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

【摘要】：金屬—有機(jī)骨架材料(Metal-Organic Frameworks,MOFs)作為多孔材料領(lǐng)域的新型材料,在九十年代初期開始進(jìn)入大眾視野,它是一類含有特定官能團(tuán)的有機(jī)配體和無機(jī)金屬離子或金屬簇通過自組裝方式構(gòu)筑的具有特定結(jié)構(gòu)的多孔材料。正是由于其獨(dú)特的有機(jī)-無機(jī)雜化構(gòu)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(tuán)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(chǔ)存和分離、光學(xué)、電磁材料、化學(xué)傳感、催化和生物醫(yī)學(xué)領(lǐng)域得到廣泛應(yīng)用。近幾年,隨著MOFs在多孔材料領(lǐng)域的迅猛發(fā)展,大量具有特殊結(jié)構(gòu)的MOFs材料被合成出來,該材料的發(fā)展也逐漸從單純的設(shè)計(jì)合成具有獨(dú)特結(jié)構(gòu)的MOFs材料轉(zhuǎn)向以功能為導(dǎo)向的MOFs材料的合成,通過合理的設(shè)計(jì)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(jié)構(gòu)研究為MOFs的功能化研究提供了必要的基礎(chǔ),使MOFs的功能化研究迅速成為多孔材料領(lǐng)域的研究熱點(diǎn)。雖然MOFs材料在眾多領(lǐng)域已表現(xiàn)出優(yōu)異的性能,但是在一些領(lǐng)域依然存在著重要的問題需要研究探討。因此,設(shè)計(jì)合成具有特殊結(jié)構(gòu)和所需功能的MOFs材料在促進(jìn)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(jī)配體,在溶劑熱條件下設(shè)計(jì)合成了一例基于含氮、含氧有機(jī)配體構(gòu)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(jié)構(gòu),具有較大的碳納米管孔道,拓?fù)浣Y(jié)構(gòu)表現(xiàn)為3,8連接網(wǎng)絡(luò)結(jié)構(gòu),拓?fù)浞?hào)為(4~3)2(4~6.6~18.8~4)。正是由于該MOF材料擁有柱撐結(jié)構(gòu)、較大的孔道和較高的比表面積,其對(duì)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(dú)特的六核鈷簇結(jié)構(gòu)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(diǎn)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(duì)該MOF材料的光催化CO_2還原催化性能進(jìn)行了深入的研究探討,對(duì)其催化機(jī)理進(jìn)行了推測(cè),并通過理論計(jì)算對(duì)推測(cè)的催化機(jī)理進(jìn)行了驗(yàn)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(xué)位授予單位】：東北師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O641.4

【參考文獻(xiàn)】

相關(guān)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(hào)：1814789