镍含量对NiCoPrLa类水滑石及衍生复合氧化物的催化性能影响

用共沉淀法制备了镍含量不同的NiCoPrLa类水滑石,用FT-IR、SEM、TPD等对NiCoPrLa类水滑石及衍生复合氧化物的结构、表面形貌和催化性能进行表征。结果表明,随着Ni2+含量增大,3-6Ni/NCL-HT样品显示了较好的乙醇解离吸附性能。在Co3+含量不变的条件下,Ni2+含量增大,NiCoPrLa类水滑石衍生复合氧化物抗积碳能力逐渐下降。     

层状锌-铝类水滑石材料合成及应用进展

水滑石类化合物是一类具有双羟基层状结构的阴离子纳米材料,其中Zn-Al系水滑石由于其独特的结构和性能,在多相催化领域、吸附剂、生物医药以及高分子功能材料等方面具有广泛的应用前景。本文简要论述了近年来,Zn-Al系层状类水滑石的制备方法,介绍了水滑石及衍生的Zn-Al复合氧化物在多相催化领域、功能材料中的应用,并讨论了水滑石稳定性与组成的关系。     

镍含量对NiCoPrLa类水滑石结构及衍生复合氧化物的还原性能影响

用共沉淀法制备了镍含量不同的NiCoPrLa类水滑石,用XRD、TG和TPR对NiCoPrLa类水滑石及其衍生复合氧化物的结构、热稳定性和还原性能进行了表征。结果表明,Ni/Pr比增加,类水滑石的结晶度会随之增加,但其热稳定性随之下降;Ni2+含量增大,NiCoPrLa类水滑石样品的还原性较好,还原峰面积增大。     

水滑石类材料在氧化还原催化反应中的应用

综述了水滑石类材料在氧化还原催化反应中应用的最新研究进展,重点讨论了类水滑石及以类水滑石为前驱体衍生得到的复合氧化物在精细合成中的绿色催化应用。水滑石类材料必将在环境友好催化工业体系中扮演越来越重要的角色。     

类水滑石复合氧化物在烟道气脱SO2和NOx中的应用

简述了类水滑石复合氧化物的制备方法，并对类水滑石化合物为前驱体的复合氧化物作为环境友好催化材料在烟道气脱SO₂、NOx方面的研究进行了综述，指出应把研究重点放在类水滑石复合氧化物同时氧化吸附脱SO₂和NOx上     

锌铝复合氧化物吸附去除水中阴离子表面活性剂

用液相共沉淀法制备锌铝类水滑石颗粒.在500℃下焙烧类水滑石转化为锌铝复合氧化物,并用XRD、TG/DTA和FT-IR等对类水滑石和锌铝复合氧化物进行表征分析.用锌铝复合氧化物吸附水中的阴离子表面活性剂,对实验条件和主要影响因素进行研究,并对其吸附机理进行了探讨,实验结果表明,锌铝复合氧化物对阴离子表面活性剂去除效果明显.     

水滑石类材料碱性催化性能的应用研究

以绿色化学为基础,综述了类水滑石及其以类水滑石为前驱体衍生的复合氧化物作为一类优异的固体碱催化剂应用于醇醛缩合、克诺文诺盖尔(Knoevenagel)缩合、麦克尔(M ichael)加成以及酯交换等反应的最新研究进展。预测了水滑石类材料由于具有特殊的结构和性质必将在环境友好的催化工业体系中扮演越来越重要的角色。     

锌铝复合氧化物抗菌性能研究

以水和硫酸锌及水和硫酸铝为主要原料,通过共沉淀的方法制备了Zn∶ Al为3∶1的类水滑石(LDHs)型前驱体.采用XRD、SEM、TEM等对LDHs及其煅烧形成的复合氧化物的结构及形貌进行了研究,测试了复合氧化物对大肠杆菌ATCC 2385的抗菌性能,并考察了反应时间,焙烧温度、不同沉淀剂对该复合氧化物抗菌效果的影响.结果显示,反应时间为12h,焙烧温度为1000℃,沉淀剂为碳酸钠时得到的复合氧化物抗菌性能最为优异.     

水滑石类纳米材料的合成表征及性能研究

采用双滴共沉淀法合成Mg Al二元水滑石及其复合氧化物、Cu Mg Al三元水滑石及其复合氧化物,并对其进行化学分析。将铁作为潜在的磁性物种制备铁氧体,合成不同Mg/Fe(Ⅱ)摩尔比的磁性纳米Mg Al水滑石及其复合氧化物。通过原子力显微镜、红外光谱仪以及热重-差热分析仪对各类产物进行表征,并对磁性水滑石进行磁学性能的测试。结果表明,样品中Cu、Mg、Al的质量分数与化学式计算出的含量基本一致。原子力显微镜观测到各类样品的粒径均在20~60nm之间,且颗粒分布较均匀;IR分析和DTA分析表明:各类产物具有水滑石类化合物的结构特征。磁学性能测试表明,合成出的磁性水滑石具有一定的磁性。     

负载银的Ni-Al类水滑石复合氧化物的制备以及催化氧化性能

本文使用反应过程速率适中,无需控制pH值的尿素水解法,选用了硝酸盐、盐酸盐和硫酸盐在不同比例下制备了三组类水滑石复合氧化物,硝酸盐可在较大镍铝比例范围内制备催化剂,当x=4时催化剂及其前驱体的XRD图像都有明显的水滑石类化合物的特征衍射峰,且SEM照片中可观察到规整均匀的花状结构。将银作为活性组分,制备负载银型类水滑石复合氧化物催化剂,粒径有所减小,比表面积增大,对SO_2的吸附量大大提升。     

The impact of the “memory effect” on the catalytic activity of Mg/Al; Mg,Zn/Al; Mg/Al,Ga hydrotalcite-like compounds used as catalysts for cycloxene epoxidation

The epoxidation of cyclohexene by hydrogene peroxide and benzonitrile, in methanol as solvent on solid base catalysts, hydrotalcites (HT) and corresponding mixed oxides (C-HT) was investigated. The employed catalysts were as-synthesized Mg/Al; Mg,Zn/Al; Mg/Ga,Al hydrotalcites, their derived mixed oxides and the corresponding reconstructed hydrotalcite forms (R-HT) obtained via the “memory effect” upon a rehydration treatment of C-HT. The catalysts were characterized by XRD, CO₂-TPD and N₂ adsorption–desorption measurements.

The reconstructed HT samples exhibit higher activity in comparison to the as-synthesized carbonated HT samples. A tentative correlation of the catalytic properties with the base strength of the active sites, the structural and textural characteristics of the catalysts, has been explored.     

高稳定性的固体碱在催化合成丙二醇甲醚中的应用

利用表面嫁接法将过渡金属元素(Ti、V、Cr、Fe)嫁接到镁铝类水滑石的层板上,运用电感耦合等离子体原子发射光谱、X射线固体粉末衍射和透射电子显微镜等方法对其进行了表征,并以环氧丙烷和甲醇反应为探针反应测试了其碱催化性能。结果表明,嫁接后的镁铝水滑石仍具有良好的层状结构,Ti嫁接的镁铝水滑石比其它过渡金属元素嫁接的镁铝水滑石表现出了更优的催化性能。在适宜条件下,环氧丙烷的转化率为85.3%1,-甲氧基-2-丙醇的选择性可达81.8%。而且,该催化剂的催化性能不受空气中水和二氧化碳的影响,是一种高稳定的固体碱催化剂。     

Catalytic depolymerization of calcium lignosulfonate by NiMgFeO_x derived from sub-micron sized NiMgFe hydrotalcite prepared by introducing hydroxyl compounds

A new method for regulating the synthesis of Ni Mg Fe hydrotalcites(NMF LDHs) with the addition of hydroxyl compounds was proposed. A series of NMF LDHs were prepared by the above method, and then were calcined to obtain the Ni Mg Fe Ox(NMFOx) samples. The NMFOxsamples were characterized by XRD,SEM, TG-DTG, XPS and CO2-TPD, respectively. The catalytic performance of NMFOxfor depolymerizing calcium lignosulfonate(CLS) was evaluated by hydrothermal reaction. The results showed that the addition of hydroxyl compounds favored reducing the particle sizes of NMF LDHs. For the depolymerization of CSL, the yield of liquid product increased from 45% to 75.8% with the addition of NMFOx-ethanol(NMFOxET). The liquid products were mainly phenolics, aromatics, ketones and esters. The total selectivity of oxy-containing compounds was over 90.6%, among them, the phenolics were approximately 35.2%. The valence of Ni and Fe, crystalline phase and basicity almost remained unchanged. The NMFOx-ET samples were recycled for the depolymerization of CLS, moreover, the NMFOx-ET samples had high activity and stability after 4 cycles.     

镁铝复合氧化物催化合成丙二醇乙醚

以硝酸镁、硝酸铝和氨水为原料,通过共沉淀方法制备了一系列镁铝水滑石材料,经过焙烧处理后作为碱催化剂用于丙二醇乙醚的催化合成。采用X射线衍射、热分析、SEM、DTA-TG和CO^_2-TPD等手段对所制备的催化剂进行表征,结果表明,在实验范围所制备的催化剂均具有典型的镁铝水滑石结构。采用高压固定床反应器对催化剂进行活性评价,考察了形成沉淀的pH、晶化方式、原料中镁与铝物质的量比及焙烧温度等对镁铝水滑石及其衍生物的结构和催化活性的影响,研究了碱性与催化剂活性之间的关系,结果表明,镁与铝物质的量比为3和550 ℃焙烧的催化剂具有良好的催化合成丙二醇乙醚活性。超声晶化的方式可以提高镁铝水滑石衍生物的碱强度,但对镁与铝物质的量比不同的催化剂活性有着不同的影响。在（350～550） ℃,焙烧温度的提高可以增大催化剂的碱强度和碱量,催化活性也有显著提高,但进一步升高焙烧温度,催化剂的表面碱强度和碱量有所下降,催化活性也随之降低。     

微波加热技术在催化NOx脱除中的应用

综述了空气中氮氧化物的类型、危害及脱除方法。空气中氮氧化物主要为NO、N₂O和NO₂,化石燃料和植物体的燃烧以及土壤和动物排泄物中含氮化合物的转化是其主要来源,NOx是酸雨和雾霾天气形成的主要原因之一,严重影响人类健康。选择性催化还原技术通过氨等还原剂和催化剂的共同作用将NOx还原成N₂和H₂O,选择性非催化还原技术利用氨等还原剂在高温环境下的还原能力实现NOx的脱除。传统NOx脱除技术存在脱除效率不高和易产生二次污染的缺点。微波放电技术利用微波放电产生高能电子使NOx直接分解生成N₂,微波碳热还原技术利用微波辐照活性炭的热效应可以显著提高炭对NOx的脱除能力,对NO脱除率高于96%。以微波为基础的脱硝技术在工业催化脱硝领域中的应用研究表明,结合催化剂、微波作用等手段实现工业高效脱除氮氧化物是一种较为理想的实现方式,应用前景良好。     

Catalytic combustion of methane on novel catalysts derived from Cu-Mg/Al-hydrotalcites

Novel Cu-Mg/Al mixed oxides (designated as i-CMAO-800) were prepared by calcinations of Cu-Mg/Al hydrotalcites [(Cu²⁺ +Mg²⁺)/Al³⁺= 3] at 800 °C. Their performance for the catalytic combustion of methane was investigated. The oxides and their precursors were characterized by XRD, TG-DSC, TPR and N₂ adsorption/desorption techniques. The results showed that BET surface areas and the stability of the resultant oxides were greatly influenced by the copper contents in hydrotalcite precursors, bringing about difference in their activities for methane catalytic combustion. XRD results indicated that Cu was highly dispersed in hydrotalcite precursors in case of low copper contents, (Cu 40 wt%). For higher Cu contents, Cu(OH)₂ was formed, and, consequently, a separate phase of CuO was detected in the oxide catalysts after calcination. As indicated by the TG-DSC results, different decomposition behaviors were observed for various hydrotalcites. Thermal calcination promoted the formation of copper aluminates and segregation of CuO from the bulk phases. TPR results showed 15CMAO-800 has the highest reduction rate, and the catalytic activities of iCMAO-800 mixed oxides depend on both the reduction rates and the amounts of copper ions in mixed oxides. The catalyst 15-CMAO-800 showed the best performance.     

Mg/Al复合氧化物催化丙酮和碳酸二甲酯合成乙酰乙酸甲酯

利用先共沉淀后水热处理的方法制备出水滑石前体,将其焙烧后,得到具有不同Mg/Al摩尔比的复合氧化物,并借助电感耦合等离子原子发射光谱、XRD、CO2-TPD和氮气吸脱附等手段对其进行表征。结果表明,Mg/Al摩尔比对催化剂的结构和碱性质有较大的影响,并且在催化丙酮和碳酸二甲酯合成乙酰乙酸甲酯的反应中,其比单纯的氧化镁和氧化铝表现出了更高的催化活性。进一步的研究表明,在该反应中是复合氧化物的中强碱性位起催化活性的作用,当Mg/Al摩尔比为2时,催化剂具有最高的活性。此外,重复性实验表明,这些催化剂具有较好的稳定性和重复使用性。     

Calcined Zn/Al hydrotalcites as solid base catalysts for glycolysis of poly(ethylene terephthalate)

In this research, glycolysis of poly(ethylene terephthalate) (PET) with ethylene glycol (EG) was carried out using Zn/Al mixed oxide catalyst. These mixed oxides were prepared by calcining crystalline Zn/Al hydrotalcites at different calcination temperatures. The samples and corresponding precursors were characterized by X‐ray diffraction, BET, Fourier‐transform infrared spectra, thermogravimetry/differential thermal analysis, and Hammett titration method. The experimental results showed that Zn/Al mixed oxides obtained from hydrotalcites were found to be more active than their individual oxides for glycolysis of PET. The relationship between catalytic performance and chemical–physical features of catalysts was established. In addition, a study for optimizing the glycolysis reaction conditions, such as the weight ratio of EG to PET, catalyst amount and reaction time, was performed. The conversion of PET and yield of bis(2‐hydroxyethyl terephthalate) (BHET) reached about 92% and 79%, respectively, under the optimal experimental conditions. Moreover, it should be noted that Zn/Al mixed oxide not only provided an effective heterogeneous catalyst for glycolysis of poly(ethylene terephthalate), but also presented a novel method for decolorization of discarded colored polyester fabric. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 41053.     

Catalytic combustion of methane over mixed oxides derived from Co-Mg/Al ternary hydrotalcites

Co_xMg_3 − x /Al composite oxides (xCoMAO-800) were prepared by calcination of Co_xMg_3 − x/Al hydrotalcites (x = 0.0, 0.5, 1.0, 1.5, 2.0, 2.5, 3.0, respectively) at 800 °C. The materials were characterized using XRD, TG-DSC, N₂ adsorption-desorption and TPR. The methane catalytic combustion over the xCoMAO-800 was assessed in a fixed bed micro-reactor. The results revealed that cobalt can be homogenously dispersed into the matrices of the hydrotalcites and determines the structure, specific surface areas and porosity of the derived xCoMAO-800 oxide catalysts. The thermal stability and homogeneity of the hydrotalcites markedly depends on the cobalt concentration in the hydrotalcites. The Co-based hydrotalcite-derived oxides exhibit good activity in the catalytic combustion of methane. The catalytic activity over the xCoMAO-800 oxides enhances with increasing x up to 1.5, but subsequently decreases dramatically as cobalt loadings are further increased. The 1.5CoMAO-800 catalyst shows the best methane combustion activity, igniting methane at 450 °C and completing methane combustion around 600 °C. The catalytic combustion activity over the xCoMAO-800 oxides are closely related to the strong Co-Mg/Al interaction within the mixed oxides according to the TG-DSC, TPR and activity characteristics.     

Microwave Irradiation Effect on Hydrotalcite Synthesis

New synthesis method of hydrotalcites using microwave irradiation is presented, which avoids the autoclave high temperature treatment as well as the long crystallization time. The crystallite size of the obtained solids is smaller than in the conventionally prepared hydrotalcites. The highest irradiation time provided the lowest aluminium incorporation to the hydrotalcite network. Diminishing microwave irradiation time produces purer hydrotalcites. If the gel is irradiated only for two minutes a well crystallized hydrotalcite is obtained.