本文選題：金屬—有機骨架材料 + 六核鈷簇�。� 參考：《東北師范大學》2017年碩士論文

【摘要】：金屬—有機骨架材料(Metal-Organic Frameworks,MOFs)作為多孔材料領域的新型材料,在九十年代初期開始進入大眾視野,它是一類含有特定官能團的有機配體和無機金屬離子或金屬簇通過自組裝方式構筑的具有特定結構的多孔材料。正是由于其獨特的有機-無機雜化構成模式,該材料的孔道形狀和孔徑尺寸可以被系統(tǒng)的調(diào)節(jié),官能團易于被修飾。MOFs更是憑借其超高的比表面積、較高的孔隙率和特殊功能化的孔道表面在氣體儲存和分離、光學、電磁材料、化學傳感、催化和生物醫(yī)學領域得到廣泛應用。近幾年,隨著MOFs在多孔材料領域的迅猛發(fā)展,大量具有特殊結構的MOFs材料被合成出來,該材料的發(fā)展也逐漸從單純的設計合成具有獨特結構的MOFs材料轉向以功能為導向的MOFs材料的合成,通過合理的設計和調(diào)控來獲得具有特定性能的功能性多孔材料。最初MOFs材料的結構研究為MOFs的功能化研究提供了必要的基礎,使MOFs的功能化研究迅速成為多孔材料領域的研究熱點。雖然MOFs材料在眾多領域已表現(xiàn)出優(yōu)異的性能,但是在一些領域依然存在著重要的問題需要研究探討。因此,設計合成具有特殊結構和所需功能的MOFs材料在促進新型功能性多孔材料發(fā)展方面具有重大意義。本文中,我們選用4,4-聯(lián)吡啶和三甲酸三苯胺有機配體,在溶劑熱條件下設計合成了一例基于含氮、含氧有機配體構筑的三維(3D)多孔六核鈷簇MOF材料[Co_3(NTB)(4,4'-bpy)_(1.5)(OH)_3]·DEF(Co_6-MOF)NTB=三甲酸三苯胺,4,4'-bpy=4,4'-聯(lián)吡啶Co_6-MOF具有傳統(tǒng)的三維柱撐結構,具有較大的碳納米管孔道,拓撲結構表現(xiàn)為3,8連接網(wǎng)絡結構,拓撲符號為(4~3)2(4~6.6~18.8~4)。正是由于該MOF材料擁有柱撐結構、較大的孔道和較高的比表面積,其對N_2和CO_2表現(xiàn)出很好的吸附作用。此外,該MOF材料表現(xiàn)出很好的耐酸、耐堿性能,并且在空氣中可以穩(wěn)定存在。由于該MOF材料中獨特的六核鈷簇結構的存在,使其表現(xiàn)出較好的反鐵磁性。該MOF材料顯著的特點在于六核鈷簇與配體間的特殊連接使其在光催化CO_2還原中表現(xiàn)出較好的催化性能。本文中,我們對該MOF材料的光催化CO_2還原催化性能進行了深入的研究探討,對其催化機理進行了推測,并通過理論計算對推測的催化機理進行了驗證。
[Abstract]:Metal-Organic frameworks (MOFs), a new type of porous material, has been in public view since the early 1990s. It is a kind of organic ligands with specific functional groups and inorganic metal ions or metal clusters, which are self-assembled porous materials with specific structures. It is precisely because of its unique organic-inorganic hybrid structure that the pore shape and pore size of the material can be systematically adjusted, and that the functional groups are easily modified. High porosity and special functional pore surfaces are widely used in the fields of gas storage and separation, optics, electromagnetic materials, chemical sensing, catalysis and biomedicine. In recent years, with the rapid development of MOFs in the field of porous materials, a large number of MOFs materials with special structure have been synthesized. The development of this material has gradually changed from simple design and synthesis of MOFs materials with unique structure to the synthesis of functionally oriented MOFs materials. Through reasonable design and regulation, functional porous materials with specific properties can be obtained. The study of the structure of MOFs materials at first provided the necessary foundation for the study of MOFs functionalization, which made the functionalization of MOFs become the research hotspot in the field of porous materials. Although MOFs materials have shown excellent performance in many fields, there are still some important problems to be studied in some fields. Therefore, the design and synthesis of MOFs materials with special structure and required functions is of great significance in promoting the development of new functional porous materials. In this paper, we have designed and synthesized an organic ligands of 4 ~ 4- bipyridine and trianiline under solvothermal conditions. The porous hexagonal cobalt cluster MOF material constructed by oxygen-containing organic ligands has a traditional three-dimensional pillared structure, larger carbon nanotube channels, and a topological structure of 38-connected network structure, and its topological structure is characterized by a 38-connected network structure, which is characterized by a DEF Co6-MOFN Co_6-MOF = a trianiline, a trianiline, a bpyridine-4444-bipyridyl, a conventional three-dimensional pillared structure, a large carbon nanotube pore, and a topological structure characterized by a 38-connected network structure. The topological symbol is 4 ~ (4) ~ 3 ~ 2 ~ (6) ~ (6) ~ (6) ~ (6) ~ (18. 8) ~ (4). It is precisely because the MOF material has a pillared structure, a large pore channel and a high specific surface area, it has a good adsorption on NSP _ 2 and CO_2. In addition, the MOF material exhibits good acid resistance, alkali resistance and stable presence in air. Due to the existence of the unique hexanuclear cobalt cluster structure in the MOF material, it exhibits good antiferromagnetism. The remarkable characteristic of this MOF material is that the special connection between hexanuclear cobalt clusters and ligands makes it exhibit good catalytic performance in photocatalytic CO_2 reduction. In this paper, the photocatalytic properties of the MOF material for CO_2 reduction were studied, and the catalytic mechanism was inferred and verified by theoretical calculation.
【學位授予單位】：東北師范大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：O641.4

【參考文獻】

相關期刊論文 前1條

1 Yin-Xia Sun;Wei-Yin Sun;;Influence of temperature on metal-organic frameworks[J];Chinese Chemical Letters;2014年06期

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本文編號：1814789