水滑石负载钯纳米晶的制备及其在Suzuki偶联反应中催化机理的研究
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摘要
本论文采用离子交换-水热还原方法制备了水滑石负载不同形貌钯纳米晶催化剂,并对其在Suzuki偶联反应中的催化性能及机理进行了研究。
钯作为贵金属催化剂,广泛应用于各种有机偶联反应,尤其对偶联反应具有较好的催化效率及选择性。水滑石(LDHs)是一种以天然矿物形式存在的典型的多功能阴离子层状粘土材料,而且水滑石表面积大,价廉。论文以镁铝硝酸根水滑石(MgAl-NO3LDH)为前体,采用离子交换法制备PdCl42-插层的LDH,进而通过调节还原反应的条件(时间、温度及比例),水热还原制备了水滑石负载的不同形貌的钯纳米晶催化剂。采用了XRD, FT-IR.元素分析表征了其物相与化学组成；采用TEM、HRTEM对其结构和形貌进行了详细研究。制得水滑石负载的立方体和棒状钯纳米晶催化剂,其中立方体状的钯纳米晶暴露的是(100)晶面,而对于棒状的钯纳米晶暴露的晶面主要是侧面的(100)晶面和顶端的(111)晶面。
TEM观察表明,水滑石对于钯纳米晶具有良好的分散作用,是分散作用良好的载体,且水滑石具有一定碱性,为催化反应提供了碱性环境。初步研究了制备的水滑石负载的不同形貌的钯纳米晶在不同条件下对Suzuki偶联反应的催化性能,经过实验发现,制得的催化剂具有比较高的催化活性,而且该催化反应是一个多相催化反应。并采用X射线光电子能谱(XPS)对Suzuki偶联反应在钯纳米晶表面的的多相催化机理进行了初步探讨,并提出了可能的多相催化机理。
In this paper, hydrotalcite supported with different morphology of nanocrystalline palladium catalysts were prepared and their catalytic properties and mechanism for suzuki cross-coupling reaction were studied.
Palladium, a precious metal catalyst, has been widely used as a variety of catalytic organic coupling reactions with good efficiency and selectivity. Layered double hydroxides (LDHs), a family of multifunctional lamellar clays, are existed as a form of natural minerals, moreover, the hydrotalcite surface area is big and moderately-priced. With Mg2Al-NO3LDH as a precursor, PdCl42--LDH has successfully synthesized by ion exchange method. On this basis, hydrotalcite supported nanocrystalline palladium catalyst was prepared by reduction reaction, with modulated matter ratio, reaction time and temperature. The supramolecular structure and chemical composition of the resulting materials were confirmed by XRD, FT-IR and elemental analysis. TEM and HRTEM were employed to study the detailed morphology. These have been obtained for hydrotalcite supported nanocubes and nanorods palladium catalyst. Load obtained hydrotalcite nanocube and nanorod palladium catalyst, in which the nanocube crystals of palladium is exposed (100) plane, while for nanorod crystal palladium is mainly exposed the crystal (100) face of side surface and (111) face of the top.
TEM shows that hydrotalcites can disperse well for those supported nanocrystalline palladium, and can be acted as a good carrier for dispersion. Moreover, hydrotalcite can provide a basic alkaline environment for the catalytic reaction due to the alkaline property of hydrotalcite. In this thesis, preliminary study of the catalysis for Suzuki cross-coupling reaction under different reaction state was investigated. Furthermore, heterogeneous catalytic mechanism was discussed for the Suzuki coupling reaction at the surface of nanocrystalline palladium, determined by X-ray photoelectron spectroscopy (XPS). In the experiment showed that the catalyst prepared with a relatively high catalytic activity, and the catalytic reaction is a heterogeneous catalysis. And X-ray photoelectron spectroscopy (XPS) on the Suzuki coupling reaction at the surface of nanocrystalline palladium heterogeneous catalytic mechanism was also discussed, and possible mechanism was also raised.
钯作为贵金属催化剂,广泛应用于各种有机偶联反应,尤其对偶联反应具有较好的催化效率及选择性。水滑石(LDHs)是一种以天然矿物形式存在的典型的多功能阴离子层状粘土材料,而且水滑石表面积大,价廉。论文以镁铝硝酸根水滑石(MgAl-NO3LDH)为前体,采用离子交换法制备PdCl42-插层的LDH,进而通过调节还原反应的条件(时间、温度及比例),水热还原制备了水滑石负载的不同形貌的钯纳米晶催化剂。采用了XRD, FT-IR.元素分析表征了其物相与化学组成；采用TEM、HRTEM对其结构和形貌进行了详细研究。制得水滑石负载的立方体和棒状钯纳米晶催化剂,其中立方体状的钯纳米晶暴露的是(100)晶面,而对于棒状的钯纳米晶暴露的晶面主要是侧面的(100)晶面和顶端的(111)晶面。
TEM观察表明,水滑石对于钯纳米晶具有良好的分散作用,是分散作用良好的载体,且水滑石具有一定碱性,为催化反应提供了碱性环境。初步研究了制备的水滑石负载的不同形貌的钯纳米晶在不同条件下对Suzuki偶联反应的催化性能,经过实验发现,制得的催化剂具有比较高的催化活性,而且该催化反应是一个多相催化反应。并采用X射线光电子能谱(XPS)对Suzuki偶联反应在钯纳米晶表面的的多相催化机理进行了初步探讨,并提出了可能的多相催化机理。
In this paper, hydrotalcite supported with different morphology of nanocrystalline palladium catalysts were prepared and their catalytic properties and mechanism for suzuki cross-coupling reaction were studied.
Palladium, a precious metal catalyst, has been widely used as a variety of catalytic organic coupling reactions with good efficiency and selectivity. Layered double hydroxides (LDHs), a family of multifunctional lamellar clays, are existed as a form of natural minerals, moreover, the hydrotalcite surface area is big and moderately-priced. With Mg2Al-NO3LDH as a precursor, PdCl42--LDH has successfully synthesized by ion exchange method. On this basis, hydrotalcite supported nanocrystalline palladium catalyst was prepared by reduction reaction, with modulated matter ratio, reaction time and temperature. The supramolecular structure and chemical composition of the resulting materials were confirmed by XRD, FT-IR and elemental analysis. TEM and HRTEM were employed to study the detailed morphology. These have been obtained for hydrotalcite supported nanocubes and nanorods palladium catalyst. Load obtained hydrotalcite nanocube and nanorod palladium catalyst, in which the nanocube crystals of palladium is exposed (100) plane, while for nanorod crystal palladium is mainly exposed the crystal (100) face of side surface and (111) face of the top.
TEM shows that hydrotalcites can disperse well for those supported nanocrystalline palladium, and can be acted as a good carrier for dispersion. Moreover, hydrotalcite can provide a basic alkaline environment for the catalytic reaction due to the alkaline property of hydrotalcite. In this thesis, preliminary study of the catalysis for Suzuki cross-coupling reaction under different reaction state was investigated. Furthermore, heterogeneous catalytic mechanism was discussed for the Suzuki coupling reaction at the surface of nanocrystalline palladium, determined by X-ray photoelectron spectroscopy (XPS). In the experiment showed that the catalyst prepared with a relatively high catalytic activity, and the catalytic reaction is a heterogeneous catalysis. And X-ray photoelectron spectroscopy (XPS) on the Suzuki coupling reaction at the surface of nanocrystalline palladium heterogeneous catalytic mechanism was also discussed, and possible mechanism was also raised.
引文
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