段胜聪,李雪,李悦,陈春霞.淀粉模板法制备复合金属氧化物及其催化α-蒎烯氧化性能的研究[J].分子催化,2015,(4):339-347 |
淀粉模板法制备复合金属氧化物及其催化α-蒎烯氧化性能的研究 |
Study on Preparation of Composite Metal Oxides by Using Starch as Biotemplate and Their Catalytic Properties of α-pinene Oxidation |
投稿时间:2015-07-09 修订日期:2015-08-25 |
DOI: |
中文关键词: 生物模板法 淀粉 复合氧化物 α-蒎烯 催化氧化 |
英文关键词:biotemplate method starch composite oxide α-pinene catalytic oxidation |
基金项目:中央高校基本科研业务费专项资金项目(2572014DB04);国家自然科学青年基金(31400294);黑龙江省博士后科研启动金资助项目(LBH-Q14005)资助. |
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中文摘要: |
以淀粉为生物模板,LDHs晶核溶液为前驱体,通过共沉淀法、陈化及煅烧过程,制备了一系列复合金属氧化物多孔材料. 采用X射线衍射(XRD)、扫描电子显微镜(SEM)、X射线能谱(EDX)、N2吸附-脱附(BET)和X射线光电子能谱(XPS)等手段对样品进行形貌、结构与化学组成的表征,并比较它们H2O2-α-蒎烯催化氧化性能. 结果表明,淀粉以“嵌入”式发挥模板作用制备出具有独特形貌、孔径分布在约2~5 nm的介孔及大孔尺寸的多金属复合氧化物多孔材料,其比表面积达760.90 m2/g,具有良好的结晶度;其中MgZnAlFe四元复合氧化物催化性能最佳,在α-蒎烯/H2O2摩尔比为1:1.2、催化剂用量为10.0 mg、溶剂(V(DMF):V(水)=4:1)2 mL、20℃下反应4 h时,α-蒎烯转化率可达53.83%,产物2, 3-环氧蒎烷、马鞭草烯醇、马鞭草烯酮的选择性分别为48.90%、29.85%、21.25%. |
英文摘要: |
A series of porous composite metal oxides were successfully prepared based on coprecipitation, ageing and calcination, using starch as biotemplate and LDHs as precursors. The morphologies, structures and chemical compositions of the as-prepared samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray energy dispersive spectroscopy (EDX), N2 adsorption-desorption analysis (BET) and X-ray photoelectron spectroscopy (XPS). The results indicate that the starch plays an embedded template during the formation of composite oxides, and the prepared MgZnAlFe quaternary composite oxide has a particular morphology, good crystallinity, abundant distributions of mesoporous (2-5 nm pore size) and macroporous, and BET surface area of 760.90 m2/g. The porous composite oxides were then applied to catalyze the oxidation of α-pinene with 30 wt% H2O2 as the oxidant. The results show that the conversion rate of α-pinene can reach 53.83%, and the selectivities of 2, 3-epoxypinane, verbenol, verbenone are 48.90%、29.85% and 21.25%, respectively, under the following reaction conditions:10.0 mg porous MgZnAlFe quaternary composite oxide as the catalyst, α-pinene/H2O2 molar ratio of 1:1.2 in 2 mL DMF/H2O (volume ratio was 4:1) at 20℃ for 4 h. |
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