微波诱导SiC改性Co-Ce/Al2O3催化剂催化氧化甲苯性能的研究

采用共沉淀法制备SiC改性5%Co-2.5%Ce/Al₂O₃催化剂,研究了不同SiC负载量改性催化剂的吸波升温性能和催化氧化甲苯性能。结果表明,随着SiC负载量的增加,催化剂吸波升温性能逐渐增强。SiC最佳负载量为5%时,催化剂催化氧化甲苯性能最佳,催化剂具有较大的比表面积和适宜的微孔结构。甲苯催化氧化活性评价结果表明,5%Co-2.5%Ce/5%SiC-Al₂O₃催化剂对不同甲苯浓度具有较强适应性,对中低浓度的甲苯降解效果显著。空速低于15 000 h^-1时催化剂能发挥高效催化作用,微波功率在120～385 W有利于甲苯的催化氧化。     

甲烷在Cr改性Pd/Al2O3催化剂上的催化燃烧性能

研究了Cr改性Pd/Al2O3催化剂上低浓度甲烷的催化燃烧反应,考察了载体Cr Al的制备方法和活性组分Pd的负载方法对催化剂催化活性的影响以及添加Ce对催化剂高温稳定性的影响。采用X射线衍射、程序升温还原等表征手段分析了催化剂结构和氧化还原性。结果表明,与采用沉淀法制备的载体P-Cr Al相比,采用浸渍法制备的载体I-Cr Al具有较高的比表面积和反应活性;用Na BH3对Pd负载过程进行还原处理能明显提高催化剂活性,其原因是还原过程加强了催化剂上Pd与载体Cr Al之间的作用,通过H2-TPR证明了其还原能力得到了增加;添加Ce缓解了Al2O3高温条件下的烧结,增强了催化剂的高温稳定性。     

载体焙烧温度对Co/Al2O3催化剂F-T合成反应催化性能的影响

采用等体积浸渍法,以不同温度焙烧的Al2O3为载体制备Co/Al₂O₃催化剂,通过N₂物理吸附、X射线衍射和程序升温还原等方法对催化剂进行表征,并在固定床反应器中评价催化剂的F-T合成反应性能。结果表明,低温焙烧可获得较大比表面积的Al₂O₃载体,有利于提高活性组分的分散度,但增强了钴与载体之间的相互作用,降低催化剂活性和选择性。高温焙烧的Al2O3载体有利于提高C⁺₅选择性,尤其是柴油组分的选择性。     

氮掺杂Pd-Cu/Al2O3催化剂富氢气氛下CO优先氧化性能

以Al₂O₃为载体,采用共浸渍法制备Pd-Cu/Al₂O₃和Pd-Cu-N/Al₂O₃催化剂。利用连续流动微反应装置考察氮掺杂对Pd-Cu/Al₂O₃催化剂低温富氢气氛下CO优先氧化性能的影响,结合XRD、FT-IR、H₂-TPR和XPS等手段对催化剂进行表征。结果表明,相较于Pd-Cu/Al₂O₃,Pd-Cu-N/Al₂O₃具有更好的CO优先氧化性能。氮掺杂促进了表面Cu₂Cl(OH)₃的分散,增强了Pd和Cu之间的相互作用,提高了Pd和Cu₂Cl(OH)₃的氧化还原能力。同时,氮掺杂也有利于生成更多的表面活性Cu⁺物种,并且部分进入Pd晶格,抑制了反应过程中PdHx的形成,从而使催化剂催化性能...     

氧化还原法制备Mn3O4催化剂及其甲苯催化氧化性能与机理研究

在氧化还原法制备α-MnO₂的基础上,通过控制焙烧温度和气氛制备了Mn₃O₄催化剂,系统考察了其甲苯催化性能。结果显示,Mn₃O₄催化性能优于MnO₂,并且在230℃下保持转化率90%以上稳定运行100 h。原位红外等表征结果表明,与MnO₂相比,Mn₃O₄具有适当的氧化还原能力、更高的晶格氧活性、更多的表面吸附氧和更强的甲苯吸附能力,促使催化剂表面苯甲酸物种的快速转化,进而提高其甲苯催化性能。本研究可为锰基催化剂的制备及其甲苯催化氧化性能提升机理研究提供参考。     

TiOF2纳米催化剂的制备及催化臭氧氧化性能

以钛酸丁酯、氢氟酸为主要原料,通过水热法制备了纳米Ti OF₂臭氧氧化催化剂。利用XRD、FT-IR、SEM、XPS对合成的样品进行表征,苯胺作为目标污染物进行催化性能测试。成功制备了球花状Ti OF₂纳米催化剂,其粒径为180～200 nm,比表面积为105.38 m²/g。碱性环境可以促进反应进行,OH^-可以使反应正向进行促进污染物降解,过量的催化剂不利于反应进行,催化剂投加质量浓度高于0.6 g/L时会因团聚导致降解率下降。在催化剂投加质量浓度为0.6 g/L,初始COD为250 mg/L,臭氧流量为0.1 L/min,p H=10时,反应80 min后,降解率达到了98.83%。球花状Ti OF₂由纳米片拼插形成,这种结构为催化剂提供了复杂的表面,使催化剂具有较大的比表面积,暴露更多的活性位点,为反应提供更多的反应场所。F^-使催化剂中生成氧空位和Ti³⁺,更利于吸附H₂O形成表面—OH基团,便于吸附解离水...     

高活性CuO/Al2O3催化剂的制备及加氢性能研究

负载型催化剂中表面活性组分的分散度影响催化剂的性能,因此,合理调控合成条件提高活性组分分散度是高效催化剂开发的有效策略。通过控制焙烧条件(氛围、温度、时长)制备了多种负载型铜基催化剂(CuO/Al₂O₃),利用SEM和XRD研究了合成条件对催化剂结构和表面组成的影响,考察了所制备催化剂在对硝基苯酚(4-NP)催化加氢反应中的性能。研究结果表明,在250℃、N₂氛围中热处理6 h所制备的催化剂在3 min内即可实现4-NP及其他芳香族硝基化合物90.5%的催化加氢效率。此外,该催化剂循环利用5次仍有较高的活性,在实际工业生产中具有巨大的应用潜力。     

CuO/γ-Al2O3/SiO2催化剂制备及其苯酚废水催化降解性能

以拟薄水铝石、SiO₂微球颗粒和纳米CuO为原料,经有机溶剂分散粘结、相转化和焙烧成型制备了CuO/γ-Al₂O₃/SiO₂负载型催化剂。采用SEM,XRD,BET和ICP对负载型催化剂进行表征和组成分析。在不同浓度、pH、温度和盐浓度下,测试了负载型催化剂对废水中难降解酚类物质的催化氧化效果。经60℃下2 h催化氧化处理后,100 mg/L COD的苯酚降解率可达81.79%,出水COD低至19.00 mg/L,因而可应用难降解废水处理。     

负载型CeO_2/OMS-2催化剂对VOCs的催化氧化性能

采用回流法合成了OMS-2,同时以OMS-2为载体,采用浸渍法负载CeO_2制备了Ce/OMS-2催化剂,运用X射线衍射、拉曼光谱、BET、H_2-TPR和NH_3-TPD等方法对催化剂进行表征,并考察CeO_2/OMS-2催化剂催化氧化二氯甲烷和乙酸乙酯的性能。结果表明,CeO_2的加入并未改变OMS-2较好的八面体分子筛结构,CeO_2的晶粒很小且以高分散的形式存在;负载CeO_2的OMS-2催化剂比表面积都有增大趋势;随着CeO_2负载量的增加,低温和高温的还原峰都先向低温方向偏移再向高温方向偏移;随着CeO_2负载量的增加,高温处强酸性峰先向低温方向偏移再向高温方向偏移。反应活性结果表明,CeO_2/OMS-2催化剂活性比载体OMS-2的活性好,随着铈负载量的增加,催化活性先升高再降低,其中,CeO_2负载质量分数为1.0%(1.0Ce/OMS-2)时催化剂效果最好,这可能是由于铈的加入活化了OMS-2中的氧,影响了整体催化剂的酸性,进而影响反应性能。     

二氯甲烷在CrO3／Al2O3和Pd／Al2O3催化剂上的催化氧化

二氯甲烷在ＣｒＯ_３／Ａｌ_２Ｏ_３和Ｐｄ／Ａｌ_２Ｏ_３催化剂上的催化氧化张立庆（杭州应用工程技术学院化工系杭州３１００１２）姜玄珍，莫亦平（浙江大学化学系杭州３１００２７）关键词二氯甲烷；催化降解；负载型催化剂１引言随着有机化工，氯制品化工的迅速发展?..     

Catalytic Oxidation of Methanol by Aqueous POM on Al2O3 Supported Catalysts and Electrochemical Performance of POM

Phosphomolybdic acid (H₃PMo₁₂O₄₀, POM) was attempted to be used as the energy‐storage agent in this paper to avoid some problems of the direct methanol fuel cell (DMFC), such as catalyst poisoning and methanol permeation. Catalytic oxidation of methanol by aqueous POM on Al₂O₃ supported catalysts with Pt and Ru active metal was evaluated in the presence of liquid water. The process takes advantage of the high catalytic activities of platinum for methanol oxidation. The effects of temperature, reaction time, and methanol concentration on activity were observed. The catalytic activity of Pt/Al₂O₃ is better than that of Ru/Al₂O₃ for the oxidation of methanol by POM. The methanol conversion rate reached 93.55% on the Pt/Al₂O₃ at 80 °C after reaction for 1 h. The electrochemical experiments indicate that POM shows a larger current density in redox processes on an Au electrode than methanol. The redox process of reduced POM is a reversible multi‐electron transfer process.     

Characterization and Catalytic Performance of PtSn Catalysts Supported on Al2O3 and Na-doped Al2O3 in n-butane Dehydrogenation

PtSn/Al₂O₃ and PtSn/Al₂O₃–Na catalysts display important modifications of the metallic phase with respect to Pt/Al₂O₃ one. In this sense, TPR and XPS results show the presence of strong interactions between Pt and Sn, with probable alloy formation, which would be responsible for the decrease of the reaction rate and the increase of the activation energy in cyclohexane dehydrogenation. Besides the experiments of cyclopentane hydrogenolysis show that the alkali metal addition to bimetallic PtSn/Al₂O₃ catalysts completely eliminates the hydrogenolytic ensembles, which could be due to a geometric modification of the metallic phase. These important modifications in the nature of the metallic function due to the simultaneous addition of Na and Sn to Pt/Al₂O₃ are responsible for the excellent catalytic performance in the n-butane dehydrogenation, thus giving high conversions, selectivities to butenes higher than 95%, and lower deactivation capacity than those corresponding to bimetallic PtSn catalysts (with different Sn contents) supported on undoped alumina. The excellent stability of PtSn/Al₂O₃–Na catalysts would be due to a low carbon formation during the reaction, such as it was observed from pulse experiments.     

负载型MoO_3/SiO_2催化合成乙酸乙酯

采用等体积浸渍法制备了MoO3/SiO2负载型催化剂,并用于催化乙醇和乙酸的酯化反应。考察了催化剂的制备条件及反应条件对醋酸转化率的影响。结果表明,催化剂适宜的制备条件为焙烧温度450℃,焙烧时间4 h,MoO3负载量为20%;适宜的反应条件为反应时间3 h、原料醇酸比为1.4︰1、催化剂用量为醋酸质量的1.9%,醋酸的转化率为79%,乙酸乙酯的选择性为100%,催化剂可重复使用。     

免焙烧对FCC汽油选择性加氢脱硫CoMo/Al_2O_3催化剂性能的影响

在相同的其它条件下制备了用于流化催化裂化(FCC)汽油选择性加氢脱硫的免焙烧和焙烧的CoMo/Al_2O_3催化剂,并用扫描电镜(SEM)、X射线衍射(XRD)、红外光谱(FT-IR)等对其进行了比较性地表征和评价。结果表明,免焙烧催化剂的酸量大于焙烧催化剂的,焙烧与否对催化剂的酸类型几乎没有影响,这两类催化剂的酸中心均主要为L酸;免焙烧Co-Mo/Al_2O_3催化剂的活性组分与载体间的相互作用较弱,进而使活性组分颗粒的颗粒团聚程度降低、分布趋于均匀和易于被还原。在所考察的评价条件范围内。免焙烧Co-Mo/Al_2O_3催化剂的催化性能优于焙烧Co-Mo/Al_2O_3催化剂的。     

遗态 Al2O3-AlClx-3 材料的制备、表征及其对醇的催化氧化

以脱脂棉纤维为模板,运用模板法和化学剪裁法制备了多孔管状催化剂Al2O3-AlCl x-3,采用电场发射扫描电镜和光电子能谱对催化剂进行了表征。结果表明,该催化剂较好地复制了棉纤维的宏观和微观结构,呈现出明显的生物形貌特征。将Al2O3-AlCl x-3催化剂用于醇氧化反应,考察了溶剂体系、催化剂用量、反应温度及时间等因素对反应性能的影响。实验发现,在最优条件下Al2O3-AlCl x-3催化下可以高选择性地将醇氧化为相应的醛或酮,且该催化剂具有很好的重复使用性能,并提出了可能的反应机理。     

Ni/ZrO2/Al2O3催化剂在CO2重整CH4反应中催化性能研究

Ni/ZrO2/Al2O3催化剂在二氧化碳重整甲烷反应中,其催化活性和稳定性均优于Ni/ZrO2和Ni/Al2O3催化剂.XRD、TPD、TPR结果表明,在Ni/ZrO2/Al2O3催化剂上能形成较稳定的活性中心,负载型纳米ZrO2/Al2O3复合载体中,ZrO2以四方相形式出现,粒径为5 nm,微波和超声波的作用能诱导ZrO2和Al2O3产生新的碱性中心,有利于二氧化碳的吸附和提高活性组分的分散度.TG-DSC结果表明Ni/ZrO2/Al2O3催化剂上表面炭主要是活性较高的α炭,而Ni/ZrO2和Ni/Al2O3催化剂表面炭主要是活性较低的β炭和γ炭.     

PtSnLi/Al_2O_3催化剂在丙烷脱氢过程中的氢气选择氧化性能

采用浸渍法制备氧化铝负载三元Pt-Sn-Li催化剂(PtSnLi/A_2O_3),采用X射线衍射(XRD)、透射电镜(TEM)和物理吸附(BET)等手段对催化剂进行表征,并在固定床反应器中评价了该催化剂在丙烷脱氢过程中对氢气选择氧化性能。结果表明,PtSnLi/Al_2O_3催化剂对氢气具有良好的选择氧化性,组分Sn和Li的加入能有效提高Pt基催化剂活性和选择性。PtSnLi/Al_2O_3催化剂在常压、550℃和质量空速为1.45 h~(-1)的条件下,氢气的选择氧化性为80%,氧气转化率大于98%,烃类损耗量0.2%。与PtSn/Al_2O_3相比,氧气转化率基本相同,氢气的选择氧化增加了29.2%,烃损耗率降低了0.9%。     

Performance of CuO/Al2O3 Catalysts Promoted by SnO2 and ZrO2 in the Selective Oxidation of Carbon Monoxide

The effect of added SnO₂ and ZrO₂ to CuO/Al₂O₃ catalysts was investigated with reference to the oxygen spillover phenomena in the selective oxidation of carbon monoxide. The TPR and TPO analyses indicated that SnO₂ and ZrO₂ addition caused oxygen migration and induced the formation of high concentrations of active oxygen species on the SnO₂ and ZrO₂ surface. The catalytic activities of SnO₂ and ZrO₂ supported CuO/Al₂O₃ catalysts were superior to that for CuO/Al₂O₃ catalysts in the selective oxidation of carbon monoxide. Oxygen, when absorbed to the SnO₂ and ZrO₂ surface can spill over to the CuO phase and easily react with carbon monoxide. Consequently, the addition of SnO₂ and ZrO₂ led to significantly improved activities. This can be attributed to the enhanced migration of oxygen to the catalyst surface.     

Ethylene Hydrogenation over Pt/Ga2O3/Al2O3 Catalysts

The effects of gallia addition on the Pt dispersion and the activity for ethylene hydrogenation at 0 °C were studied for Pt-supported catalysts as a function of the reduction temperature (350, 450, and 550 °C). The catalysts contained 0.5 wt.% Pt and were prepared by successive incipient wetness impregnations with Ga(NO₃)₃ and H₂PtCl₆ aqueous solutions. CO and H₂ chemisorption data indicated that, the addition of small amount of Ga₂O₃ caused an increase of the Pt dispersion and a decrease of ethylene conversion. Both of them decreased appreciably when Ga₂O₃ addition was increased, particularly, for the case where β-Ga₂O₃ was used as a support. The increase in reduction temperature magnified the negative effects of the gallia addition on dispersion and activity, although the addition of small amount of gallia improved the resistance to metal sintering. Results were interpreted in terms of the presence of reduced Ga species, which can encapsulate Pt particles.