室温下MnOx/HZSM-5催化氧化甲醛的性能和机理分析

以HZSM-5分子筛、高锰酸钾和甲醇为原料制备MnOx/HZSM-5催化剂,室温催化氧化甲醛。采用X射线衍射(XRD)、拉曼光谱(Raman)、扫描电子显微镜(SEM)、透射电镜(TEM)、光电子能谱(XPS)等表征方法分析催化剂的形貌结构、化学成分,研究MnOx/HZSM-5的催化性能和再生性能,探讨其对甲醛的催化氧化机理。结果表明,MnOx/HZSM-5具有良好的催化活性和再生能力,动态测试1020min后MnOx/HZSM-5对甲醛的清除率仍然保持在90%,再生5次后,MnOx/HZSM-5对甲醛清除率仍然保持在91%,静态测试中甲醛清除率达到97%,甲醛转化率达到92%。对MnOx/HZSM-5氧化甲醛的机理分析后发现,甲醛首先被催化剂吸附至MnOx活性位点,之后被初步氧化为甲酸盐或碳酸盐等中间产物,最后被深度氧化为二氧化碳和水。     

沉淀剂对花球状Au/CeO_2催化剂催化氧化CO活性的影响

采用水热合成法制备花状CeO_2载体,并选择了3种沉淀剂NH_4OH、Na_2CO_3和NaOH,通过沉积-沉淀法分别制备Au/CeO_2催化剂。以CO氧化为探针反应,研究不同沉淀剂对催化剂催化CO氧化性能的影响,通过ICP-AES、XRD、TEM、XPS、H_2-TPR等手段对催化剂进行表征,探讨了不同沉淀剂对Au/CeO_2催化CO氧化性能的影响。结果表明,以NaOH为沉淀剂制备催化剂室温活性最低,以NH_4OH和Na_2CO_3为沉淀剂制备的催化剂具有较好的CO氧化催化活性,室温转化率高于95%,但后者的室温催化活性相对更高。不同沉淀剂制备的催化剂活性与其实际金的负载量、金颗粒尺寸和载体还原的难易程度密切相关。     

纳米Au/Fe_2O_3-MO_x催化剂的制备及低温催化氧化CO的研究EI北大核心

用沉积-沉淀法制备了纳米Au/Fe2O3-MOx(M=La和Ce)系列催化剂,考察了催化剂对于CO的低温催化氧化性能,并通过XRD,BET和AAS等表征手段对催化剂进行了表征,分析了稀土氧化物的掺杂对Au/Fe2O3催化剂性能的影响。结果表明:CeO2的加入能够有效提高Au/Fe2O3催化剂的催化活性,而La2O3的加入对催化剂性能没有明显的影响。     

纳米Au／Fe2O3-MOx催化剂的制备及低温催化氧化CO的研究

用沉积-沉淀法制备了纳米Au/Fe2O3-MOx(M=La和Ce)系列催化剂,考察了催化剂对于CO的低温催化氧化性能,并通过XRD,BET和AAS等表征手段对催化剂进行了表征,分析了稀土氧化物的掺杂对Au/FezO3催化剂性能的影响.结果表明:CeO2的加入能够有效提高Au/Fe2O3催化剂的催化活性,而La2O3的加入对催化剂性能没有明显的影响.     

富氢气氛中CO选择性氧化CuO/CeO2催化剂的研究

选择负载型铜催化剂为研究对象,以富氢条件下研究CO选择性氧化反应为导向,考察了反应气氛、焙烧温度、CuO含量及Al2O3掺杂对CuO/CeO2催化剂的CO选择性氧化催化性能的影响,并采用TEM表征技术探讨结构与性能的关系。     

贵金属催化剂低温催化氧化一氧化碳研究进展

随着“双碳”政策的不断推行以及人们环保意识的不断提高,一氧化碳(CO)作为典型的大气污染物,已成为工业废气和汽车尾气排放的主要控制对象。贵金属型CO氧化催化剂具有优异的低温活性、抗中毒抗性能,是CO催化氧化处理的最为有效的手段之一。基于贵金属型CO氧化催化剂的研究现状,重点围绕Pt、Pd、Au、Ag、Rh贵金属催化剂的贵金属调控技术和载体可控技术进行综述,总结了贵金属型CO氧化催化剂的性能优化策略和发展方向,为开发高性能的CO氧化催化剂提供指导。     

Au/Fe_2O_3-MO_x催化剂在气体纯化中的应用研究

电子产业对所使用的气体纯度要求越来越高,气体的纯化工艺变得尤为重要。文中引入了第五周期过渡金属、稀土金属,并考察这些助剂对Au/Fe2O3催化剂性能的影响规律,以期筛选出具有高活性和高稳定性的CO氧化负载型纳米Au/Fe2O3-MOx催化剂,为负载型纳米金催化剂在高纯气体生产领域的应用奠定良好的基础。     

Au/CexZr1-xO2催化剂乙醇部分氧化催化性能的研究

用共沉淀法制备了一系列不同铈锆摩尔比CexZr1-xO2,并用沉积沉淀法制备了Au/CexZr1-xO2催化剂,以乙醇部分氧化制氢为探针反应,研究了Zr掺杂对Au/CeO2催化剂乙醇部分氧化性能的影响,并运用XRD、TEM、TPD、BET等方法对催化剂进行了表征.结果表明,Zr掺杂使Au/CeO2催化剂的颗粒分散更均匀...     

制备参数对花状Au/CeO2催化剂上CO低温氧化性能的影响

采用水热合成法、沉积沉淀法分别制备花球状CeO_2和负载型Au/CeO_2。考察了反应液pH、金的负载量和煅烧温度对Au/CeO_2催化氧化CO活性的影响,确定最佳制备参数,并对优化的Au/CeO_2进行稳定性、储存性和再生性测试。结果表明:反应液的最适宜pH为8.5~9,最适宜的负载量和焙烧温度分别是2%(质量分数)和300℃。优化的Au/CeO_2催化剂,室温下将1%CO催化氧化至1.8×10-6,连续反应67h活性开始下降,当温度升至55℃时,连续反应700h,CO浓度仍然保持在8×10-6以下。此外,该催化剂还表现出良好的储存性和再生性。     

Mn、Fe和Cu氧化物在低温等离子体催化氧化甲苯体系中的活性比较

采用等体积浸渍法制备了MnOx/γ-Al2O3、FeOx/γ-Al2O3和CuOx/γ-Al2O3催化剂,测定了不同催化剂在低温等离子体场内分解甲苯的活性,用X射线衍射(XRD)、氢气程序升温还原(H2-TPR)技术对催化剂进行表征。结果表明催化剂分解甲苯的活性的顺序是MnOx/γ-Al2O3>FeOx/γ-Al2O3>CuOx/γ-Al2O3。催化剂分解臭氧的实验表明,不同催化活性组分对臭氧的催化分解性能顺序与对甲苯的分解性能顺序是一致的。MnOx/γ-Al2O3催化剂的Mn负载量对其催化活性有明显影响,Mn的含量为1%(质量分数)时,催化剂的活性最高,当能量密度为19J/L时,其对甲苯催化氧化的转化率接近100%。催化剂表征结果表明当Mn含量为1%(质量分数)时,氧化锰在载体γ-Al2O3上最接近单层分散量,此时活性组分与载体表面的相互结合力最强,在载体上有很好的分散性,从而表现出对甲苯分解的最好性能。     

Effect of water addition on catalytic activity of nanosized gold catalysts for CO oxidation

The effect of water in the reactant gas on the catalytic activity for CO oxidation over Au/Co3O4 catalysts has been investigated. Water in the reactant gas had a negative effect on the catalytic activity for CO oxidation in Au/Co3O4 catalyst. Furthermore, it was observed that the average particle size of gold on Au/Co3O4 catalysts increased after stability testing both in dry and wet conditions.     

Preparation and characterization of nanosized gold catalysts supported on Co3O4 and their activities for CO oxidation

Gold catalysts supported on Co3O4 were prepared by co-precipitation (CP), deposition-precipitation (DP), and impregnation (IMP) methods. The Au/Co3O4 catalysts were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and temperature programmed reduction (TPR) to understand the different activities for CO oxidation with different preparation methods. Gold particles below 5 nm supported on Co3O4 by DP method were found to be more exposed to the surface than those by CP and IMP methods, and this catalyst was highly active and stable in CO oxidation. Finally, catalytic activity of Au/Co3O4 catalyst for CO oxidation was strongly dependent on the gold particle size.     

A true nanocomposite: Single crystalline Au nanoparticles on single crystalline Fe3O4 nanoparticles

An Au/Fe₃O₄ nanocomposite catalyst was fabricated through a simple deposition-precipitation method. The Au/Fe₃O₄ nanocomposite is a true nanocomposite that has single crystalline Au nanoparticles supported on single crystalline Fe₃O₄ nanoparticles. Lattice fringes from both Au and Fe₃O₄ single nanoparticles were simultaneously observed by transmission electron microscope (TEM). This nanocomposite catalyst showed much high activity in low temperature CO oxidation reaction. The Au/Fe₃O₄ nanocomposite catalyst reaches 100% CO conversion at 40 °C. In comparison, Au/commercial Fe₃O₄ catalyst needs 375 °C to convert CO. This Au/Fe₃O₄ nanocomposite is an ideal sample to study synergetic effect between the catalyst and the support at nanoscale.     

CO combustion catalyst for micro gas sensor application

CO combustion catalysts of Au loaded on Co₃O₄ which contains high concentration of Au (3, 10, 20, and 40 wt%) for the integration on the microdevice were developed and the combustion performance of these catalysts were evaluated. The highly dispersed Au/Co₃O₄ catalyst was prepared using the mechanical mixing of the Au colloid (average particle size of 3 nm) and a cobalt oxide powder (particle size of 20–30 nm). The catalyst preparation by the colloid process could result a better dispersion of Au particles in the Au/Co₃O₄ catalyst. The Au particle size of the Au content of 20 wt% was 1/10 of that by the catalyst of same composition prepared by impregnation process in our previous studies. This improvement of microstructure enhanced the combustion performance of the catalyst, which was improved 10 times as compared to that of our previous study. Moreover, the CO selectivity of the Au/Co₃O₄ catalyst on the microdevice depended on the Au particle size.     

Pd负载型介孔ZrO2-TiO2复合材料的设计合成及其CO催化氧化性能研究

以介孔结构的复合ZrO₂-TiO₂为载体负载活性组分, 制备了具有高CO催化氧化活性的Pd/ZrO₂-TiO₂与PdCu/ZrO₂-TiO₂负载型催化剂。XRD、TEM研究结果表明: 活性组分Pd、Cu物种可均匀分散于介孔载体中。系统考察了不同的催化剂载体、制备方法和助催化剂等对该介孔复合材料CO催化氧化性能的影响, 结果表明: 以ZrO₂-TiO₂为载体的催化剂其CO催化氧化活性明显优于以介孔Al₂O₃或介孔SBA-15为载体的催化剂; 一步法制备的介孔Pd/ZrO₂-TiO₂催化剂其CO催化氧化的低温活性较浸渍法制备的Pd/ZrO₂-TiO₂有很大提高; 并且Pd和Cu物种共负载的介孔ZrO₂-TiO₂复合催化剂具有最优的CO催化氧化活性, 其CO的完全催化氧化温度可降至170℃, O₂-TPD分析说明Pd和Cu之间的相互作用使得PdCu/ZT催化剂在更低温度具有氧化还原活性。     

Au/LaVO4 Nanocomposite: Preparation, characterization, and catalytic activity for CO oxidation

The size of the gold particles is a very important parameter to get active catalysts. This paper reports a novel colloidal deposition method to prepare Au/LaVO₄ nanocomposite catalyst with monodispersed Au colloids and uniform LaVO₄ nanoplates in nonpolar solvent. Monodispersed Au colloids with tunable size (such as 2, 5, 7, 11, 13, and 16 nm) and LaVO₄ nanocrystals with well-defi ned shapes were pre-synthesized assisted with oleic acid/amine. During the following immobilization process, the particle size and shape of Au and LaVO₄ were nearly preserved. As-prepared Au/LaVO₄ nanocomposite showed high catalytic activity for CO oxidation at room temperature. Since sizes of gold particles were well-defi ned before the immobilization process, size effect of gold particles was easy to be investigated and the results show that 5-nm Au/LaVO₄ nanocomposite has the highest activity for CO oxidation. This synthetic method can be extended further for the preparation of other composite nanomaterials.     

Engineering 3D Ru/Graphene Aerogel Using Metal–Organic Frameworks: Capture and Highly Efficient Catalytic CO Oxidation at Room Temperature

Noble metals (Au, Pt, and Ru) loaded into carbon supports show excellent performance for CO oxidation. Herein, a tunable metal–organic framework (MOF) coating is applied to a macroscopic 3D Ru/graphene aerogel (Ru/GA) composite, using a facial step‐by‐step method. The open macroporous structure of the Ru/GA provides pathways for the access and diffusion of reactant and product molecules. The resulting HK (HKUST‐1)‐containing MOF composite exhibits good performance for CO adsorption. It can simultaneously adsorb and oxidize CO, which improves the reaction rate. In this work, the catalytic efficiency of the resulting catalyst is higher than that (≈48.4%) of the Ru/GA. These findings provide a simple method for increasing the instantaneous concentration of reactants around the catalyst, which in turn increases the reaction rate. The catalytic performances of composites subjected to different pretreatment conditions are also investigated. Hopefully, this finding may provide a feasible direction for the effective management of the diverse environment issues.     

Control of Catalytic Activity of Nano‐Au through Tailoring the Fermi Level of Support

The catalytic properties of nanometals are strongly dependent on their electronic states which, are influenced by the interaction with the supports. However, a precise manipulation of the electronic interaction is lacking, and the nature of the interaction is still ambiguous. Herein, using Au/ZnFe_xCo_2?xO₄ (x = 0–2) as a model system with continuously tuned Fermi levels of supports, the electronic structure of the Au catalyst can be precisely controlled by changing the Fermi level of the support, which arises from the charge redistribution between the two phases. A higher Fermi level of ZnFe₂O₄ support makes nano‐Au negatively charged and thus facilitates the oxidation of CO, and in contrast, a lower Fermi level of ZnCo₂O₄ support makes nano‐Au positively charged and is preferential to the oxidation of benzyl alcohol. This work represents a solid step towards exploration of advanced catalysts with deliberate design of electronic structure and catalytic properties.