Preparation And Energy Catalytic Application Of Two-dimensional Graphdiyne Carbon Material

Graphdiyne is a new all-carbon nanostructured material composed of sp and sp~2hybrid carbon atoms,and is a two-dimensional network structure formed by butadiyne connecting benzene rings.This unique structure makes graphdiyne have highπconjugation,unique electron distribution and rich and uniformly distributed pores,so graphdiyne has excellent semiconductor properties and has broad application prospects in the fields of energy catalysis,rechargeable batteries,medicine,energy storage,wa ter purification and gas separation.The artificial chemical synthesis of graphdiyne has greatly promoted the research of graphdiyne,and researchers in different fields in the world have also shown high attention and great interest in it.Graphdiyne has been listed as the most potential important development material in developed countries such as Europe and the United States,and China has been leading the development of graphdiyne,and the research on graphdiyne has made certain breakthroughs in all aspects.However,at present,there is still a lack of breakthroughs in the preparation of graphdiyne materials with precise doping atoms,high crystallinity and tunable semiconductor properties,controllable macro preparation of graphdiyne materials,regulation of structure characterization and properties and their major foundations,and the controllable synthesis of single-layer graphdiyne films and a few layers of thin films and new characterization methods and technologies suitable for graphdiyne materials are the key problems to be solved in the research of graphdiyne materials.Based on the above research background,this paper is divided into the following parts:1.In recent years,halogen functionalization of carbon materials has received extensive attention,due to the different electronegativity and atomic size of halogen atoms,doping halogen atoms in carbon materials can more accurately adjust the molecular pore size and conductivity of carbon materials,which provides opportunities to optimize the conductivity,band gap and morphological characteristics of carbon materials.Therefore,1,3,5-triethynyl-2,4,6-trifluorobenzene,1,3,5-triethynyl-2,4,6-trichlorobenzene,1,3,5-triethynyl-2,4,6-tribromobenzene were used as precursors for the polymerization reaction,and graphdiyne doped with fluorine,chlorine and bromine was grown on copper sheets by Glaser-Hay coupling in pyridine solution.Test methods such as SEM,TEM,Raman and XPS are used to systematically characterize their structures and test their electrical properties.2.Since the successful synthesis of graphdiyne in 2010,more and more researchers have actively invested in the synthesis of graphdiyne.After more than ten years of development,a variety of synthesis methods have been proven to be feasible,but most of the known means of synthesizing graphdiyne have low yield and high cost,resulting in limited application fields.Therefore,the existing preparation methods of graphdiyne still need to be improved.Based on the above background,we use copper sulfate crystals instead of copper tablets in traditional methods as catalysts and templates for graphdiyne polymerization to obtain high-quality graphdiyne on a large scale.3.Adsorption separation is usually used to obtain good hydrocarbon separation performance through molecular screening.Pores,metal organic frameworks(MOFs)and covalent organic frameworks(COFs)have been confirmed to promote the efficient separation of aromatic and fat-oriented petrochemical products.Thanks to its unique monolayer structure and abundant and evenly distributed pores,graphdiyne also has great application potential in the field of gas separation.In summary,we have attempted to introduce acetylene bonds into trianglimine to obtain graphdiyne analogues and are ready to further explore their applications in compound separation.