基于CQDs的纳米碳材料的设计、合成及其催化性能的研究

发布时间：2018-05-16 02:18

本文选题：碳量子点 + 掺杂碳量子点　；参考：《苏州大学》2015年硕士论文

【摘要】：碳材料在多年的研究中主要是作为催化剂载体,其新的研究进展是直接作为催化剂广泛应用于包括现代工业、农业、医药等主要领域。寻找和设计一种能够直接作为高效催化剂的纳米碳材料是至关重要的。碳量子点(CQDs)以及修饰的CQDs,引领着零维纳米结构这一新的领域,具有较强的稳定性和生物适应性,同时具有很强且可调的荧光性由于其特殊的物理化学特性,得以在催化剂研究方面广泛的应用。本论文中,从研究CQDs出发,设计合成了系列掺杂CQDs以及在半碳化材料中原位生成CQDs,并探究了它们在氢键催化、氧还原反应以及碳氢化合物选择性氧化方面的应用,主要包括以下内容:(1)通过简单的电化学刻蚀法制备了三种不同尺寸的CQDs,包括大于10nm、5nm和1-4nm的CQDs,并用TEM、HRTEM、UV-Vis、FT-IR、Raman、PL等表征方法研究了催化剂的形貌及基本性质,进而探索了它对系列羟醛缩合反应的氢键催化性能,结果发现5nm的CQDs在可见光照射下对羟醛缩合反应具有良好的催化效果和稳定性。(2)通过简单的火焰法制备了一系列的单/双掺杂CQDs,包括B-CQDs、N-CQDs、P-CQDs、S-CQDs、BN-CQDs、PN-CQDs和SN-CQDs,并用TEM、EDX、XPS、AFM、UV-Vis、FT-IR、Raman、PL等表征方法研究了催化剂的形貌及基本性质,进而探索了它对氧还原反应的催化性能,结果发现BN-CQDs对氧还原反应具有良好的催化效果和稳定性。(3)利用纤维素和葡萄糖为原料,通过简单的方法制备了系列不同碳化程度(100-900°C)的三维介孔碳球C-3DMPCS和G-3DMPCS纳米碳材料,其中半碳化程度的C-3DMPCS-500和G-3DMPCS-600内部结构中原位的生成部分的CQDs。使用SEM、TEM、BET、Raman等表征方法研究了其形貌和性质,进而在无溶剂、以叔丁基过氧化氢为引发剂、空气中的氧气为氧化剂、可见光照射的条件下,探索了对顺式环辛烯的选择性氧化催化性能,发现半碳化的C-3DMPCS-500和G-3DMPCS-600表现出优异的催化效果。
[Abstract]:Carbon materials are mainly used as catalyst carriers in many years of research. The new research progress is that carbon materials are widely used as catalysts in modern industry, agriculture, medicine and other main fields. It is very important to find and design a nano-carbon material that can be directly used as a high-efficient catalyst. Carbon quantum dots (CQDs) and modified CQDslead a new field of zero-dimensional nanostructures with strong stability and bioadaptability, and strong and adjustable fluorescence due to their special physical and chemical properties. It can be widely used in catalyst research. In this thesis, a series of doped CQDs and in situ formation of CQDs in semicarbonized materials were designed and synthesized from the study of CQDs, and their applications in hydrogen bond catalysis, oxygen reduction reaction and selective oxidation of hydrocarbons were investigated. The main contents are as follows: (1) three kinds of CQDswith different sizes were prepared by simple electrochemical etching method, including CQDsof larger than 10nm and 1-4nm. The morphology and basic properties of the catalysts were studied by means of TEM / HRTEMU UV-VisFT-IRN RamanPL. Furthermore, the hydrogen-bond catalytic activity for a series of hydroxaldehyde condensation reactions was explored. The results show that the CQDs of 5nm has a good catalytic effect and stability for the condensation of hydroxyl aldehyde under visible light irradiation.) A series of single / double doped CQDswere prepared by simple flame method, including B-CQDsOP-CQDsCQDsBN-CQDsPN-CQDDs and SN-CQDs. the characterization methods were studied by means of TEM-EDXX XPSAFMU UV-Vis-FT-IR Ramanine PL. The morphology and basic properties of the catalyst were investigated. The results showed that BN-CQDs had a good catalytic effect and stability for oxygen reduction reaction. It was found that cellulose and glucose were used as raw materials. A series of three-dimensional mesoporous carbon spheres (C-3DMPCS and G-3DMPCS nanocrystalline carbon materials with different carbonation degrees of 100-900 掳C) were prepared by a simple method, in which C-3DMPCS-500 and G-3DMPCS-600 with semicarbonization degree in situ formed part of CQDs. The morphology and properties of the samples were studied by means of Ding Ji Tem BET-Raman method, and then, under the conditions of solvent-free, tert Ding Ji hydrogen peroxide as initiator, oxygen in air as oxidant and visible light irradiation, the morphology and properties were studied. The catalytic performance of selective oxidation of cis-cyclooctene was investigated. It was found that the semicarbonized C-3DMPCS-500 and G-3DMPCS-600 showed excellent catalytic effects.
【学位授予单位】：苏州大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TQ127.11;TB383.1

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