CdS柱撑钛铌酸介孔复合材料的制备与光解水制氢活性

以钛铌酸纳米片层为主体,CdS纳米颗粒为客体,通过剥离-重堆积法合成了不同投料比的CdSTiNbO₅介孔复合材料,材料的层间距为1.19nm,比表面积约为93m₂·g^-1.CdSTiNbO₅复合材料表现出良好的光解水制氢活性,当投料比n_CdS/n_HTiNbO5=1:2时,复合材料在模拟太阳光和可见光下的产氢速率分别为231和184μmol·h^-1·g^-1,是CdS的8.6和9.7倍.复合材料光催化活性的提高归因于比表面积的增加和光生载流子的有效分离.     

Incorporation of Pure Fullerene into Organoclays: Towards C60‐Pillared Clay Structures

In this work, we demonstrate the successful incorporation of pure fullerene from solution into two‐dimensional layered aluminosilicate minerals. Pure fullerenes are insoluble in water and neutral in terms of charge, hence they cannot be introduced into the clay galleries by ion exchange or intercalation from water solution. To overcome this bottleneck, we organically modified the clay with quaternary amines by using well‐established reactions in clay science in order to expand the interlayer space and render the galleries organophilic. During the reaction with the fullerene solution, the organic solvent could enter into the clay galleries, thus transferring along the fullerene molecules. Furthermore, we demonstrate that the surfactant molecules, can be selectively removed by either simple ion‐exchange reaction (e.g., interaction with Al(NO₃)₃ solution to replace the surfactant molecules with Al³⁺ ions) or thermal treatment (heating at 350 °C) to obtain novel fullerene‐pillared clay structures exhibiting enhanced surface area. The synthesized hybrid materials were characterized in detail by a combination of experimental techniques including powder X‐ray diffraction, transmission electron microscopy, X‐ray photoemission, and UV/Vis spectroscopy as well as thermal analysis and nitrogen adsorption–desorption measurements. The reported fullerene‐pillared clay structures constitute a new hybrid system with very promising potential for the use in areas such as gas storage and/or gas separation due to their high surface area.     

Supramolecular inclusion of a pillared double-layered host by an anion-directed second-sphere coordination

In this paper, we have illustrated the utilisation of a second-sphere coordination approach to construct supramolecular inclusion solids with varieties of guest molecules. A flexible molecule N,N,N′,N′-tetra-p-methylbenzyl-ethylenediamine (L1) bearing doubly protonated H-bond donors was designed, capable of forming N–H…Cl hydrogen bonds with a crystallographically unique chloride anion, to construct an anion-directed ligand. The pillared double-layered host framework was constructed by an anion-directed ligand and primary coordination sphere [CoCl₄]^2 ?  through weak C–H…Cl hydrogen-bonding interactions. A variety of guest molecules, such as p-anisaldehyde, 1,4-dimethoxy-2,5-bis(methoxymethyl)benzene, can be included, leading to the formation of novel supramolecular inclusion solids: [L1]·4[H]⁺·[CoCl₄]^2 ? ·2Cl^? ·1.5[C₈H₈O₂]·0.25[CH₃OH] (1) and [L1]·4[H]⁺·[CoCl₄]^2 ? ·2Cl^? ·1.5[C₁₂H₂₀O₄]·0.5[CH₃OH] (2).

We have presented herein the utilisation of a second-sphere coordination approach to construct supramolecular inclusion solids with a variety of guest molecules. A novel type of a pillared double-layered host framework was constructed by a second-sphere coordination between the anion-directed ligand (L1 = N,N,N′,N′-tetra-p-methylbenzyl-ethylenediamine) and [CoCl₄]^2 ?  through weak C–H…Cl hydrogen-bonding interaction, and a variety of guest molecules, such as p-anisaldehyde, 1,4-dimethoxy-2,5-bis(methoxymethyl)benzene, can be included, leading to the formation of supramolecular inclusion solids: [L1]·4[H]⁺·[CoCl₄]^2 ? ·2Cl^? ·1.5[C₈H₈O₂]·0.25[CH₃OH] (1) and [L1]·4[H]⁺·[CoCl₄]^2 ? ·2Cl^? ·1.5[C₁₂H₂₀O₄]·0.5[CH₃OH] (2)

     

羟基铬交联蒙脱土的制备及物化性能的研究

本文以钠型蒙脱土（Ｎａ－Ｍｔ）为原料，以羟基铬聚合阳离子为交联剂制备出羟基铬交联蒙脱土（Ｃｒ－Ｍｔ）并对其物化性能进行研究。结果表明Ｃｒ－Ｍｔ的物化性能优于Ｎａ－Ｍｔ，ｄ＿（００１）值１．６～１．９ｎｍ，比表面积８０～１９０ｍ￣２·ｇ￣（－１），１．８～５．０ｎｍ的孔约占半数以上，表面总酸量为６．１×１０￣（－４）～６．５×１０￣（－４）ｍｏｌ·ｇ￣（－１）、阳离子交换量在９．０×１０￣（－３）～４２×１０￣（－３）ｍｏｌ／１００ｇ样，但其热稳定性有待进一步提问。     

Liquid Sorption and Nanoparticle Intercalation in Layer-Structured Materials

Abstract

Alkylammonium intercalated graphite oxides (R-GO), palladium intercalated alumina-pillared montmorillonites (Pd/Al₂O₃-PILC) and titania-pillared montmorillonites (TiO₂-PILC) have been prepared and the intercalation materials have been characterized by BET surface area analysis, UV/VIS spectroscopy, ICP-AES, DTG-DTA, XRD and TEM measurements. R-GO particles were prepared by oxidation of natural graphite followed by organophilization with cationic surfactants. For TiO₂-PILC and Pd/Al₂O₃-PILC the synthesis included the interlamellar adsorption of precursor species (polyaluminium-hydroxide, Pd-acetate and tetraethyl orthotitanate) from dilute solutions and subsequent chemical reactions at the montmorillonite/solution interface.     

羟基铝离子柱撑蒙脱石材料的制备与结构表征

采用水洗过滤提纯蒙脱石原矿,以NaCl作为钠化改型剂对提纯后的蒙脱石原矿进行了钠化改型,以NaOH水解AlC13溶液制备了铝柱化剂,并采用离子交换法使铝柱化剂柱撑进入钠基蒙脱石层间得到羟基铝离子柱撑蒙脱石。采用XRF,XRD,SEM等方法对铝柱撑蒙脱石载体的结构进行了表征。柱撑前后样品的测试结果表明,羟基铝离子通过离子交换反应进入蒙脱石层间。     

氨水介质和氟处理对铝柱层柱粘土性质的影响

 分别在氨介质和钠介质中制备了层柱蒙脱土和层柱累托石,并用氟化铵、氟硅酸铵和氟铝酸铵对层柱粘土进行处理,考察了处理条件对层柱粘土结构和酸性的影响. NH3-TPD和IR分析结果表明,氨介质中制备的层柱粘土比钠介质中制备的具有更强的酸性,经氟处理后层柱粘土的酸性有较大的提高. 氨介质中制备的层柱粘土的低钠含量是其酸性改善的主要原因,而氟处理对层柱粘土酸性的提高主要来自氟对铝柱的表面作用. 氟处理层柱粘土对异丙苯裂解具有很高的催化活性.     

Pillared layered transition metal oxides

This paper reviews the reecent progress in the synthesis and application of pillared transition metal oxides during the last decade ,mainly concerning the synthetic methods,structures ,physical properties and catalytic appli-cations of the laycred transition metal oxides pillared by inorganic oxides,The factors and their affecting regularity in the process of preparation,and some important results obtained in the catalytic application studies are summarized.Finally,a prospect on the potential new directions in this research area is presented.     

杂多阴离子柱撑水滑石类层柱状化合物的合成与表征

以硝酸根型水滑石做交换前驱体，采用离子交换法合成了过渡金属离子三元取代硅钨杂多阴离子柱撑水滑石Ｍ＿２Ａｌ（ＯＨ）＿６－ＳｉＷ＿９Ｚ＿３（Ｈ＿２Ｏ）＿３Ｏ＿（３７）（Ｍ＝Ｍｇ￣（２＋），Ｚｎ￣（２＋），Ｎｉ￣（２＋），Ｚ＝Ｃｕ￣（２＋），Ｃｏ￣（２＋））．用元素分析、ＸＲＤ、ＩＲ、ＵＶ－ＤＲＳ和ＤＴＡ等手段对产物的组成和结构进行了表征。结果表明，杂多阴离子引入水滑石层间后，水滑石的层间距从０．９２ｎｍ增大到１．４７ｎｍ；提高了柱撑材料的热稳定性，随层的组成不同热稳定性顺序为：Ｍｇ＿２Ａｌ≥Ｎｉ＿２Ａ１＞Ｚｎ＿２Ａｌ；随柱的组成不同热稳定性顺序为：ＳｉＷ＿９Ｃｏ＿３＞ＳｉＷ＿９Ｃｕ＿３．处于层中的杂多阴离子在层的脱羟基温度以下均能保持良好的Ｋｅｇｇｉｎ结构。     

层状材料HMWO_6(M=Nb,Ta)的研究进展

近年来层状材料的发展已经引起人们的广泛关注,而HMWO6具备层状材料的所有共性。HMWO6不仅可用作酸催化剂,改性后还具有比较优越的光催化应用价值。主要从结构、性质、发展等方面综述了层状材料HMWO6的研究现状。