CuO对贵金属/CeO_2/Al_2O_3催化剂的作用

制备含少量贵金属Ｐｔ、Ｐｄ 的不同Ｃｕ 和Ｃｅ摩尔含量比（０∶１０，１∶９，２∶８）的催化剂，实验条件下加入ＣｕＯ可以提高Ｐｔ催化剂的二效活性；加入Ｃｕ∶Ｃｅ＝ ２∶８ 的ＣｕＯ降低了Ｐｄ 催化剂的三效性能，然而Ｃｕ∶Ｃｅ＝ １∶９时可以改善Ｐｄ 催化剂的三效催化性能⒚通过结构分析，认为ＣｕＯ的存在可以提高Ｐｄ 催化剂的比表面积，改善ＰｄＯ的分散度     

掺杂ZrO2、TiO2、γ－Al2O3对Pt、Pd／Al2O3燃烧

运用ＸＲＤ、ＢＥＴ、ＤＴＡ等测试技术，研究并考察了掺杂ＺｒＯ２，ＴｉＯ２，ｒ－Ａｌ２Ｏ３对Ｐｔ－Ｐｄ．Ａｌ２Ｏ３燃烧催化剂性能的影响，结果表明，ＺｒＯ２对Ａｌ２Ｏ３晶相的γ型转为α型有明显的抑制作用，而ＴｉＯ２的添入则起促进作用。     

钯、铜、锰、铈三效催化剂性能研究

应用脉冲－火焰反应装置、ＸＲＤ、ＴＰＲ和氢氧滴定技术来研究Ｐｄ－Ｃｕ－Ｍｎ－Ｃｅ－Ｏ三效催化剂的性能。实验结果表明，不同的制备Ｐｄ－Ｃｕ－Ｍｎ－Ｃｅ－Ｏ催化剂的方法，则催化活性各不相同。在分层制备的催化剂中，催化性能主要以外层组分性能为主；以混合浸渍法制备的样品中，ＣｕＭｎ＿２Ｏ＿４相消失，Ｃｕ－Ｍｎ－Ｃｅ－Ｏ表面氧环境发生变化；表面活性剂的添加改变了Ｐｄ的分布，使催化剂表面易于还原；这些改变均对催化剂的三效性能发生影响。催化剂表面的有效贮氧量与三效活性没有明显的关系。     

催化加氢转化CO2的研究

研究催化加氢法转化ＣＯ２,在Ｆｅ／ＡＣ催化剂上采用不同的反应条件,可将ＣＯ２分别转化成低碳烯烃,液化石油气和液态烃,其转化率均在４０％－５０％之间。在Ｃｕ－Ｚｎ－分子筛催化剂上,３５％ＣＯ２可被转化成二甲醚;在Ｒｈ－Ｖ／ＳｉＯ２催化剂上,ＣＯ２可被转化成乙醇,其单程转化率在５％以上。     

烟气中SO2/NOx同时吸收催化脱除的研究

根据同时脱硫脱硝的要求,对以ＣＵＯ为主要活性组分催化剂的制备和反应过程进行研究,活性测试的结果表明,催化剂的最佳活化温度和活化时间分别为４５０℃和２ｈ。当反应温度为４００℃,空间速度为２×１０＾４ｈ＾－１以及ＣｕＳＯ４／ＣｕＯ摩尔比和Ｃｕ／Ｓ分别保持在１．４６和０．８３以上时,ＳＯ２和ＮＯｘ的脱除率可达９０％以上。     

载体对负载钯催化剂的CO氧化活性的影响

采用ＣＯ－ＴＰＳＲ和ＣＯ氧化活性测试等方法考察了不同载体对Ｐｄ催化剂的ＣＯ表面氧化性能的影响，结果表明，载体对Ｐｄ催化剂的ＣＯ氧化性能、ＣＯ吸附能力影响很大，ＣＯ的吸附能力顺序为Ｐｄ／ＣｅＯ２（吸附量、０．５９ｍｌ／１００ｍｇ）〉Ｐｄ／Ａｌ２Ｏ３（吸附量：０．０５２ｍＬ／１００ｍｇ）〉Ｐｄ／ＴｉＯ２（吸附量：０．００１ｍＬ／１００ｍｇ），催化剂的ＣＯ氧化活性与ＣＯ吸附能力有很好的对应关系，尤其是Ｐ     

CO2催化氢化研究--REY负载双金属催化剂的催化作用

用高压釜实验评价了用离子交换法制备的负载于ＲＥＹ和ＺＳＭ－５分子筛上的多种过渡金属对ＣＯ２加氢合成醇和甲烷化的催化活性。实验结果表明,双金属催化剂的活性按下列顺序降低,ＣＯ２甲烷化;Ｒｕ＞ＮｉＲｕ＞ＮｉＰｄ＞ＮｉＩｒ;合成醇：ＮｉＣｕ＞Ｎｉ＞ＮｉＭｎ＞ＮｉＣｏ。用２％Ｒｕ／ＲＥＹ催化剂,在４７３Ｋ,３．９ＭＰａ,ＣＯ２／Ｈ２＝１／５,反应时间２０ｈ条件下,７６％的ＣＯ２转化为甲烷。反应温度,压力和     

汽车尾气净化剂的发展,现状及前景

催化净化是控制汽车尾气污染的主要手段。文章介绍了汽车尾气催化剂的发展过程：描了了当今普遍使用的三效转化催化剂“提出了未来尾气净化催化剂的发展趋势及需要解决的问题，ＴＷＣ催化剂是以贵金属Ｐｔ，Ｐｄ和Ｒｈ为适性组元，引入Ｃｅ，Ｌａ，Ｂａ和Ｚｒ等为助剂，担载在高比表面物质上制备面成一的类性能优虹的催化剂，它能对尾气中的３种主要有害物质ＮＯｘ，ＣＯ和ＨＣ同时进行转化。     

PrO/γAl2O3等稀土氧化物催化还原SO2的研究

进行了负载于氧化铝上的镨，钕，锌，镧，钐等稀土氧化物上，ＣＯ，ＣＨ３及Ｈ２催化还原ＳＯ２反应的研究。实验着重考察了Ｐｒ－Ｏ／γ－Ａｌ２Ｏ３上ＣＯ２催化还在ＳＯ２的反应，测定了不同反应温度，不同反应物配比及不同空速下的活性，同时对Ｐｒ－ｏ／γ－Ａｌ２Ｏ３催化剂进行了ＴＰＤ，ＴＧ，ＸＲＤ，ＸＰＳ表征。结果表明，稀土氧化物具有非常高的ＣＯ催化还原ＳＯ２反应的活性，在５００℃，ＣＯ：ＳＯ２＝２：１，空速比     

Fe2O3对型煤固硫作用的机理探讨

根据煤中硫的着火点,发现硫的固定主要发生在温度低于５００℃的阶段,升温时间应小于３０ｍｉｎ,Ｆｅ２Ｏ３用量增多,ＣａＳＯ３转化生成ＣａＯ＋ＳＯ２＋０．５Ｏ２→ＣａＳＯ４的反应来模拟实际的煤燃烧时硫的固定过程,发现Ｆｅ２Ｏ３的加入对硫的固定起着较大的促进作用,而且Ｆｅ２Ｏ３主要是促进ＣａＯ＋ＳＯ２→ＣａＳＯ３这一反应过程。     

Effects of Ce on catalytic combustion of methane over Pd-Pt/Al2O3 catalyst

Activity and stability of 1%Pd-0.2%Pt/Al₂O₃ and 1%Pd-0.2%Pt/0.6%Ce/Al₂O₃ catalysts prepared by impregnation method for catalytic combustion of methane in air were investigated. The catalysts before and after reaction were characterized by BET, CO chemisorption, XRD and XPS techniques. Results showed that the presence of Ce significantly increased the activity and thermal stability of the Pd-Pt/Al₂O₃ catalyst towards methane combustion, which could be attributed to more highly-dispersed active PdO particles over the Pd-Pt/Ce/Al₂O₃ catalyst surface as well as the retarded sintering of PdO and the maintained oxidized state of surface Pd during the combustion process in the presence of Ce.     

Mo-modified Pd/Al2O3 catalysts for benzene catalytic combustion

Mo-modified Pd/Al2O3catalysts were prepared by an impregnation method and tested for the catalytic combustion of benzene. The catalysts were characterized by N2 isothermal adsorption, X-ray diffraction（XRD）, X-ray photoelectron spectroscopy（XPS）, temperatureprogrammed desorption of NH3（NH3-TPD）, H2temperature-programmed reduction（H2-TPR）, and high-angle annular dark-field scanning transmission electron microscopy（HAADF-STEM）. The results showed that the addition of Mo effectively improved the activity and stability of the Pd/Al2O3catalyst by increasing the dispersion of Pd active components, changing the partial oxidation state of palladium and increasing the oxygen species concentration on the surface of catalyst. In the case of the Pd-Mo/Al2O3catalyst,benzene conversion of 90% was obtained at temperatures as low as 190°C, which was 45°C lower than that for similar performance with the Pd/Al2O3catalyst. Moreover, the 1.0% Pd-5% Mo/Al2O3catalyst was more active than the 2.0% Pd/Al2O3catalyst. It was concluded that Pd and Mo have a synergistic effect in benzene catalytic combustion.     

Effect of pretreatment on Pd/Al2O3 catalyst for catalytic oxidation of o-xylene at low temperature

The effect of pretreatment on Pd/Al₂O₃ catalysts for the catalytic oxidation of o-xylene at low temperature was studied by changing the pretreatment and testing conditions. The fresh and pretreated Pd/Al₂O₃ catalysts were characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD). The results showed that the pretreatment dramatically changed the Pd/PdO ratio and then significantly affected the Pd/Al₂O₃ activity; while the pretreatment had not much influence on Pd particle size. The Pd/Al₂O₃ pre-reduced at 300℃/400℃, which has fully reduced Pd species, showed the highest activity; while the fresh Pd/Al₂O₃, which has fully oxidized Pd species, presented the worst performance, indicating the Pd chemical state plays an important role in the catalytic activity for the o-xylene oxidation. It is concluded that metallic Pd is the active species on the Pd/Al₂O₃ catalyst for the catalytic oxidation of o-xylene at low temperature.     

Pd/CZ/Al2O3催化剂的制备、表征与三效催化性能

以共浸渍法制得的氧化铝负载铈锆固溶体为载体,并浸渍贵金属Pd得到了Pd/CZ/Al₂O₃催化剂.实验结果表明,该催化剂在老化前后都表现出良好的三效催化活性,新鲜样品Pd/CZ/Al₂O₃活性与Pd/CZ相当,老化后样品前者优于后者.结合XRD,BET,TPR等表征手段,讨论了Pd/CZ/Al₂O₃的催化活性特别是高温老化后活性与其组成结构之间的内在关系,揭示了其老化后仍具有较高活性的主要原因在于保持了Pd与CZ/Al₂O₃复合载体之间的强相互作用(SMSI).     

Catalytic activity of cerium-doped Ru/Al2O3 during ozonation of dimethyl phthalate

In this paper, factors influencing the mineralization of dimethyl phthalate (DMP) during catalytic ozonation with a cerium-doped Ru/Al₂O₃ catalyst were studied. The catalytic contribution was calculated through the results of a comparison experiment. It showed that doping cerium significantly enhanced catalytic activity. The total organic carbon (TOC) removal over the doped catalyst at 100 min reached 75.1%, 61.3% using Ru/Al₂O₃ catalyst and only 14.0% using ozone alone. Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto Al₂O₃ support. Results of experiments on oxidation by ozone alone, adsorption of the catalyst, Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%, which showed the obvious effect of Ru-Ce/Al₂O₃ on catalytic activity. __________ Translated from China Environmental Science, 2006, 26(4): 445–448 [译自: 中国环境科学]     

Nano-sized alumina supported palladium catalysts for methane combustion with excellent thermal stability

Pd/Al₂O₃ catalysts supported on Al₂O₃ of different particle sizes were synthesized and applied in methane combustion. These catalysts were systematically characterized by Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD), high resolution-transmission electron microscopy (HR-TEM), high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), H₂-temperature-programmed reduction (H₂-TPR), O₂-temperature-programmed oxidation (O₂-TPO), X-ray photoelectron spectroscopy (XPS), and X-ray absorption fine structure (XAFS). The characterization results indicated that nano-sized Al₂O₃ enabled the uniform dispersion of palladium nanoparticles, thus contributing to the excellent catalytic performance of these nano-sized Pd/Al₂O₃ catalysts. Among them, Pd/Al₂O₃-nano-10 (Pd/Al₂O₃ supported by alumina with an average particle size of 10 nm) showed superior catalytic activity and stability for methane oxidation under harsh practical conditions. It maintained excellent catalytic performance for methane oxidation for 50 hr and remained stable even after harsh hydrothermal aging in 10 vol.% steam at 800°C for 16 hr. Characterization results revealed that the strong metal-support interactions and physical barriers provided by Al₂O₃-nano-10 suppressed the coalescence ripening of palladium species, and thus contributed to the superior sintering resistance of the Pd/Al₂O₃-nano-10 catalyst.     

Effect of Ce doping of TiO2 support on NH3-SCR activity over V2O5-WO3/CeO2-TiO2 catalyst

CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction（SCR） of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping（molar ratio of Ce/Ti = 1/10） in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.     

Effect of CeO2 and Al2O3 on the activity of Pd/Co_3O_4/cordierite catalyst in the three-way catalysis reactions (CO/NO/CnHm)

The present article studies the effect of CeO₂ and Al₂O₃ on the activity of Pd/Co₃O₄/cordierite catalyst in conversion of NO, CO, C_nH_m. The catalysts were characterized by temperature programmed reduction with hydrogen, X-ray diffraction, X-ray photoelectron spectroscopy and transmission electron microscopy. It is shown that the effect of CeO₂ on the properties of Pd/Co₃O₄/cordierite catalyst depends on preparation method. The catalyst obtained by co-deposition of cerium and cobalt oxides has higher activity in CO oxidation (CO + O₂ and CO + NO) and total hexane oxidation (C₆H₁₄ + O₂). Such phenomenon is probably caused by more than stoichiometric amount of formed oxygen vacancies, an increase in both mobility of surface oxygen and dispersity of components in the catalytic composition. It is demonstrated that CeO₂ addition promotes the SO₂ resistance of Pd/Co₃O₄/cordierite. The second support decreases the activity of Pd/Co₃O₄/cordierite catalyst in the reactions of CO and C₆H₁₄ with oxygen because of CoAl₂O₄ formation.     

Toward cleaner production of hydrogen peroxide in China

Industrial production of hydrogen peroxide by anthraquinone (AO) process in China was briefly introduced. The pathways for cleaner production of hydrogen peroxide were discussed in detail from the viewpoint of process development and design, these included the replacement of Raney-Ni catalyst by highly active and highly selective Pd/Al₂O₃ catalyst, the reduction of raw materials, steam and power consumption, the usage of high boiling point, low water-soluble and low toxic solvents, the regeneration of degradations, the proper treatment of waste gas, water and solids. Because of these innovations and improvements, the AO process with Pd/Al₂O₃ catalyst for producing hydrogen peroxide was certified as a cleaner production technology by the Chinese government.     

Cu-Al2O3中骨架铜类芬顿催化去除水中有机污染物

为解决传统铁基芬顿催化剂在水体通常酸碱(pH6)条件下活性低的问题,采用简单共沉淀法制备了Cu掺杂的Al_2O_3类芬顿催化剂.通过X射线衍射(XRD)、X射线光电子能谱(XPS)和紫外可见(UV-vis)吸收光谱分析表明,Cu-Al_2O_3中铜掺杂的质量分数低于4.77%时,催化剂中铜主要以Cu~(2+)和Cu~+的形式共存于Al_2O_3的骨架结构中,形成Al—O—Cu键;过量的铜掺杂会导致外骨架铜物种如铜氧化物团簇的存在.以难降解有机污染物2-氯苯酚(2-chlorophenol,2-CP)和染料罗丹明B(Rhodamine B,Rh B)为目标污染物,对Cu-Al_2O_3的类芬顿催化性能进行了详细地研究.结果表明,骨架铜物种在中性温和条件下对2-CP和Rh B显示出很高的催化去除效率和稳定性,反应2 h,Cu-Al_2O_3(Cu质量分数4.77%)对2-CP的去除率达到54%,相应的TOC去除率达到49%,而铜离子溶出浓度仅为0.025 5 mg·L-1,而Cu-Al_2O_3(Cu质量分数7.58%)由于外骨架铜的存在导致催化活性增加缓慢和稳定性下降.ESR测试结果表明,·OH和HO_2~-/O_2~-·是反应中主要的活性物种.