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用于甲醇催化转化 CO2 的氧化铈纳米晶体的形态控制。

Morphology control of ceria nanocrystals for catalytic conversion of CO2 with methanol.

机构信息

Key Laboratory for Green Chemical Technology, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, PR China.

出版信息

Nanoscale. 2013 Jun 21;5(12):5582-8. doi: 10.1039/c3nr00831b.

Abstract

This paper describes the synthesis of ceria catalysts with octahedron, nanorod, nanocube and spindle-like morphologies via a template-free hydrothermal method. The surface morphologies, crystal plane and physical-chemical structures were investigated via field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) and temperature-programmed desorption of ammonia and carbon dioxide (NH3-TPD and CO2-TPD). The catalytic performance over these ceria catalysts with different exposed planes were tested for dimethyl carbonate (DMC) synthesis from CO2 and methanol. The results showed that the spindle-like CeO2 showed the highest DMC yields, followed by nano-rods, nano-cubes and nano-octahedrons. A synergism among the exposed (111) plane, defect sites, and acid-basic sites was proposed to be crucial to obtaining the high reactivity of DMC formation.

摘要

本文通过无模板水热法合成了具有八面体、纳米棒、纳米立方体和纺锤形形态的氧化铈催化剂。通过场发射扫描电子显微镜(FE-SEM)、透射电子显微镜(TEM)、高分辨率透射电子显微镜(HRTEM)、X 射线衍射(XRD)和氨和二氧化碳程序升温脱附(NH3-TPD 和 CO2-TPD)研究了表面形态、晶面和物理化学结构。在不同暴露面上的这些氧化铈催化剂上测试了用于从 CO2 和甲醇合成碳酸二甲酯(DMC)的催化性能。结果表明,具有纺锤形的 CeO2 表现出最高的 DMC 产率,其次是纳米棒、纳米立方体和纳米八面体。提出暴露(111)面、缺陷位和酸碱位之间的协同作用对于获得高 DMC 形成反应性至关重要。

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