新穎的多金屬氧酸鹽基有機—無機雜化層狀物的離子熱合成與表征
發(fā)布時間:2018-03-11 05:29
本文選題:多金屬氧酸鹽 切入點:離子熱合成 出處:《長春工業(yè)大學(xué)》2017年碩士論文 論文類型:學(xué)位論文
【摘要】:多金屬氧酸鹽(POM)基有機-無機材料在燃料電池,醫(yī)學(xué),光催化等廣闊領(lǐng)域中有巨大的應(yīng)用。這樣的雜化物材料為人們在單一相中進(jìn)行結(jié)合有機與無機組分進(jìn)而得到某些獨特性質(zhì)提供了良好的機會。混合材料的這些性質(zhì)取決于POM和有機組分的連接,由于POM具有很高的離散性和可迅速移動的離子結(jié)構(gòu),POM被認(rèn)為是質(zhì)子傳導(dǎo)的有吸引力的候選物質(zhì)之一。在基于POM的混合有機-無機材料中,導(dǎo)電性通常來自配體水和配位水作為質(zhì)子給體或載體,這些性能啟發(fā)了我們在在燃料電池中進(jìn)行應(yīng)用質(zhì)子導(dǎo)體,需要大量和高遷移率的質(zhì)子載體以實現(xiàn)高質(zhì)子傳導(dǎo)性。但是,這種材料的合成是合成化學(xué)中最具挑戰(zhàn)性的問題之一。由于許多材料在離子熱合成條件下制備較為簡單,離子熱現(xiàn)在被認(rèn)為是一種更有效和環(huán)境友好的合成方法。本文制備了兩種POM(通過單晶X-射線衍射儀測試指明了是目標(biāo)化合物),三種有機配體(通過紅外光譜,固體紫外光譜測試等證實是目標(biāo)化合物),在實驗中使用離子熱合成法進(jìn)行制備目標(biāo)晶體。離子熱的條件下構(gòu)筑了兩例多酸基有機無機雜化化合物(H4C3N_2(C6H4N)2N_2C3H4)2/∞[Mo11O34]·H2O(1)和(H6C5N(CH2)3NC5H6)1/∞[Mo4O13](2),它們是基于∞[Mo_nO_(3n+1)]~(2-)(n=11,4)基本結(jié)構(gòu)單元,并且分別與Bis-(4-imidazol-1-yl-phenyl)-diazene和1,3-Di-(4-pyridyl)-propane有機配體作為抗衡陽離子組成的。基于β-[Mo8O26]4-的構(gòu)筑了1例同多鉬酸鹽基金屬有機開放框架合物[AgL][Mo~VMo_3~(VI)O_(12)](L=BBTZ=1,4-bis((1H-1,2,4-triazol-1-yl)methyl)benzene,化合物3),有機配體和多金屬氧酸鹽(POM)通過離子熱合成法合成了內(nèi)部由Mo-N鍵直接相連的目標(biāo)化合物。制備的化合物通過單晶X-射線衍射儀進(jìn)行結(jié)構(gòu)表征,得到化合物的晶體結(jié)構(gòu)數(shù)據(jù),利用晶體結(jié)構(gòu)解析軟件對所得晶體數(shù)據(jù)進(jìn)行了結(jié)構(gòu)優(yōu)化處理,并通過專業(yè)晶體繪圖軟件diamond得到化合物晶體結(jié)構(gòu)示意圖;衔镞M(jìn)行了拉曼,紅外,XPS等一系列光譜表征以輔助確定化合物的晶體結(jié)構(gòu),最后對化合物的質(zhì)子導(dǎo)電、光催化、氣體吸附等性質(zhì)做了詳細(xì)的研究。
[Abstract]:Polyoxometalate POM-based organic-inorganic materials in fuel cells, medicine, Such hybrid materials provide a good opportunity for people to combine organic and inorganic components in a single phase and obtain some unique properties. Quality depends on the connection between POM and organic components, POM is considered to be one of the attractive candidate materials for proton conduction because of its high dispersion and rapidly moving ionic structure. In mixed organic-inorganic materials based on POM, Electrical conductivity usually comes from ligand water and coordination water as proton donors or carriers. These properties inspire us to apply proton conductors in fuel cells, requiring a large number of proton carriers with high mobility to achieve high proton conductivity. The synthesis of this material is one of the most challenging problems in synthetic chemistry. Ion heating is now considered to be a more efficient and environmentally friendly method of synthesis. Two kinds of POM (identified by single crystal X-ray diffractometer as target compounds, three organic ligands) have been prepared. Under the condition of ion-thermal synthesis, two polyacid-group organic-inorganic hybrid compounds, H4C3N2C3Nnt2N2C3H4H4 / 鈭,
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