Decomposition of hexachlorobenzene over Al2O3 supported metal oxide catalysts

Decomposition of hexachlorobenzene (HCB) was investigated over several metal oxides (i.e., MgO, CaO, BaO, La₂O₃, CeO₂, MnO₂, Fe₂O₃, and Co₃O₄) supported on Al₂O₃, which was achieved in closed system at a temperature of 300°C. Catalysts were prepared by incipient wetness impregnation with different metal oxides loading and impregnating solvents. The decomposition efficiency of different catalysts for this reaction depends on the nature of the metal oxide used, and Al₂O₃ supported La₂O₃ was found to be the most active one. Pentachlorobenzene (PeCB), and all tetrachlorobenzene (TeCB), trichlorobenzene (TrCB), and dichlorobenzene (DCB) isomers were detected after the decomposition reaction, indicating that the decomposition was mainly a dechlorination process. The detection of all lower chlorinated benzenes suggested the complexity of decomposition and the presence of more than one dechlorination pathway.     

Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process

Characteristics of toluene decomposition and formation of nitrogen oxide(NOx) by-products were investigated in a dielectric barrier discharge(DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide(Mn Ox), iron oxide(Fe Ox), cobalt oxide(Co Ox) and copper oxide(Cu O), supported on Al2O3/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO2 selectivity. In addition, NOx was suppressed with the decrease of specific energy density(SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the Cu O catalyst showed the best performance in NOx suppression. The Mn Ox catalyst exhibited the lowest concentration of O3 and highest CO2 selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.     

Al2O3为载体的催化剂净化贫燃汽车尾气研究

在富氧条件下,考察了C₃H₆和C₂H₅OH在Ag/Al₂O₃、In/Al₂O₃、Sn/Al₂O₃、Co/Al₂O₃、Pt/Al₂O₃和Ag/Al₂O₃+Pt/Al₂O₃组合催化剂上选择性还原NO的性能.结果表明,Ag/Al₂O₃具有最高的NO还原活性.在负载型过渡金属氧化物催化剂上,会生成显著量的CO,其HC和CO氧化转化温度也远远高于Pt/Al₂O₃催化剂.串联组合Ag/Al₂O₃+Pt/Al₂O₃催化剂可显著拓宽活性温度范围,促进HC和CO氧化,降低N₂O和CH₃CHO生成量.     

负载型燃烧催化剂La_(0.8)Ce_(0.2)CoO_3/Ce_(0.8)Zr_(0.2)O_2制备及性能研究

以复合氧化物La0.8Ce0.2CoO3为活性组分,Ce0.8Zr0.2O2固溶体为载体,采用柠檬酸络合法制备出负载型燃烧催化剂La0.8Ce0.2CoO3/Ce0.8Zr0.2O2。用XRD、BET和SEM对其进行表征,考察了焙烧温度、反应时间、反应温度及H2S存在对催化剂活性的影响。结果表明,载体表面形成了均一的钙钛矿相;该负载型催化剂对二甲苯完全氧化反应具有较高的催化活性,有良好的热稳定性、操作稳定性和强的抗H2S毒化能力。这可能是载体与负载组分之间密切的协同作用所导致。     

CeO2-La2O3/γ-Al2O3稀土氧化物混合物催化还原SO2的实验研究

在La₂O₃ 中加入变价稀土氧化物CeO₂,组成一种稀土氧化物的混合物,以这种混合物作为CO还原SO₂的催化剂.采用连续流动固定床反应器,在反应气体SO₂和CO按SO₂∶CO = 1∶3,载流气体为N₂,气体流量为1000 mL/min的条件下,实验研究了该催化剂的活化过程以及温度和反应物浓度配比对活化反应的影响,用XRD和XPS对反应前后催化剂进行了表征,分析了相结构的变化.结果表明:CeO₂和La₂O₃ 2种稀土氧化物的混合物,在CO还原SO₂的催化反应中,活化温度比单个的CeO₂或La₂O₃氧化物下降了50℃～100℃,而且具有更高的活性.这可能是CeO₂和La₂O₃氧化物之间存在着某种协同作用所致.     

不同方法制备的铟催化剂选择性还原NO

不同负载量的In/Al₂O₃催化剂分别以浸渍法、共沉淀法和溶胶-凝胶法制得,对比评价了不同方法制备的样品在富氧条件下以丙烯为还原剂,选择性催化还原NO的活性,考察了氧气浓度、H₂O对活性的影响.研究表明,铟催化剂有较高的去除NO活性,制备方法对催化剂活性具有显著影响.其中,溶胶-凝胶法和共沉淀法最高活性都可达90%左右;而浸渍法样品的活性较差,最高转化率不到60%.氧气浓度对NOx最高转化率及其相应反应温度均有重要影响.随着O2浓度的提高,最高活性对应的反应温度降低.反应气氛中H₂O的加入使铟催化剂活性大幅降低.铟与其他多种金属活性组分相比,一个突出的不同表现是,3种方法各自的最佳负载量相差不大.     

金属氧化物负载γ-Al_2O_3粒子电极对酸性橙Ⅱ的电催化氧化研究

以γ-Al_2O_3作为载体,采用浸渍热分解法制备了Sn、Mn、Cu、Pb单组分氧化物和Sn-Ce-Sb复合氧化物粒子电极。通过对酸性橙II(AOII)的降解实验,以及采用重复试验和扫描电镜(SEM)、紫外光谱扫描等方法,探讨了粒子电极材料的性能。研究结果表明:Sn/γ-Al_2O_3相比于Mn/γ-Al_2O_3、Cu/γ-Al_2O_3、Pb/γ-Al_2O_3等单组分氧化物粒子电极表现出了更好的电催化活性和稳定性。掺杂Ce、Sb后电极表面晶体粒径细小且分布均匀,有利于提高Sn/γ-Al_2O_3粒子电极的性能。电流密度为20 m A/cm2,曝气量0.5 L/min反应条件下,反应3 h后Sn-Ce-Sb/γ-Al_2O_3粒子电极对AOII的去除率为100%,TOC的去除率达84.2%,重复使用5次后TOC去除率仍保持在80%以上。表明Sn-Ce-Sb/γ-Al_2O_3粒子电极具有较好的应用前景。     

Influence of NOx on the activity of Pd/θ-Al2O3 catalyst for methane oxidation: Alleviation of transient deactivation

Alumina supported Pd catalyst（Pd/Al₂O₃） is active for complete oxidation of methane, while often suffers transient deactivation during the cold down process. Herein, heating and cooling cycle tests between 200 and 900 °C and isothermal experiments at 650 °C were conducted to investigate the influence of NO_x on transient deactivation of Pd/θ-Al₂O₃ catalyst during the methane oxidation. It was found that the co-fed of NO alleviated transient d...     

Recent advances in catalytic decomposition of ozone

Ozone (O₃), as a harmful air pollutant, has been of wide concern. Safe, efficient, and economical O₃ removal methods urgently need to be developed. Catalytic decomposition is the most promising method for O₃ removal, especially at room temperature or even subzero temperatures. Great efforts have been made to develop high-efficiency catalysts for O₃ decomposition that can operate at low temperatures, high space velocity and high humidity. First, this review describes the general reaction mechanism of O₃ decomposition on noble metal and transition metal oxide catalysts. Then, progress on the O₃ decomposition performance of various catalysts in the past 30 years is summarized in detail. The main focus is the O₃ decomposition performance of manganese oxides, which are divided into supported manganese oxides and non-supported manganese oxides. Methods to improve the activity, stability, and humidity resistance of manganese oxide catalysts for O₃ decomposition are also summarized. The deactivation mechanisms of manganese oxides under dry and humid conditions are discussed. The O₃ decomposition performance of monolithic catalysts is also summarized from the perspective of industrial applications. Finally, the future development directions and prospects of O₃ catalytic decomposition technology are put forward.     

Preparation and catalytic properties of ZrO2-Al2O3 composite oxide supported nickel catalysts for methane reforming with carbon dioxide

ZrO2-Al2O3 composite oxides and supported Ni catalysts were prepared, and characterized by N2 adsorption/desorption, X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) techniques. The catalytic performance and carbon deposition was also investigated. This mesoporous composite oxide is shown to be a promising catalyst support. An increase in the catalytic activity and stability of methane and carbon dioxide reforming reaction was resulted from the zirconia addition, especially at 5wt% ZrO2 content. The Ni catalyst supported ZrO2-Al2O3 has a strong resistance to sintering and the carbon deposition in a relatively long-term reaction.     

地下水脱硝催化剂的制备及其性能研究

以Al2O3为载体制备了负载型催化剂,通过甲酸催化还原脱除地下水中硝酸盐对该催化剂进行了活性评价,并研究了催化剂制备条件对催化性能的影响,发现催化剂种类、配比及其含量不同,催化剂的催化性能也相应发生变化,其中4%Pd-1%Cu/Al2O3催化剂可以在45min内将100mg/L的NO3-被完全去除。     

Bioaccumulation of heavy metals by Phragmites australis cultivated in synthesized substrates

Accumulation of heavy metals from various oxides with adsorbed cadmium by wetland plant Phragmites australis was studied to evaluate the fate of heavy metals in the sediment of constructed wetlands. Hoagland solution was used as nutrition supply, and single metal oxide with adsorbed cadmium was applied as contaminant to study the accumulation characteristics of cadmium and the substrate metals by P. australis. After 45-d treatment, the bioaccumulation degree in root followed the order: Al(OH)3 > Al2O3 > Fe3O4 > MnO2 > FeOOH. Heavy metals absorbed by P. australis were largely immobilized by the roots with little translocation to aboveground parts.     

高湿度条件下分解臭氧的锰催化剂

分别以硝酸锰和乙酸锰为前体 ,用浸渍法制备了MnOx γ Al2 O3催化剂 ,考察了它们对高湿度高浓度臭氧的催化分解性能。分析了在不同的温度煅烧和用不同的前体制备的催化剂上的氧化锰的形态。实验表明 ,以乙酸锰为前体 ,在 4 0 0℃煅烧得到的催化剂的臭氧催化分解活性最高 ,保持 95 %的臭氧分解率 ,其使用寿命在 10 0h以上 ,该催化剂上锰的主要形态为Mn2 O3,在载体上分散性最好     

程序升温条件下铁及其氧化物在CO存在时对N_2O的还原机理

应用热综合分析仪 (TG FTIR)研究了在还原性气氛下Fe及其氧化物对N2 O的催化还原作用 .研究发现铁氧化物对氮氧化物的催化还原能力相当弱 ,而Fe可以高效地降低N2 O分解的初始温度和提高N2 O向N2 的转化率 .在Fe和CO的作用下 ,N2 O的初始分解温度为 92 0K和 10 0 0K .在 112 3K时 ,N2 O的转化率达到 95 %和 80 % .TG/DSC曲线表明了在Fe与N2 O反应过程中CO的作用表现为通过与N2 O在反应表面的竞争吸附使铁氧化物还原为金属铁 ,X射线衍射证明Fe与N2 O反应后的氧化物为Fe2 O3 ;扫描电镜对反应后Fe表面物理形态的研究发现 ,在CO作用下 ,Fe的表面呈松散结构 ,可以保证Fe对氮氧化物反应的连续进行     

外加氮源影响下铁铝氧化物在土壤氮素转化中的作用

土壤中铁铝氧化物在团聚体稳定性和有机碳吸附方面具有重要作用,而氮添加对土壤氮循环影响的变化也可能与其有关,但是目前尚缺乏在氮循环方面的研究.为了探究铁铝氧化物在土壤氮素转化中的作用,选择福建省建瓯罗浮栲森林土壤为研究对象,采用选择性溶提技术准备不同的土壤——未经处理（T1）的土壤和去除游离态铁铝氧化物（T2）土壤、去除非晶质铁铝氧化物（T3）土壤、去除络合态铁铝氧化物（T4）土壤,在这些土壤中添加不同形态氮（40 mg/kg）——丙氨酸（氨基酸态氮,AA）、硫酸铵（铵态氮,AN）、硝酸钠（硝态氮,NAN）和亚硝酸钠（亚硝态氮,NIN）,进行室内培养试验,分析氮含量变化和氮素转化情况.结果表明:①与CK处理相比,AA和AN处理均增加了T1土壤中w（NH₄+-N）,NAN处理增加了w（NO₃--N）,但低于添加量,表明添加氨基酸和铵态氮均会促进氮矿化,添加硝态氮会增加NO₃--N的固定且抑制其硝化.②在CK处理下,与T1土壤相比,T2和T4土壤中w（NH₄+-N）、w（NO₃--N）和w（氨基酸）均降低,但T3土壤中w（NH₄+-N）和w（氨基酸）增加、w（NO₃--N）降低,表明土壤中游离态氧化铁铝和络合态氧化铁铝的存在有助于氮素矿化,非晶质氧化铁铝有助于硝化.③在不同氮处理下,各土壤的氮含量及其转化速率与CK处理规律相似.与CK处理相比,各氮处理均未显著增加T2和T4土壤中w（NH₄+-N）,且AA和AN处理均未影响T2、T3和T4土壤中w（NO₃--N）和w（氨基酸）.结果显示,氮添加并没有改变铁铝氧化物的作用,其中,矿化和氨化作用均表现为游离氧化铁铝>络合氧化铁铝>非晶质氧化铁铝,硝化作用表现为非晶质氧化铁铝>游离氧化铁铝>络合态氧化铁铝.因此,土壤铁铝氧化物的不同存在状态应该是调节氮素转化的重要土壤条件.      

生物质型煤固硫添加剂的固硫增强作用

在管式炉中进行了生物质型煤的燃烧固硫试验,考察了Al₂O₃、Fe₂O₃和MnO₂共3种添加剂对钙基固硫剂的固硫增强作用.结果表明,只有Al₂O₃增强了型煤的固硫作用.通过TGA试验进一步证实,在还原性气氛下Al₂O₃可有效地抑制固硫产物CaSO₄的高温分解.XPS和XRD分析表明,Al₂O₃通过与CaSO₄和CaO作用,形成了热稳定性高的复盐CaSO₄·3CaO·3Al₂O₃,并包裹在CaSO₄晶体的表面,从而抑制了CaSO₄的分解.     

Al3+离子掺杂对负载TiO2薄膜光催化活性的影响

以钛酸丁酯和Al2(SO4)3·18H2O为原料,采用溶胶凝胶法在钛片、玻璃、釉面瓷砖、陶瓷、不锈钢和铝片六种载体上制备了Al3+掺杂TiO2薄膜,讨论了不同Al3+掺杂浓度下,不同载体表面上制备的TiO2薄膜对甲基橙脱色率的影响。试验结果表明Al3+对TiO2薄膜的掺杂效果与载体的类型密切相关,并且不同载体其Al3+掺杂的最佳浓度也不同。Al3+掺杂后,TiO2薄膜光催化活性提高最大的是玻璃,其次是釉面瓷砖、铝片、钛片、陶瓷,最差的是负载不锈钢。     

铝合金在模拟海岛环境中腐蚀产物的红外光谱研究

目的研究弹药金属元件中铝合金材料在高湿、高盐雾环境中的腐蚀规律。方法在模拟海岛环境的高湿、高盐雾条件下研究铝合金的腐蚀过程,利用红外光谱法(IR)对腐蚀产物进行表征,并对其腐蚀机理作出初步探讨。结果铝合金暴露在潮湿的空气中,在其表面易于吸附一层薄的液层,液层中发生电化学反应,在铝合金表面生成一层Al(OH)3,同时Al(OH)3慢慢脱水后就形成了更为稳定的Al2O3。结论当铝合金表面沉积有盐粒时,由于Cl-的强侵蚀性和Na Cl的潮解作用,在铝合金试样表面形成了无数的微电池,最终导致Al2O3保护膜的破裂,腐蚀介质就会与基体接触,使得腐蚀不断地发展延伸,加快了基体的腐蚀。     

Unraveling SO2-tolerant mechanism over Fe2（SO4）3/TiO2 catalysts for NOx reduction

Developing low-temperature SO₂-tolerant catalysts for the selective catalytic reduction of NO_x is still a challenging task. The sulfation of active metal oxides and deposition of ammonium bisulfate deactivate catalysts, due to the difficult decomposition of the as-formed sulfate species at low temperatures（<300 °C）. In recent years, metal sulfate catalysts have attracted increasing attention owing to their good catalytic activity and strong SO₂ tolerance at hi...     

催化分解N_2O催化剂的研究新进展

直接催化分解N2O技术已成为当前国内外工业脱除N2O应用研究的主流和发展方向,催化剂是技术核心。综述了贵金属、金属氧化物、沸石以及其他用于分解N2O的新型固体催化剂的最新研究现状。对催化剂的研究方法、思路进行了评述,总结了现存的问题,并展望了直接催化分解N2O催化剂未来的发展方向。其中,沸石类催化剂由于高活性和结构稳定性,有望成为理想的商用催化剂。