本文關(guān)鍵詞： 單分子磁體 多齒螯合配體 3d-過(guò)渡金屬 3d-4f混金屬 磁性　出處：《武漢工程大學(xué)》2016年碩士論文　論文類(lèi)型：學(xué)位論文

【摘要】：配位化學(xué)是當(dāng)前無(wú)機(jī)化學(xué)的重要分支,它與有機(jī)化學(xué)、物理化學(xué)、生物化學(xué)、固體化學(xué)、材料化學(xué)和環(huán)境化學(xué)等相互滲透,已經(jīng)成為眾多學(xué)科的交叉點(diǎn)。單分子磁體(SMMs)屬于配位化學(xué)中重要研究領(lǐng)域,相比于傳統(tǒng)磁性材料,單分子磁體具有尺寸小、易加工、能耗低、傳輸效率高等特點(diǎn),并在磁性信息儲(chǔ)存和量子計(jì)算等方面存在潛在應(yīng)用。由于3d過(guò)渡金屬配合物在結(jié)構(gòu)與磁性方面的局限性,人們對(duì)單分子磁體配合物的研究逐漸轉(zhuǎn)向了3d-4f混金屬配合物的研究,這歸功于3d-4f混金屬配合物的能壘和阻塞溫度相比過(guò)渡金屬單分子磁體的確有明顯提高。這給人們對(duì)于單分子磁體的設(shè)計(jì)提供了新思路,也促進(jìn)了人們對(duì)新的合成方法的不斷探索。本論文介紹了單分子磁體的特點(diǎn),綜述了近年來(lái)過(guò)渡金屬(3d)和稀土金屬(4f)及3d-4f混金屬簇合物的研究進(jìn)展,并設(shè)計(jì)、合成了一系列結(jié)構(gòu)新穎的配合物。本文在設(shè)計(jì)合成3d-4f過(guò)渡-稀土金屬單分子磁體配合物的過(guò)程中,也合成出了一些3d過(guò)渡金屬配合物,其中一些還具有較好的單分子磁體性質(zhì),為進(jìn)一步合成過(guò)渡-稀土混合金屬配合物打下基礎(chǔ)。主要研究?jī)?nèi)容如下:第一章為緒論。簡(jiǎn)要介紹配位化學(xué)的研究背景、金屬配合物的性質(zhì)及功能、以及分子磁體簡(jiǎn)介,并著重闡述了單分子磁體的研究進(jìn)展,其中包括基本合成方法和最近人們對(duì)該領(lǐng)域的的探索成果,最后提出本論文的研究構(gòu)想。第二章盡管在反應(yīng)體系中加入4f稀土金屬鹽,但得到的6個(gè)配合物稀土離子都沒(méi)有進(jìn)去,形成6個(gè)3d過(guò)渡金屬配合物,并對(duì)這些配合物進(jìn)行單晶結(jié)構(gòu)、元素分析、紅外光譜表征并對(duì)部分化合物的磁性進(jìn)行了測(cè)試和詳細(xì)表征。這六個(gè)配合物分別為:一個(gè)[Mn_6Na_4]二聚體配合物、一個(gè)[Fe_6O_2Cl_4(hmp)_8]·Fe_2OCl_6(其中Hhmp=2-吡啶甲醇)配合物、一個(gè)[Fe_7]配合物、一個(gè)八面體[Fe_6]配合物、一個(gè)[Ni4]配合物及一個(gè)[Mn_7]配合物。通過(guò)磁性研究發(fā)現(xiàn)[Mn_7]配合物具有單分子磁體所具有的頻率依賴現(xiàn)象。第三章為了獲得過(guò)渡-稀土(3d-4f)混合金屬配合物,在含有2,2-二吡啶酮和2,6-吡啶二甲醇混合配體的溶液中加入3d過(guò)渡金屬Fe鹽和4f稀土金屬鹽,獲得了四個(gè)3d-4f混合金屬配合物[Fe_4Ln_2](Ln=Dy、Ho、Er、Gd,這四個(gè)化合物是目前第一個(gè)含有混合配體的3d-4f混金屬配合物),并對(duì)所得到的四個(gè)配合物分別進(jìn)行單晶結(jié)構(gòu)分析、元素分析、紅外光譜表征和磁性研究。由于四個(gè)化合物的結(jié)構(gòu)性質(zhì)相似,在本文中具體描述了其中一個(gè)化合物[Fe_4Ho_2]的結(jié)構(gòu),通過(guò)磁性研究發(fā)現(xiàn)[Fe_4Dy_2]配合物在2000 Oe外加場(chǎng)下交流磁化率虛部具有單分子磁體所擁有的頻率依賴現(xiàn)象,并出現(xiàn)峰值,通過(guò)阿倫尼烏斯公式擬合,有效能壘達(dá)到22.07 K。
[Abstract]:Coordination chemistry is an important branch of inorganic chemistry, which permeates with organic chemistry, physical chemistry, biochemistry, solid chemistry, material chemistry and environmental chemistry. Monolayer magnets (SMMs) are important research fields in coordination chemistry. Compared with traditional magnetic materials, monolayer magnets have small size, easy processing and low energy consumption. High transport efficiency and potential applications in magnetic information storage and quantum computation. Due to the structural and magnetic limitations of 3D transition metal complexes. The study of monolayer magnets has gradually turned to the study of 3d-4f mixed metal complexes. This is due to the fact that the energy barrier and blocking temperature of the 3d-4f mixed metal complexes are obviously higher than that of the transition metal monolayer magnets, which provides a new idea for the design of monolayer magnets. It also promotes the continuous exploration of new synthetic methods. In this paper, the characteristics of monolayer magnets are introduced. The research progress of transition metal (3d) and rare earth metal (4f) and 3d-4f mixed metal clusters in recent years are reviewed and their designs are also reviewed. A series of novel complexes have been synthesized. In the process of designing and synthesizing 3d-4f transition metal monolayer magnets, some 3D transition metal complexes have also been synthesized. Some of them also have good properties of monomolecular magnets. The main research contents are as follows: the first chapter is introduction. The background of coordination chemistry, the properties and functions of metal complexes are briefly introduced. A brief introduction of molecular magnets is given, and the research progress of monolayer magnets is emphasized, including the basic synthesis methods and the recent achievements in this field. In the second chapter, although 4f rare earth metal salts were added to the reaction system, the six complexes were not found in the reaction system, and 6 transition metal complexes were formed. These complexes were characterized by single crystal structure, elemental analysis, IR spectra and magnetic properties of some compounds. [Mn_6Na_4] dimer complex, a. [Fe_6O_2Cl_4(hmp)_8] 路Fe2OCl6 (Hhmp-2-pyridyl) complex, a. [Fe_7] complex, an octahedron. [Fe_6] complex, a. [Ni4] complex and a. [Mn_7] complexes. [Mn_7] complexes have the frequency dependence of monolayer magnets. In chapter 3, in order to obtain transition rare earth 3d-4f metal complexes, the complexes contain 2O2-dipyridinone and 2. Four 3d-4f mixed metal complexes were obtained by adding 3D transition metal Fe salt and 4f rare earth metal salt into the solution of 6-pyridine dimethanol mixed ligand. [The four compounds are the first 3d-4f mixed metal complexes containing mixed ligands. The four complexes were characterized by single crystal structure analysis, elemental analysis, infrared spectroscopy and magnetic analysis. Because the four compounds have similar structure and properties, one of them is described in this paper. [The structure of Fe_4Ho_2 was found by magnetic study. [The Fe_4Dy_2] complex exhibits the frequency dependent phenomenon of monolayer magnets in the imaginary part of AC magnetic susceptibility under the external field of 2000Oe and the peak value is obtained, which is fitted by the Arrhenius formula. The effective base reached 22.07 K.
【學(xué)位授予單位】：武漢工程大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2016
【分類(lèi)號(hào)】：O641.4

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本文編號(hào)：1455051