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N-摻雜—維多孔碳自組裝及電催化氧還原反應(yīng)

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  本文選題:碳化 切入點(diǎn):量子點(diǎn) 出處:《大連理工大學(xué)》2016年碩士論文


【摘要】:氧還原反應(yīng)(ORR)是大多數(shù)燃料電池及金屬-空氣電池的陰極反應(yīng),也是許多金屬在腐蝕過程中的共軛反應(yīng)。目前該反應(yīng)催化性能最好的是鉑基催化劑,但是由于其資源短缺和耐持久性差等缺陷嚴(yán)重制約其應(yīng)用。因此,開發(fā)非金屬類催化劑就顯得尤為重要,摻雜型碳催化劑由于其獨(dú)特的電子特性、多孔結(jié)構(gòu)、豐富的碳源(如:有機(jī)化合物、金屬有機(jī)框架(MOFs)材料、共價有機(jī)材料(COM))等特點(diǎn)而成為人們研究的熱點(diǎn)。本課題利用模板法,設(shè)計并合成納米纖維結(jié)構(gòu),并以此作為非金屬催化劑的來源研究其在電催化氧還原反應(yīng)中的應(yīng)用。首先,以自組裝的CdTe納米線為犧牲模板,利用聚乙烯毗咯烷酮(PVP)與MOFs材料的相互作用誘導(dǎo)沸石咪唑類骨架結(jié)構(gòu)ZIF-8(二價鋅離子為配位中心,2-甲基咪唑為配體形成的六元環(huán)狀結(jié)構(gòu))前驅(qū)物在其表面成核及生成從而形成CdTe@ZIF-8納米纖維結(jié)構(gòu)。其次,通過高溫碳化CdTe@ZIF-8來制備氮(N)摻雜的一維中空/多孔碳結(jié)構(gòu)。通過在0.1 M KOH電解液中對比直接從ZIF-8晶體中制備的N摻雜多孔碳與上述制備的一維中空/多孔碳結(jié)構(gòu)的催化活性時,N摻雜的一維中空/多孔碳結(jié)構(gòu)表現(xiàn)出更好的電催化活性,更高擴(kuò)散極限電流密度和更正的半波電位。而導(dǎo)致其性能優(yōu)越的原因是以CdTe@ZIF-8作為碳源時,由于其獨(dú)特的電子結(jié)構(gòu)使其在碳化過程中石墨化程度提高,并且在碳化過程中CdTe納米線的揮發(fā)而留下的中空和多級多孔結(jié)構(gòu)有利于其物質(zhì)的傳輸。
[Abstract]:Oxygen reduction reaction (ORR) is the cathodic reaction of most fuel cells and metal-air cells, and is also the conjugation reaction of many metals in the process of corrosion.At present, the best catalyst is platinum-based catalyst, but its application is restricted seriously due to its shortage of resources and poor durability.Therefore, the development of non-metallic catalysts is particularly important. Due to their unique electronic properties, porous structure, rich carbon sources (such as organic compounds, organometallic frameworks and MOFss), doped carbon catalysts are very important.The characteristics of covalent organic materials have become the focus of research.In this paper, the structure of nanofibers was designed and synthesized by template method, and used as a non-metallic catalyst to study its application in electrocatalytic oxygen reduction reaction.First, using self-assembled CdTe nanowires as a sacrificial template,Nucleation and generation of zeolites imidazole framework structure ZIF-8 (hexagonal ring structure formed by divalent zinc ion as coordination center, 2-methylimidazole) on the surface of zeolite imidazole by the interaction of polyvinylpyrrolidone (PVP) with MOFs materialsThus, the structure of CdTe@ZIF-8 nanofibers was formed.Secondly, N-N doped one-dimensional hollow / porous carbon structure was prepared by carbonization of CdTe@ZIF-8 at high temperature.By comparing the catalytic activity of N-doped porous carbon prepared directly from ZIF-8 crystal with that of one-dimensional hollow / porous carbon structure prepared in 0.1m KOH electrolyte, the N-doped one-dimensional hollow / porous carbon structure showed better electrocatalytic activity.Higher diffusion limit current density and corrected half wave potential.The reason for its superior performance is that when CdTe@ZIF-8 is used as carbon source, the graphitization degree of CdTe@ZIF-8 is improved during carbonization because of its unique electronic structure.The hollow and multilevel porous structures left by the volatilization of CdTe nanowires during carbonization are beneficial to the transport of materials.
【學(xué)位授予單位】:大連理工大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2016
【分類號】:O643.36

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