活性组分稀土氧化物对甲苯催化燃烧性能的影响

以活性组分氧化铜、氧化锰为基础,加入活性组分稀土氧化物,研究对甲苯催化燃烧性能影响。研究结果表明,在所选稀土氧化物中,加入氧化铈时甲苯的起燃温度和完全燃烧温度最低;在一定的负载量下,Cu∶Mn∶Ce摩尔比为1∶2∶0.7时,制备的Cu Mn Ce/Zr O2整体催化剂甲苯完全燃烧温度最低;催化剂合理的焙烧温度为500℃,此时甲苯的起燃温度约200℃,完全燃烧温度为220℃;催化剂合理的焙烧时间为3 h。     

钾掺杂对铈锆固溶体催化性能的影响

为研究钾掺杂对铈锆固溶体催化性能的影响,以Ce0.7Zr0.3O2为基体制备了一系列钾掺杂的铈锆固溶体xK-Ce0.7Zr0.3O2(x=0.05、0.10、0.15、0.20、0.25、0.30)催化剂样品,通过程序升温氧化(TPO)过程进行活性评价,并通过XRD、BET、H2-TPR和O2-TPD进行分析表征。结果表明,采用溶胶凝胶法制备的催化剂的催化性能比络合燃烧法所制备的稍好;当钾的掺杂量为0.10≤x≤0.30时,xK-Ce0.7Zr0.3O2催化碳烟颗粒燃烧的活性得到提高,起燃温度和最大燃烧速率温度分别在315℃和375℃附近,明显优于Ce0.7Zr0.3O2;掺杂钾后的催化剂样品均能形成萤石结构,并且随钾掺杂量的增大比表面积减小。     

纳米TiO2负载CuMnOx对二甲苯完全燃烧的催化性能研究

以金红石型纳米TiO2为载体,采用等体积浸渍法制备了负载型CuMnOx/TiOo2催化剂,研究了其对易挥发性有机物二甲苯完全燃烧反应的催化活性.结果表明,控制锰铜质量比为1:1和锰铜负载量为20%(质量分数)时,经500℃焙烧2 h制备的催化剂具有良好的催化活性,二甲苯催化燃烧的起燃温度(T10%)和完全燃烧温度(T95%)分别为155℃和270℃.由X射线衍射(XRD)分析结果得出,催化剂的主要活性相是类尖晶石Cu1.5Mn1.5O4,纳米TiO2载体对活性相有很好的分散作用,其晶粒小,使得CuMnOx/TiO2催化剂的活性高.     

B,N和Ce共掺杂TiO_2催化剂光催化活性研究

采用溶胶-凝胶法制备出B,N和Ce共掺杂TiO2光催化剂,并用XRD、SEM等表征了其结构特征。以酸性大红染料溶液的光催化降解为探针反应,考察了制备条件对共掺杂TiO2催化剂活性的影响。结果表明,在400℃,当B,N和Ce的原子比为1∶2∶0.1,焙烧3 h时,光催化剂活性最大,大红染料的降解率达到98%。     

B,N和Ce共掺杂TiO2催化剂光催化活性研究

采用溶胶-凝胶法制备出B,N和Ce共掺杂TiO2光催化剂,并用XRD、SEM等表征了其结构特征。以酸性大红染料溶液的光催化降解为探针反应,考察了制备条件对共掺杂TiO2催化剂活性的影响。结果表明,在400℃,当B,N和Ce的原子比为1∶2∶0.1,焙烧3 h时,光催化剂活性最大,大红染料的降解率达到98%。     

新型Cu-Co-O_x催化剂的制备及其催化燃烧甲苯的性能研究

采用浸渍法制备自制载体负载复合金属氧化物Cu-Co-Ox催化剂。研究了Cu-Co-Ox催化剂催化燃烧甲苯的活性。分别考察了Cu-Co-Ox负载量、Cu/Co(摩尔比)及焙烧温度对催化燃烧甲苯活性的影响,并采用X射线衍射(XRD)及扫描电镜(SEM)等表征技术,分别对复合金属氧化物Cu-Co-Ox的晶型与结晶形貌进行了分析。结果表明,焙烧温度为600℃,Cu-Co-Ox负载量为5%(质量分数),Cu/Co为1∶2时,Cu-Co-Ox催化燃烧甲苯的活性最高。当反应温度为250℃,甲苯的转化率达到95%以上。XRD分析表明,Cu-Co-Ox催化剂主要活性相为CuCo2O4尖晶石。     

制备方法对Mn-Ce/TiO2催化剂低温选择性催化还原活性的影响

采用溶胶凝胶法、浸渍法以及两者相结合的方法制备了Mn-Ce/TiO2催化剂.运用XRD、BET和SEM等技术对催化剂进行了表征,发现溶胶凝胶法制备的Mn-Ce/TiO2催化剂为锐钛矿结构,具有较大的比表面积,中孔结构丰富,Mn、Ce活性组分在载体表面高度分散或形成了无定形结构.实验研究了催化剂对氨选择性催化还原NO反应的催化性能,结果表明,用溶胶凝胶法制备的Mn-Ce/TiO2催化剂脱硝活性最好,当Mn、Ce负载量为20％,NH3/NO摩尔比为1.1,空速为9 436 h-1,烟气温度为240℃时,NO转化率大于90％.     

Ce掺杂纳米TiO2光催化剂的制备及降解甲醛的研究

介绍了溶胶-凝胶法制备Ce离子掺杂纳米TiO2的工艺流程.采用X射线衍射(XRD)、紫外可见分光光度法(UV-Vis)等方法表征了Ce掺杂TiO2的相组成、紫外可见漫反射率与掺杂量的关系.结果表明,掺杂的TiO2在520℃、650℃焙烧2 h呈锐钛矿结构,在520℃焙烧2 h的TiO2的晶粒尺寸大约为20 nm,而掺杂Ce后其晶粒尺寸均减小,大约为12nm.UV-Vis吸光度分析表明,掺Ce后吸收带边明显发生红移,但随着Ce掺杂浓度的增大,其对可见光的吸收影响不大.光催化降解反应表明,未掺杂Ce的TiO2反应2 h后对甲醛的没有降解作用,而Ce掺杂TiO2反应2 h后甲醛降解率达15%.     

锰铜铈氧化物催化剂氧化NO性能及动力学研究

实验以TiO2为载体采用浸渍法制备CuOx/TiO2、CeOx/TiO2、CuCeOx/TiO2和MnCuCeOx/TiO2催化剂,考察这些催化剂氧化NO活性,探究Cu、Ce摩尔比和添加Mn元素对CuCeOx/TiO2催化剂氧化NO活性的影响,使用扫描电镜观察催化剂表面结构。研究发现,Cu、Ce元素配合后的CuCeOx/TiO2催化剂氧化活性明显好于单独含Cu、Ce的催化剂,当Cu、Ce摩尔比为Cu:Ce=1∶2时,CuCeOx/TiO2催化剂氧化活性最好,在NO浓度500×10-6,O210%,空速为24 000 h-1,350℃时,NO氧化度为0.62;添加Mn元素可以提高CuCeOx/TiO2催化剂低温氧化活性,250℃时,MnCuCe/Ti-3和MnCuCe/Ti-5催化剂氧化度为0.53和0.69,300℃时,MnCuCe/Ti-3和MnCuCe/Ti-5催化剂氧化度均为0.76;此外,实验还研究了NO在MnCuCe/Ti-3催化剂上反应的动力学方程。     

Ce掺杂纳米TiO2光催化剂的制备及降解甲醛的研究

介绍了溶胶-凝胶法制备Ce离子掺杂纳米TiO2的工艺流程。采用X射线衍射（XRD）、紫外可见分光光度法（UV-Vis）等方法表征了Ce掺杂TiO2的相组成、紫外可见漫反射率与掺杂量的关系。结果表明，掺杂的TiO2在520℃．650℃焙烧2h呈锐钛矿结构，在520℃焙烧2h的TiO2的晶粒尺寸大约为20nm，而掺杂Ce后其晶粒尺寸均减小，大约为12nm。UV-Vis吸光度分析表明，掺Ce后吸收带边明显发生红移，但随着Ce掺杂浓度的增大，其对可见光的吸收影响不大。光催化降解反应表明，未掺杂Ce的TiO2反应2h后对甲醛的没有降解作用，而Ce掺杂TiO2反应2h后甲醛降解率达15％。     

Degradation of explosives-related compounds using nickel catalysts

We report the ability of nickel-based catalysts to degrade explosives compounds in aqueous solution. Several nickel catalysts completely degraded the explosives, although rates varied. Nearly all of the organic explosive compounds tested, including 2,4,6-trinitrotoluene (TNT), hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX), and octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX), were rapidly degraded to below detection limits by a powdered nickel on an alumina-silicate support (Aldrich nickel catalyst). Perchlorate degradation was minimal (<25%). Degradation of TNT by Aldrich nickel catalyst resulted in apparent first-order kinetics. Significant gaseous 14C was released and collected in an alkaline solution (most likely carbon dioxide) from [14C]RDX and [14C]HMX, indicating heterocyclic ring cleavage. Significant gaseous 14C was not produced from [14C]TNT, but spectrophotometric evidence indicated loss of aromaticity. Degradation occurred in low ionic strength solutions, groundwater, and from pH 3 to pH 9. Degradation of TNT, RDX, and HMX was maintained in flow-through columns of Aldrich nickel catalyst mixed with sand down to a hydraulic retention time of 4h. These data indicate that nickel-based catalysts may be an effective means for remediation of energetics-contaminated groundwater.     

Noble metal catalysts for methane removal

Using a bench-scale rig, the activities of Pt, Pd and Pt+Pd catalysts supported on gamma-Al(2)O(3) and on TiO(2) (anatase) for the complete oxidation of methane (300 ppmv) in air have been measured as a function of temperature; values of T(10), T(50) and T(90) together with the Arrhenius parameters (activation energy and pre-exponential factor) are reported. Pt is less active than Pd when deposited on the surface of the TiO(2), but more active when deposited on gamma-Al(2)O(3), however when combined, the Pt+Pd mixture is more active than either metal individually. The T(10) for Pt+Pd/gamma-Al(2)O(3) was being as low as 228 degrees C. The significance of the Arrhenius parameters, for metal containing catalysts is that they exhibit compensation with increasing activation energy, while securing a more rapid increase in conversion from 0% to 100% when the temperature is increased.     

氧化镁基催化剂及脱硝性能研究

为控制燃烧烟气中NOx的污染,对共混合方法制备的氧化镁基催化剂进行烟气直接催化分解法脱硝实验研究,分析模拟烟气脱硝塔内温度及床层高度及氧气浓度、NO浓度和空速对脱硝效率的影响.研究表明:氧化镁基催化剂可以采用直接催化分解法对烟气脱硝,脱硝率85%～95%,氧化镁基催化吸附剂组成为氧化镁、固化剂、添加剂;脱硝的床层高度4～5 cm,脱硝反应温度130～170℃,烟气空速2 500～3 000 h-1;研究推测出氧化镁基催化剂存在活性缺陷,并对脱硝机理进行了初步分析.     

钴磷合金催化剂的制备及其催化分解磷化氢的研究

采用诱导化学沉积法制备系列Co-P合金,并将其引入PH3的分解试验.结果表明,所有样品均具有在较低温度下催化分解PH3的性能,且测定的表观催化反应温度随合金中磷质量分数的升高而降低,当磷的质量分数≥7.7%时,表观催化反应温度＜450 ℃.选取Co86.3P13.7样品进行催化分解PH3气体的研究表明,实验条件下,PH3分解率随催化反应温度的升高呈现先增后减的趋势,但随总通气流量QPH3 QN2或通气量比QN2∶QPH3的增大而降低.控制催化反应温度为470 ℃、PH3进气流量QPH3=4～6 mL/min、通气比QN2∶QPH3=33～35时,催化剂可发挥最佳的催化性能,此时PH3的分解率达95%以上.对Co86.3P13.7不同处理温度下的X射线衍射(XRD)表征分析表明,样品在催化反应温度下发生晶化,有磷化物Co2P析出,但催化反应测试温度范围内晶化后的催化剂基本保持稳定.     

Catalytic destruction of dichloromethane using perovskite-type oxide catalysts

Dichloromethane (DCM, also known as methylene chloride [CH2Cl2]) is often present in industrial waste gas and is a valuable chemical product in the chemical industry. This study addresses the oxidation of airstreams that contain CH2Cl2 by catalytic oxidation in a tubular fixed-bed reactor over perovskite-type oxide catalysts. This work also considers how the concentration of influent CH2Cl2 (Co = 500-1000 ppm), the space velocity (GHSV = 5000-48,000 1/hr), the relative humidity (RH = 10-70%) and the concentration of oxygen (O2 = 5-21%) influence the operational stability and capacity for the removal of CH2Cl2. The surface area of lanthanum (La)-cobalt (Co) composite catalyst was the greatest of the five perovskite-type catalysts prepared in various composites of La, strontium, and Co metal oxides. Approximately 99.5% CH2Cl2 reduction was achieved by the catalytic oxidation over LaCoO3-based perovskite catalyst at 600 degrees C. Furthermore, the effect of the initial concentration and reaction temperature on the removal of CH2Cl2 in the gaseous phase was also monitored. This study also provides information that a higher humidity corresponds to a lower conversion. Carbon dioxide and hydrogen chloride were the two main products of the oxidation process at a relative humidity of 70%.     

废汽车尾气三元催化剂的回收利用研究进展

随着汽车行业的迅猛发展,中国的废汽车尾气三元催化剂(TWCs)产生量将越来越大。由于废汽车尾气TWCs中富含铂、钯、铑等铂族贵金属,对其的不合理回收和提炼,不仅导致稀缺贵金属资源的流失,还会造成严重的环境污染。从废汽车尾气TWCs的回收政策、回收体系和回收技术3个层面,分析了国内外相关国家的最新进展,指明了中国在废汽车尾气TWCs回收过程中亟待解决的问题,最后还提出了应对建议。     

Humic substances as catalysts in condensation reactions

Humic substances (HS) demonstrate appreciable impact on the rate of the condensation reactions as shown in the example of the reaction between hydrazine and 4-(dimethylamino)-benzaldhyde in an aquatic environment. The catalytic activity of HS has also been demonstrated in Knoevenagel and Claisen-Schmidt reactions for condensation of carbonyl compounds with CH acids. The aquatic fulvic acids are the most active in these reactions. The velocity of the studied reactions also depends on pH, temperature, the concentration and origin of HS used. A possible micellar and acid-base catalysis mechanism in aquatic media has been suggested.     

钴钛层柱粘土催化剂催脱除零价汞简

采用钴-钛层柱粘土催化剂，向烟气中添加HCl气体进行零价汞的催化脱除实验研究。考察了反应温度及催化剂的焙烧温度、Ti/粘土、活性组分（Co）负载量等制备条件对零价汞催化脱除效果的影响。研究表明，在HCl含量20×10^-6的模拟烟气中，焙烧温度为400℃、Ti/粘土为15 mmol/g、Co含量为5 wt%（以CoO计）的钴钛层柱粘土催化剂（Co-Ti-PILCs）在空速为1.0×10⁴ h^-1、温度为300℃时零价汞脱除效率为86.7%。