新型碳纳米材料的制备及其在催化中的应用
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摘要
本论文的主要目的是探索简单高效的制备新型碳纳米材料的方法,并研究所制备的碳材料的应用前景,尤其是结合我们实验室的特点,尝试碳材料作为催化剂载体在催化中的应用。主要结果如下:
1.利用水热法,以廉价的淀粉、葡萄糖、环糊精等生物质材料为前驱物,以原位生成的铁氧化物为模板,利用铁氧化物的自发溶解,一步得到空心的碳纳米棒状和球状材料。
2.以Ni和Fe粒子为催化剂,聚苯乙烯为碳前驱,微波法合成了高度石墨化的碳材料。得到了直径600、350、90和40 nm的一系列空心碳球以及直径小到8-13 nm的碳纳米管。当采用含氮的高分子材料(聚丙烯腈)为碳前驱体时,可以得到氮参杂的碳材料。尝试了在这种氮参杂的碳材料表面担载了Pd纳米粒子,展示了其在催化中的潜在应用价值。
3.微波法制备了空心碳球包裹贵金属粒子的担载型催化剂。得到了分别包裹Pt、Pd、Au、Ru、Rh粒子的空心碳球。并将空心碳球包裹的Pd催化剂用于马来酸酐液相加氢反应,得到100%的转化率和对琥珀酸酐100%的选择性。同一份催化剂连续进行四次反应循环后损失很小,催化活性未见降低。
The purpose of this dissertation was to find a facile way to the synthesis of carbon materials and demonstrate their application in catalysis.In summary,we obtained the following results:
1.Synthesized hollow carbon nanorods and nanospheres using an one pot hydrothermal process,with iron oxide as template and starch,glucose,cyclodextrin as precursors.
2.Produced highly graphitic carbon materials via a microwave induced solid-state process.Both hollow carbon nanospheres with a size of 600,350,90,40 nm and carbon nanotubes with a diameter of 8-13 nm were obtained.N doped carbon materials are also produced with PAN as precursor.Pd nanoparticles were supported on the N doped carbon materials.
3.Pt,Pd,Au,Ru,Rh nanoparticles were encapsulated in hollow carbon spheres. Pd in carbon catalyst was used in hydrogenation of maleic anhydride.100% conversion and 100%selectivity to succinic anhydride were demonstrated.
1.利用水热法,以廉价的淀粉、葡萄糖、环糊精等生物质材料为前驱物,以原位生成的铁氧化物为模板,利用铁氧化物的自发溶解,一步得到空心的碳纳米棒状和球状材料。
2.以Ni和Fe粒子为催化剂,聚苯乙烯为碳前驱,微波法合成了高度石墨化的碳材料。得到了直径600、350、90和40 nm的一系列空心碳球以及直径小到8-13 nm的碳纳米管。当采用含氮的高分子材料(聚丙烯腈)为碳前驱体时,可以得到氮参杂的碳材料。尝试了在这种氮参杂的碳材料表面担载了Pd纳米粒子,展示了其在催化中的潜在应用价值。
3.微波法制备了空心碳球包裹贵金属粒子的担载型催化剂。得到了分别包裹Pt、Pd、Au、Ru、Rh粒子的空心碳球。并将空心碳球包裹的Pd催化剂用于马来酸酐液相加氢反应,得到100%的转化率和对琥珀酸酐100%的选择性。同一份催化剂连续进行四次反应循环后损失很小,催化活性未见降低。
The purpose of this dissertation was to find a facile way to the synthesis of carbon materials and demonstrate their application in catalysis.In summary,we obtained the following results:
1.Synthesized hollow carbon nanorods and nanospheres using an one pot hydrothermal process,with iron oxide as template and starch,glucose,cyclodextrin as precursors.
2.Produced highly graphitic carbon materials via a microwave induced solid-state process.Both hollow carbon nanospheres with a size of 600,350,90,40 nm and carbon nanotubes with a diameter of 8-13 nm were obtained.N doped carbon materials are also produced with PAN as precursor.Pd nanoparticles were supported on the N doped carbon materials.
3.Pt,Pd,Au,Ru,Rh nanoparticles were encapsulated in hollow carbon spheres. Pd in carbon catalyst was used in hydrogenation of maleic anhydride.100% conversion and 100%selectivity to succinic anhydride were demonstrated.
引文
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