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首页> 外文期刊>RSC Advances >Zirconium-doped porous magadiite heterostructures upon 2D intragallery in situ hydrolysis-condensation-polymerization strategy for liquid-phase benzoylation
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Zirconium-doped porous magadiite heterostructures upon 2D intragallery in situ hydrolysis-condensation-polymerization strategy for liquid-phase benzoylation

机译：锆掺杂的多孔木酰胺异质结构在2D液相苯甲酰化的原位水解 - 缩聚 - 缩聚策略中的异质结构

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摘要

Novel zirconium-doped porous magadiite heterostructures (PMH-xZr, x = Zr/Si molar ratio) are fabricated by two-dimensional intragallery cosurfactant-directing in situ hydrolysis-condensation-polymerization method of TEOS and Zr-n-propoxide from synthetic Na-magadiite and characterized systematically by XRD, SEM/(HR) TEM, Si-29 MAS NMR, BET, UV-vis DRS, NH3-TPD, pyridine FT-IR, and XPS techniques. The results indicate that the obtained PMH-xZr materials possess high surface area and high thermal stability upon effective assembly of interlayer Zr-doped meso-structural silica and the layers of magadiite. The PMH-xZr samples with x < 0.2 show successful incorporation of Zr into the lattice of interlayer mesostructural silica framework leading to considerably generated Bronsted sites Zr-O(H)-Si and obviously increased Lewis sites Zr-O-Si along with well-kept layered supermicro-mesostructure, while PMH-0.2Zr shows delaminated layers. PMH-0.1Zr exhibits the highest liquid-phase benzoylation activity of anisole with benzoyl chloride (Conv. 99.5%) and yield for 4-methoxybenzophenone (4-MBP) (94.1%) due to the strongest synergy between the high concentration of surface Bronsted sites and supermicro-mesostructure. PMH-0.1Zr can be reused by no further chemical treatment for at least five runs with a slightly reduced 4-MBP yield. These PMH-xZr materials can serve as a promising solid acid catalyst and/or acidic support with high surface area and thermal stability in broad range of catalysis applications.
机译：新型锆掺杂多孔杂体异质结构（PMH-XZR，X = Zr / Si摩尔比）通过二维内脏含量表面接合 - 来自合成NA-的TEOS和ZR-N-丙醇的原位水解 - 冷凝聚合方法引导 - 通过XRD，SEM /（HR）TEM，Si-29MAS NMR，Bet，UV-Vis，NH3-TPD，吡啶FT-IR和XPS技术系统地系统地进行了系统地进行了系统地表征。结果表明，所获得的PMH-XZR材料在有效组装中间型Zr掺杂的中间结构二氧化硅和木马二矿层时具有高表面积和高热稳定性。具有X <0.2的PMH-XZR样品显示成功掺入Zr到中间层培Mesosturation硅框架的晶格中，导致显着产生的布朗斯特位点ZR-O（H）-SI，明显增加了Lewis位点Zr-O-Si以及良好的Zr-O-Si。保存分层的超级微生物结构，而PMH-0.2ZR显示分层层。 PMH-0.1ZR具有苯甲酰氯（Conv.9.5％）和4-甲氧基二苯甲酮（4-MBP）（94.1％）的最高液相苯甲酰化活性，因为高浓度的表面勃朗斯特之间的最强协同作用网站和超级微观结构。 PMH-0.1ZR不能再用，除了至少五次的进一步进行化学处理，略微降低4mbp产率。这些PMH-XZR材料可以用作具有高表面积和高度催化应用的高表面积和热稳定性的有前途的固体酸催化剂和/或酸性载体。

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  • 来源
    《RSC Advances》 |2015年第83期|共13页
  • 作者

    Ma Yuewen; Sun Huan; Sun Qi; Zhang Hui;

  • 作者单位

    Beijing Univ Chem Technol State Key Lab Chem Resource Engn Beijing 100029 Peoples R China;

    Beijing Univ Chem Technol State Key Lab Chem Resource Engn Beijing 100029 Peoples R China;

    Beijing Univ Chem Technol State Key Lab Chem Resource Engn Beijing 100029 Peoples R China;

    Beijing Univ Chem Technol State Key Lab Chem Resource Engn Beijing 100029 Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;
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