积制备Pt/TiO2工艺条件探究及其催化氧化甲醛性能

为了提高Pt在TiO₂上的分散,进一步提高Pt/TiO₂催化氧化甲醛活性,采用超临界流体沉积(SCFD)方法制备Pt/TiO₂,并对沉积工艺条件进行探索。对比不同催化剂Pt/TiNT和Pt/P25的催化活性,并采用TEM、N₂吸附-脱附、TPR和XPS等对两种催化剂进行表征。结果表明,采用共溶剂(V_乙醇∶V_乙二醇=1∶1)、沉积时间1 h、沉积温度70℃及质量分数0.4%的Pt负载量时,催化剂的催化性能较佳,室温条件下甲醛在Pt/TiNT和Pt/P25上均发生了完全催化氧化反应,Pt/TiNT使甲醛在16 h内净化了82.4%(降解率近100%),Pt/P25使甲醛净化了52.4%(降解率70.3%)。表征结果表明,TiNT管状阵列结构在SCFD中更有利于活性组分的有效分散,Pt和TiNT之间具有更强的相互作用,催化剂表面具有更多的负电荷和氧空位,因而表现出更高的催化活性。     

Pt/C催化剂制备方法的选择

研究了以HCl酸洗、H_2O_2、浓H_2SO_4、HNO_3氧化处理后的活性炭为载体,用不同方法制备了Pt担载量为3%的担载型Pt/C催化剂。TEM统计结果表明,HCl酸洗、HNO_3氧化活性炭为载体,甲醛还原法制备的催化剂分散度最高,平均粒径最小为2．2nm。FT-IR结果表明,HNO_3氧化处理活性炭,活性炭表面含氧基团明显增加。     

Au-Promoted Pt nanoparticles supported on MgO/SBA-15 as an efficient catalyst for selective oxidation of glycerol

A systematic study of Au-promoted and unpromoted Pt/MgO/SBA-15 catalyst is developed to separate the promoter effect from electron transfer effect between Au and Pt. Multi-characterizations revealed that Au and Pt metals in these bimetallic catalysts mainly exist in the form of alloy, and the main role of Au is to reduce the size of AuPt alloy nanoparticles, thus enhancing the adsorption and activation of intermediate products. Through the optimization of various factors (including MgO content, Au/Pt molar ratio, reaction temperature and time), the Au₁Pt₂/MgO/SBA-15 (0.05) catalyst exhibits excellent catalytic activity and glyceric acid selectivity for the selective oxidation of glycerol. Density functional theory calculation confirmed that the synergistic effect between Pt and Au active sites could facilitate the oxidation of primary hydroxyl group by promoting the activation of C H bond and the oxidation of aldehyde group. The results may give insights on designing effective Pt based bimetallic catalyst for selective oxidation of glycerol.     

Hydrogenation of methyl propionate over Ru–Pt/AlOOH catalyst: Effect of surface hydroxyl groups on support and solvent

A ruthenium–platinum bimetallic catalyst supported on boehmite was prepared by co-impregnation and hydrothermal reduction and characterized by XRD, TEM and TG–DTG. Reduction time of the catalyst affected the conversion of γ-Al₂O₃ to boehmite and the specific surface area of the catalyst, and consequently influenced the catalytic performance of the catalyst. Under the same conditions, the Ru–Pt/AlOOH catalyst showed much higher activity and selectivity than the Ru–Pt/γ-Al₂O₃ in aqueous hydrogenation of methyl propionate. The selectivity to 1-propanol of 97.8% could be obtained at methyl propionate conversion of 89.1% over Ru–Pt/AlOOH at 453 K under 5 MPa of H₂ for 6 h. It is postulated that the high performance of this novel catalyst is related to the cooperation of the hydroxyl groups of support surface and water solvent.     

用Pt/C催化剂通过浸渍-还原法制备疏水催化剂

选择XC-72R炭黑为载体,采用改进的浸渍-还原法制备了2~3 nm高分散度Pt/C催化剂。研究了还原温度、还原剂、pH和甲醛用量等工艺条件对Pt粒径大小及分散度的影响,采用透射电镜和X射线衍射等对催化剂进行表征。结果表明,提高溶液pH和反应温度、增加甲醛用量均有助于得到Pt粒子粒径较小的高分散度Pt/C催化剂,较佳的工艺条件为:用乙二醇与水为炭黑分散溶剂,反应温度80~90℃,pH≈11,甲醛用量80倍于PtCl62-物质的量,可以制备Pt粒子粒径在2 nm左右的高分散度Pt/C催化剂。     

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.     

Incorporation of La3+ into a Pt/CeO2/Al2O3 catalyst

The effects of La³⁺ incorporation into a Pt/CeO₂/Al₂O₃ catalyst were investigated by a combination of activity, temperature-programmed reduction (TPR), oxygen storage capacity (OSC), noble-metal surface area, and X-ray diffraction (XRD) measurements. Incorporation of La³⁺ ions into the Al₂O₃, before CeO₂ is added, promoted higher Pt and CeO₂ dispersions. The oxygen storage capacity was also higher in the presence of La³⁺. This is attributed to a combination of Pt and CeO₂ particle-size effects and possible blockage of the reaction between Al₂O₃ and CeO₂. The XRD data show that La³⁺ forms LaAlO₃ with Al₂O₃ and prevents -Al₂O₃ formation after various heat treatments.     

正十二烷在Pt/ZSM-22和Pt/ZSM-23上的加氢异构反应性能

采用常规水热合成法合成了ZSM-22和ZSM-23分子筛,进而制备了分别含有上述分子筛的催化剂,并借助XRD、SEM、NH3-TPD和Py-IR表征了这两种分子筛和催化剂的结构和酸性,同时以正十二烷为模型化合物,采用固定床反应器研究了Pt/ZSM-22和Pt/ZSM-23催化剂上正十二烷加氢异构反应性能。结果表明,在这种模型反应基础上,催化剂的反应活性和选择性主要取决于催化剂的酸量和酸强度以及酸分布,相对而言,ZSM-22分子筛催化剂由于其弱酸和中等强度酸的含量较高,具有更佳的异构化选择性。     

电感耦合等离子发射光谱法测定Pt/Al_2O_3催化剂中的Pt

用电感耦合等离子发射光谱法测定了Al2O3基催化剂中的Pt,考察了基体及所用试剂对Pt测定的影响,发现Al2O3基体、硫酸等对Pt测定均有负干扰,应在标准溶液与基体匹配的情况下进行测定。该方法的检出限为Pt0.10mg/L;样品的加标回收率96%以上。     

In situ hydrogen generation from cycloalkanes using a Pt/CNF catalyst

Pt catalyst supported on carbon nanofibers (CNFs) has been prepared via ion-exchange and it was characterized by XRD, TEM, N₂ physisorption and CO chemisorption. The Pt/CNF catalyst has a small Pt crystallite size in the range of 2–3 nm. This catalyst has been tested in the dehydrogenation of decalin, which is a cycloalkane proposed in the literature as H₂ storage media for vehicles and portable devices. The objective is finding a Pt catalyst suitable for in situ generation of H₂ from chemical storage in decalin. The results revealed that Pt supported on CNF outperforms a Pt catalyst supported on micro–mesoporous activated carbon. Finally, we propose a reactor configuration aiming at the intensification of H₂ production in continuous.