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层状双羟基阴离子粘土的合成及其对NO_x的吸附性能研究

Synthesis and Adsorption Ability for NO_x of Anion Layered Double Hydroxides Materials

【作者】 郭志强

【导师】 葛忠华; 倪哲明;

【作者基本信息】 浙江工业大学 , 工业催化, 2004, 硕士

【摘要】 对于具有层状结构的材料和性能研究是近年来的研究热点。水滑石是一种典型的层状阴离子粘土,其结构和水镁石(Mg(OH)2)相似,水镁石中的Mg2+部分地被Al3+同晶取代而形成的衍生物称作水滑石。类水滑石化合物通式可表示为:[M1-xMx(OH)2]x+(An-)x/n·mH2O,由于M2+与M3+的比例在一定范围内可以调变,不仅可以维持其层状结构,而且可以调节它的酸碱性,甚至氧化还原性质。因此水滑石被众多的催化研究者所青睐。 本论文采用共沉淀法合成出了各类类水滑石样品,通过FT-IR,TG-DTA,XRD等表征手段,并在常温下对NOx的静态吸附进行了研究,以确定各类水滑石样品的制备条件,得到如下的研究结果。 合成了二元金属类水滑石化合物。经表征,样品具有典型的水滑石层状结构;作为前驱体对NOx均具有良好的吸附性能,其中锌铝型类(Zn/Al摩尔比为3)水滑石对NOx饱和吸附量最大,可达1851mg/g。 合成了铜钴铝等三元的不同摩尔投料比的碳酸根型水滑石,Cu/Co/Al摩尔之比分别为1:1:1~1:7:1,用XRD、IR、TG-DTA分析对它们进行了表征,测定了对氮氧化物的吸附性能。结果表明,Cu-Co-Al的摩尔之比在1:1:1~1:7:1时合成的化合物都具有水滑石结构,Co的含量增加,水滑石层间高度略有增加,热稳定性减弱热重-差热分析结果显示合成样品的分解均有两个过程。二元的Co3Al-HTlc吸附NOx优于三元的CuCoAl-HTlcs,三元的CuCo3Al-HTlc对NOx吸附性能优于其它三元的类水滑石化合物,二元的Co3Al-HTlc和三元的CuCo3Al-HTlc吸附容量分别为1781mg/g、1286mg/g。 采用离子交换法,将具有Keggin结构的磷钨酸、硅钨酸引入到Mg-Al、Mg-Al-Cu类水滑石(Hydrotalcite-like compounds,HTlcs)层间,成功制备了层有序度高,结晶度好的杂多酸阴离子柱撑类水滑石,得到了通道高度达1.15nm的大层间的催化材料,并用红外、XRD表征了材料的结构.测定了对NOx的吸附性能.

【Abstract】 The research on the structure and properties of laminated structure materials has become a hotspot recently. Hydrotalcite is a kind of negative ion clay with typical laminated structure. Its structure is similar with brucite Mg(0H)2, in which Mg2+ could be isomorphously replaced by Al3+ partly. The general formulas Hydrotalcite-like compounds are usually written as [MIIVxMIIIx(OH)2]x+ (An-)x/n mH2O. The ratio of M2+ and M3+ could be adjusted in wide range, which can not only maintain its laminated structure but also adjust its acidity and basicity, even oxidation-reduction nature. So hydrotalcites are widely used for numerous catalysis pursuers.This research work in this paper is mainly about that numerous hydrotalcite-like compounds were synthesized by co-precipitation. The samples were characterized by XRD, IR,TG-DTA; and the adsorption capacity of the samples after calcination at 500 ℃ for nitrogen oxides was measured. At last, optimal preparation condition is decided and some meaning conclusions are drawed.Diatomic metal hydrotalcite-like compounds were synthesized. The results show that the samples had typical layer hydrotalcite structure via characterization. The adsorption capacity of Zn3Al-HTlc for NOX was maximal, and the static saturation adsorption capacity was 1851mg/g.Carbonate pillared hydrotalcite-like compounds ( CuCoAl-HTlcs ) with different Cu/Co/Al molar ratios were synthesized by coprecipitation and characterized by XRD, IR, TG-DTA. The abilities of their adsorption on NOX were also measured. The results showed that the samples with Cu/Co/Al molar ratios of 1 : 1 : 1~1 : 7 : 1 have hydrotalcite structure and layer spacings increased with Co amount increase. The TG-DTA results showed that the materials decomposed in two stages and the thermal stability of the hydrotalcites decreased with increasing Co amount. The adsorption ability of the Co3Al-HTlc for NOX was much better than that of the CuCoAl-HTlcs,the adsorption ability of CuCO3Al-HTIC was better than the other the other CuCoAl-HTlcs. The adsorption capacities of the Co3Al-HTlc and CuCo3Al-HTlc were 1781mg/g and 1286mg/g respectively.The preparation of Mg-Al-hydrotalcite(WP-keggin, WSi-keggin) Mg-Al-Cu-hydrotalcite (WP-keggin, WSi-keggin) was studied. The POM-HTLs was synthesized using ion-exchange by introducing POM (heteropolyanions) into the layer of HTLcs. The POM-HTLcs was synthesized with high crystallization and high-order layers with the layered height of approximate 1.15nm successfully. The absorption ability of samples for NOx was also measured.

  • 【分类号】O647.3
  • 【被引频次】2
  • 【下载频次】216
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