Linbo Li, Yijun Du, Yao Li, Linjun Shao, Chenze Qi, Shujing Zhou, Jinjing Li
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引用次数: 0
摘要
摘要 开发一种简便、准确的方法来评估支撑金属的催化活性,可极大地促进支撑金属催化剂的制备和应用。本文合成了五种具有希夫碱官能团的 MCM-41 材料,并将其用作铜阳离子的载体。傅立叶变换红外光谱(FT-IR)和 X 射线光电子能谱(XPS)表征了铜阳离子在载体上的化学结构和配位。通过分析热重分析(TGA)和元素分析(EA)的结果,计算了接枝密度。透射电子显微镜(TEM)和 X 射线衍射(XRD)分析了这些支撑铜催化剂的微观结构。利用硫代苯甲醚氧化成甲基苯基亚砜的过程测定了这些支撑铜催化剂的催化活性,同时利用正电子湮灭寿命光谱评估了它们的邻苯基湮灭特性。研究发现,邻苯基湮灭特性与其催化活性呈线性相关。因此,通过 o-Ps 原子湮灭可以很容易地确定被不同官能团包围的支撑铜催化剂的催化活性。
Evaluation of the Catalytic Activities of Supported Copper Catalysts Surrounded with Different Functional Groups by o-Ps Annihilation
Developing a facile and accurate method for assessing catalytic activities of supported metals can significantly promote the preparation and application of supported metal catalysts. Herein, we synthesized five MCM-41 materials functionalized with Schiff-base groups, which were employed as the supports for copper cations. The chemical structures and coordination of copper cations on the supports were characterized by Fourier-transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). The grafting densities were calculated by analyzing the results of thermal gravimetric analysis (TGA) and elemental analysis (EA). The microstructures of these supported copper catalysts were analyzed by transmission electron microscopy (TEM) and X-ray diffraction (XRD). The oxidation of thioanisole to methylphenyl sulfoxide was employed to determine the catalytic activities of these supported copper catalysts while their o-Ps annihilation properties were evaluated by the positron annihilation lifetime spectroscopy. It is found that the o-Ps annihilation properties were linearly correlated with their catalytic activities. Therefore, the catalytic activities of supported copper species surrounded by different functional groups can be easily determined through o-Ps annihilation.
期刊介绍:
Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.