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    Please use this identifier to cite or link to this item: http://ir.lib.ncu.edu.tw/handle/987654321/6093


    Title: 金屬草酸-膦酸化合物與矽酸、鍺酸鈾化合物之合成、結構與性質研究;Synthesis and Characterization of Metal Oxalatophosphonates and Uranium Silicates and Germanates
    Authors: 林佳惠;Chia-Hui Lin
    Contributors: 化學研究所
    Keywords: 金屬草酸-膦酸化合物;矽酸、鍺酸鈾化合物;Metal Oxalatophosphonates;Uranium Silicates and Germanates
    Date: 2009-01-09
    Issue Date: 2009-09-22 10:13:07 (UTC+8)
    Publisher: 國立中央大學圖書館
    Abstract: 在本論文中共利用3種長晶法合成13個新穎化合物:利用中溫水熱反應合成6個金屬草酸-膦酸化合物,以高溫、高壓水熱反應合成5個具有新穎結構的稀土矽酸、鍺酸鈾化合物,以助熔劑長晶法合成2個鋰矽酸、鍺酸鈾化合物。按照化合物含膦酸與矽酸、鍺酸鹽,將此論文的研究分成了兩個系列。 第一個系列主要介紹使用不同的金屬(鎵、鐵以及錳)藉由中溫水熱反應來合成具新穎結構的金屬草酸-膦酸鹽。這一系列化合物皆利用有機模板當作結構導引試劑,加入草酸當作金屬的配位基,得到了多樣變化的結構型態,我們將這一系列中的兩個重要結論摘錄如下:(a) 化合物A1是第一個有機胺模板金屬草酸-膦酸鹽。(b) 在雙膦酸鹽的系統中,只是使用不同的金屬來源,便可合成出結構截然不同的化合物A5與A6。化合物A5為二維層狀結構,化合物A6為一維鏈狀結構,這兩個化合物分別藉由不同的氫鍵作用力形成三維的孔洞結構。 第二個系列主要介紹使用不同的鹼金屬陽離子(鋰、鉀、銣以及銫)藉由高溫、高壓水熱反應與助熔劑長晶法來合成具新穎結構的鈾矽酸、鍺酸鹽。在這一系列中我們得到了五種結構型態,我們將這一系列中的一些結論摘錄如下:(a) 化合物B1與B2結構中含有以共用(UO2)+單元上的氧所形成的(UO2/2O2/2O2/1)3三重鏈。在一些五價的錒系化合物中,利用(AnO2)+單元上的氧相互連接的情形,只有在U5+化合物結構中才能發現。(b) 化合物B3與B4是第一個利用水熱法得到的混價鍺酸鈾(Ⅴ,Ⅵ),化合物結構中含有以共用角的連接方式形成的–U6+–O–U5+–O–U6+–一維鈾氧八面體鏈,是第一個將六價的鈾原子以角共用的方式連接起來的例子。(c) 化合物B5是第一個利用高溫、高壓水熱法合成具有12員環規則孔道的三維鈾鍺酸鹽結構,其結構熱穩定性相當的好,可以穩定至700 ℃,同時伴隨著吸附、脫附結晶水的特性。(d) 化合物B6與B7是六價鈾的鋰矽酸、鍺酸鹽,在鈾矽酸、鍺酸鹽的系統中並未看到以鋰當陽離子的化合物存在。 There are six metal oxalatophosphonates and seven uranium silicates and germanates introduced in this thesis. Two of them were obtained via flux-growth method and the others were synthesized under hydrothermal method. These compounds have divided into two series by their components. The first series (A1 to A6) represents metal oxalatophosphonates which has been synthesized under mild hydrothermal conditions. We highlight two conclusions of first serise as follows: (a) A1 is the first organically templated gallium oxalatophosphonate. (b) The A5 has a 2D layer structure and the A6 adopts a 1D chain structure. These two compounds contain different hydrogen bond to form 3D frameworks. The second series (B1 to B7) describes seven uranium silicates and germanates which have been synthesized under high-temperature, high-pressure hydrothermal conditions or flux-growth method. We extract some conclusions as below: (a) B1 and B2 contain three parallel strings of a-UF5 type, which are joined via common corners to form a uranate column with the composition (UO2/2O2/2O2/1)3. This uranate column only occur in U(Ⅴ) compound. (b) B3 and B4 are the first examples of mixed-valence uranium(V,VI) germinates and their structures consist of strings of UO6 polyhedra sharing common corners to give infinite –U6+–O–U5+–O–U6+– chains. (c) B5 is a highly thermal stable extra-large pore uranyl germanate which is stable to 700 °C in air and is able to absorb water reversibly. (d) B6 and B7 are lithium uranyl silicate and germanate.
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