Catalytic combustion properties of nanocomplex oxide for natural gas

The catalysts of copper oxide supported on cerium dioxide were prepared by different methods for methane catalytic combustion. The effects of copper content in the catalysts and calcination temperatures of the catalysts on the catalytic activity are investigated. Results show that the complex oxide catalyst exhibits high catalytic activity for methane combustion due to the synergistic effect of CuO and CeO₂. The catalyst prepared by impregnation is more active than that prepared by controlled coprecipitation even if CuO content is the same. When W(CuO)<13%, the light-off temperature and full conversion temperature for the CH₄ reaction decrease with the increasing of CuO content in the catalysts. However, when the copper content is above 13%, the excess CuO has a negative effect on the catalytic activity owing to the formation of bulk CuO particles. A proper calcinations temperature of 650 ℃ can lead to a high dispersion of CuO and accordingly can enhance the catalytic activity of the composites.     

Synthesis of a novel triple-site diphosphinoamine （PNP） ligand and its applications in ethylene tetramerization

A novel triple-site diphosphinoamine （PNP） ligand was synthesized and characterized. In combination with Cr（Ⅲ） and methylaluminoxane （MAO）, it generated active catalytic systems for ethylene tetramerization toward 1-octene with high catalytic activity and long lifetime. The effects of reaction temperature, molar ratio of AI/Cr and molar ratio of ligand/Cr on catalytic activity and selectivity to 1-octene were studied with reaction kinetics of the catalytic system for ethylene tetramerization described. At the AI/Cr molar ratio of 100, the catalytic activity is up to 2.29×10^6 g· mol^-1 （Cr）· h^-1 and the selectivity to 1-octene is 49.65 wt%.     

Fe3O4@C nanoparticles as high-performance Fenton-like catalyst for dye decoloration

Water pollution has become serious environmental problem nowadays. Advanced oxidation processes(AOP) have been widely applied in water treatment.However, traditional Fenton reaction based on Fe2﹢-H2O2 system has obvious drawbacks, which limit its applications In this study, magnetic Fe3O4core-C shell nanoparticles(Fe3O4@C NPs) were prepared for the decoloration of methylene blue(MB) via the co-precipitation followed by the hydrothermal dehydrogenation of glucose. Fe3O4@C NPs showed high catalytic activity of the decoloration of MB through the decomposition of H2O2 in Fenton-like reactions. Fe3O4@C NPs had much higher activity than bare Fe3O4 cores, suggesting the coating of carbon enhanced the catalytic activity. The performance of Fe3O4@C NPs was better at lower pH and higher temperature, but was significantly inhibited in the presence of radical scavenger tertiary butanol. Fe3O4@C NPs could be magnetic separated and regenerated, and maintained with very good catalytic activity. The implication for the applications of Fe3O4@C NP-catalyzed Fenton-like reactions in water treatment was discussed.     

Preparation of 1-octene by ethylene tetramerization with high selectivity

Two novel PNP ligands have been synthesized and characterized by ^1H-NMR, elemental analysis, and mass spectra. In combination with Cr（Ⅲ） and cocatalyst MAO, they generate active catalytic systems that tetramerize ethylene with both high catalytic activity and high selectivity to produce 1-octene. The results show that these catalyst systems are able to catalyze ethylene tetramerization, with high catalytic activity up to 0.89×10^6 g/mol Cr.h, and the selectivity of C8 in products is 72.52%, and the percentage of 1-olefins in the C8 cut is 97.87%.     

Effect of B sites on the catalytic activities for perovskite oxides La_(.6)Sr_(.4)Co_xFe_(1-x)O_(3-δ) as metal-air batteries catalysts

The effect of B sites on the catalytic activities of oxygen evolution reaction(OER)for perovskite oxides La_(0.6)Sr_(0.4)Co_xFe_(1-x)O_(3-δ)(x=0,0.2,0.4,0.6,0.8,1,denoted as LSF,LSCF-28,LSCF-46,LSCF-64,LSCF-82 and LSC,respectively)prepared by a convenient and simple method of electrospinning technique is reported.The prepared La_(0.6)Sr_(0.4)Co_xFe_(1-x)O_(3-δ)catalysts possess almost same crystal structures,similar morphologies(except for the LSC catalyst)and slightly different BET surface areas.Upon the optimization of the Co/Fe atomic ratio,the optimal LSCF-82 catalyst exhibits the OER performance with a low onset potential of 1.541 V,a small Tafel slope of 80.56 mV dec~(-1),a high charge-transfer rate and a large electrochemical surface area in 0.1 M KOH solution.LSCF-82 catalyst exhibits the long-term stability under the catalytic operation condition for 12 h.Such catalytic activity may mainly cause by the synergy of higher catalytic activity Co and lower catalytic activity Fe.Thus,the reasonable optimization of the transition metal composition in B sites for the perovskite oxides is in favor of the improvement of OER performance.     

Preparation and Catalytic Oxidation Activity on 2-mercaptoethanol of a Novel Catalytic Cellulose Fibres

Cobalt tetra(N-carbonylacylic) aminophthalocyanine was supported on cellulose fibres by graft reaction to obtain a novel polymer catalyst, catalytic cellulose fibres (CCF),and the optimal supporting conditions were pH = 6, 80℃,t = 120 min. The catalytic oxidation activity of CCF towards oxidation of 2-mereaptoethanol (MEA) in aqueous solution was investigated. The experimental results demonstrated that CCF had good catalytic oxidation activity on MEA at room temperature, causing no secondary pollution and remaining efficient for the repetitive tests with no obvious decrease of catalytic activity.     

Ethylene tetramerization with a highly active and long-lifetime trinuclear diphenylphosphinoamine/Cr（III）/MAO catalyst

The synthesis and characterization of a novel trinuclear diphosphinoamine ligand 2 are reported. The ligand combined with Cr(III), activated with methylaluminoxane, lead to highly active and long-lifetime catalytic systems for the tetramerization of ethylene to form 1-octene. The effects of reaction temperature, reaction pressure, molar ratio of Al/Cr and bis(diphenylphosphino)amine/Cr on the catalytic activity and product selectivity were studied. Compared with its mononuclear analogue 1, ligand 2 showed a higher catalytic activity and longer lifetime for ethylene tetramerization in the presence of methylaluminoxane as cocatalyst. High molecular weight polyethylene was generated as a by-product with extremely broad molecular weight distributions.     

A novel method for preparing platinized counter electrode of nanocrystalline dye-sensitized solar cells

The platinized FTO glass counter electrode was prepared by employing techniques of colloid preparation, Langmuir-Blodgett film and serf-assembly. The present electrode had very low platinum loading, high catalytic activity for iodine/triiodide reduction reaction. Compared with the conventional counter electrodes used in nanocrystalline dye-sensitized solar cells, the present electrode had provided a much higher catalytic performance which was attributed to the structure of platinum nanoclusters distributed homogeneously on the electrode.     

Preparation and catalytic performance of Fe-SBA-15 and FeO x /SBA-15 for toluene combustion

High-surface-area and well-ordered mesopor- ous Fe-incorporated SBA-15 （xFe-SBA-15） and SBA-15- supported FeOx （yFeOx/SBA-15） with the Fe surface den- sity between 0.09 to 1.11 Fe-atom/nm2 have been prepared using the one-step synthesis and incipient wetness impregnation methods, respectively. Physicochemical properties of these materials were characterized by means of numerous techniques, and their catalytic activities for the combustion of toluene were evaluated. It is found that the xFe-SBA-15 and yFeOx/SBA-15 samples possessed rod- or chain-like morphologies. The Fe species were of high dispersion when the Fe surface density was lower than 0.76 Fe-atom/nm2 in xFe-SBA-15 and 0.64 Fe-atom/nm2 in yFeOx/SBA-15. At a similar Fe surface density and space velocity, the xFe-SBA-15 catalysts showed better activity than the yFeOJSBA-15 catalysts, in which the xFe-SBA- 15 catalyst with Fe surface density 0.59 Fe-atom/nm2 performed the best. It is concluded that the good perfor- mance of the xFe-SBA-15 sample with Fe surface density 0.59 Fe-atom/nm2 was associated with its large surface area, high Fe species dispersion, and good low-temperature reducibility.     

MOF-derived Fe based catalysts for efficiently Advanced Oxidation Processes: From single atoms to diatomic and nanoparticles

Sub-nanometer catalysts have drawn great attention based on their superior catalytic activity and extensive application in advanced oxidation processes(AOPs). Nonetheless, the precise regulation of the coordination environment and exploration of the peroxymonosulfate(PMS) activation mechanism remain the focus of research.Herein, we report the preparation of Fe catalysts with diverse sizes, including single atoms(SAs), double atoms(DAs), and nanoparticles(NPs) via adjusting the precursor. Sub-nan...     

有序中孔铁催化剂的费-托合成催化性能研究

以KIT-6为模板用硬模板法合成了有序中孔铁催化剂,并引入Cu助剂,考察其费-托合成反应催化性能,采用原位小角X-射线衍射和N2物理吸附等对其表征,考察了Cu助剂和CO还原对其催化性能和结构的影响.结果表明：模板法合成的铁催化剂不同于传统沉淀铁催化剂,它具有特殊的有序中孔结构和较大的比表面积,较高的费-托合成反应活性和C5＋选择性.Cu助剂使有序中孔铁催化剂的还原性提高,故活性最高.CO还原后的催化剂为孔径均一的中孔结构,比表面积较大,但有序性降低,存在部分孔坍塌.     

天然水体主要本底成分对催化臭氧氧化草酸的影响

采用浸渍法制备了Fe2O3负载活性炭（Fe2O3/AC）催化剂,考察了Fe2O3/AC催化臭氧氧化草酸的活性以及天然水体主要本底成分对Fe2O3/AC催化臭氧氧化草酸的影响. 结果表明,臭氧氧化草酸过程中Fe2O3/AC显示了良好的催化活性,草酸的去除主要基于催化贡献. HCO3-、CO32-及腐殖酸对Fe2O3/AC催化臭氧氧化草酸体系均有抑制作用. HCO3-和CO32-加入使催化臭氧氧化体系pH升高,进而降低Fe2O3/AC催化臭氧氧化草酸的活性. 此外,HCO3-和CO32-也是羟基自由基抑制剂,HCO3-、CO32-对体系的抑制作用从侧面验证Fe2O3/AC催化臭氧氧化草酸遵循羟基自由基机理. 腐殖酸加入体系后,与草酸形成竞争吸附和竞争氧化,从而抑制草酸的降解.     

ZIF-derived Co–N–C ORR catalyst with high performance in proton exchange membrane fuel cells

Metal and nitrogen-doped carbon (M-N-C) materials have been considered as the most promising non-precious metal oxygen reduction (ORR) catalysts to replace expensive Pt catalysts. Due to high Fenton catalytic activity of Fe element and the resulting instability, Co-based N–C (Co–N–C) catalysts without Fenton catalytic activity should be a worthier ORR catalyst being explored. Although the high ORR activity of Co–N–C catalyst has been demonstrated in aqueous half-cell tests, their performance under PEMFC working condition is still far away from that of state-of-the-art Fe–N–C catalysts. In this study, a high-performance Co–N–C catalyst was synthesized by one-step pyrolyzing Co-doped ZIF-8 (zeolitic imidazolate framework-8) particles in-situ grown on the high-surface-area KJ600 carbon black with high electronic conductivity. The resulting Co–N–C catalyst exhibited high intrinsic ORR activity, fast mass transfer rate and high electronic conductivity, and thus yielded a remarkable peak power density of 0.92 W cm^-2 in H₂–O₂ PEMFC, which is comparable to state-of-the-art Fe–N–C catalyst. This strategy is helpful to synthesize highly active M-N-C ORR catalysts with improved mass transfer and electric conductivity.     

Sr_2Fe_(1-x)Mg_xMoO_6复合氧化物的甲烷催化燃烧性能研究

采用溶胶凝胶法制备了双钙钛矿结构Sr2Fe1-xMgxMoO6系列氧化物,通过XRD、BET、XPS、TG等手段对催化材料进行了物性表征;以甲烷纯氧燃烧为目标反应,研究了Mg离子对Fe离子进行掺杂替代对催化材料性能的影响.结果表明:Sr2Fe1-xMgxMoO6主要有两个阶段的失重过程,分别与吸附态氧和晶格氧的失去有关;Mg2+掺杂导致B位有序度的提高,对催化活性不利.     

纳米固体超强酸SO42-/Fe2O3催化合成柠檬酸三丁酯

合成了纳米固体超强酸，考察了该催化剂在柠檬酸三丁酯合成中的催化活性，并与非纳米的SO4^2-/TiO2,SO4^2-/ZrO2,SO4^2-/Fe2O3，浓H2SO4催化剂进行了比较，同时对酯化反应的几种影响因素进行了研究。     

纳米固体超强酸SO_4~(2-)/Fe_2O_3催化合成乙酸异戊酯

合成了纳米固体超强酸 ,考察了该催化剂在乙酸异戊酯合成的催化活性 ,并与非纳米的SO2 - 4/TiO2 ,SO2 - 4/ZrO2 ,SO2 - 4/Fe2 O3,浓H2 SO4 催化剂进行了比较 ,同时对酯化反应的影响因素诸如催化剂的制备、用量及反应时间进行了研究。     

甲缩醛氧化制浓甲醛：Ⅱ.催化剂制备工艺条件的研究

考察了制备 方法、焙烧温度和成型助剂对甲缩醛氧化制甲醛铁相钴三元催化剂活性的影响。采用比表面、孔结构、ＸＲＤ和ＸＰＳ等测试技术研究了催化剂的宏观结构、晶相组成，表面、钼离子价态和浓度。     

担载Ni催化剂中Ni担载量及金属助剂对CH4与CO2重整反应活性的影响

考察了金属Ni担载量对Ni/Al2 O3、Ni/MgO/Al2 O3催化剂用于甲烷与二氧化碳重整反应活性的影响 ,结果表明 :Ni担载量对反应活性的影响受反应温度的制约 .在低担载量时 ,催化活性随Ni担载量的增加而增加 ,到 3%时CH4及CO2 转化率分别达到 10 0 %和88% ;但对高担载量催化剂如 2 0 %Ni/MgO/Al2 O3,高温时 (>10 73K)因Ni的聚集等使反应器堵塞 ,导致活性骤降 .与Ni/Al2 O3相比 ,Ni/MgO/Al2 O3具有更好的稳定性 .助剂对催化活性及稳定性也有一定影响 .各助剂对CH4转化的影响次序为 :La >Mn >Co >Fe .助剂的加入有助于Ni催化剂稳定性的提高 .     

铁离子掺杂TiO2基自洁净玻璃的制备及性能

用溶胶—凝胶法制备了表面镀有Fe—TiO2光催化薄膜的自洁净玻璃，并利用DTA—TG，XRD，SEM等手段研究了Fe—TiO2光催化薄膜的结构与特征。利用紫外—可见光分光光度计测量了不同镀膜层数的玻璃的透光率。通过光催化降解有机磷农药敌敌畏的水溶液，研究了不同铁含量以及不同镀膜层数对自洁净玻璃光催化活性的影响。研究结果表明：光催化薄膜主要由粒径为几十纳米的Fe3O4和TiO2颗粒构成；铁离子掺杂可以提高自洁净玻璃的光催化活性，在同样镀膜层数(2层)的情况下，[Fe]/[TiO2](摩尔比)＝0．005时的光催化性能最好；当用同样浓度的铁离子掺杂时，镀膜层数为9的光催化活性最高。     

Fe/Cu催化还原去除饮用水消毒副产物三氯乙酸

以高致癌风险的饮用水卤化消毒副产物(halogenated disinfection by-products,HDBPs)三氯乙酸(TCAA)为去除目标物,研究了Fe/Cu催化还原去除TCAA的效果,包括Fe/Cu质量比、Fe/Cu混合物投加量、pH值、有机物浓度和摇床转速等因素对Fe/Cu催化还原去除TCAA的影响.结果表明,Fe/Cu能够有效脱除TCAA,m(Fe):m(Cu)为10:1时的TCAA去除效果最佳;Fe/Cu最佳投加量为30 g·L-1;Fe/Cu还原脱氯去除TCAA最佳pH值在4～8之间;有机物浓度对Fe/Cu还原脱氯存在负面影响;在摇床转速、反应时间、投加量、pH值和UV254分别为200 r·min-1,160 min,30 g·L-1,6.82和0.117 cm-1的条件下,Fe/Cu催化还原对TCAA的去除率达到97.39%,并且Cu未被消耗,外扩散Fe/Cu催化还原反应的影响可以忽略,Fe/Cu对TCAA的催化还原脱氯降解过程符合拟一级反应.