本文選題：地球化學實驗 + 鈾成礦模擬�。� 參考：《西北大學》2017年碩士論文

【摘要】：鈾在自然界成礦過程中伴隨有機能源礦產(chǎn)(如煤、石油、煤層氣等)共存的現(xiàn)象十分普遍。說明有機-無機礦產(chǎn)在形成過程中有著較為明顯的相互作用,有機質參與金屬礦物的吸附吸收、遷移沉淀、富集還原等一系列的地球化學過程,而鈾元素在化石能源演化形成的過程中也起到了催化活化的作用。有機質既作為路易斯堿與鈾元素配位,又作為電子給體充當還原劑。有機質中的腐殖酸吸附鈾酰離子,通過形成配合物阻滯鈾酰離子的遷移,形成鈾礦的初始地質沉積背景;天然氣和石油作為還原劑,將活潑且遷移能力強的六價鈾還原成難以遷移的四價鈾,最終形成鈾礦(藏)。為研究天然氣的還原成礦機理和有機質配位成鍵規(guī)律,我們通過模擬鈾元素地球化學的實驗來反映其與有機質作用的化學變化。從理論的角度出發(fā),為鈾與多種能源礦產(chǎn)共存提供化學解釋,從而揭示無機-有機礦產(chǎn)之間的相互聯(lián)系。本文將氮雜芳香多羧酸與鈾酰離子反應,通過對其晶體結構的解析,推測腐殖酸中含氧官能團與鈾酰離子的配位模式和化學結合能力。根據(jù)亮晶方解石捕獲的原生流體包裹體溫度推測成礦溫度,模擬地質條件下盆地較深部鈾源在天然氣存在下與鈾酰離子還原反應,研究天然氣攜鈾能力。1.將含有雜原子的芳香有機多羧酸與鈾酰離子作用,在水熱條件下合成配位聚合物,從而反映腐殖酸中含氧官能團在鈾成礦過程中的化學配位能力。總共培養(yǎng)得到7種鈾酰配合物的單晶,通過X-射線單晶衍射確定其化學結構,對其進行元素分析、光譜分析和熱重-差熱分析測試。2.在自行設計的高溫高壓反應釜中,將天然氣通入到低氧、含鈾的水溶液中進行地球化學實驗模擬,模擬鈾在地質條件下與天然氣的還原過程。將得到的固態(tài)產(chǎn)物進行分離,通過X-射線粉末衍射驗證,得到的反應產(chǎn)物的主要成分為UO3的水合物。3.有機質的存在有利于天然氣的溶解,將天然氣通入到低氧、含鈾的水-乙醇體系中進行模擬反應,將粗產(chǎn)物進行酸解處理后,對產(chǎn)物進行X-射線粉末衍射測試,得到處于混合價態(tài)的鈾氧化物(U308)。
[Abstract]:The coexistence of organic energy minerals (such as coal, petroleum, coalbed methane) is very common in the process of uranium mineralization in nature.The results show that there is obvious interaction between organic-inorganic minerals during their formation. Organic matter is involved in a series of geochemical processes, such as absorption, migration and precipitation of metal minerals, enrichment and reduction, etc.Uranium also plays a catalytic role in the evolution of fossil energy.Organic matter can coordinate with uranium as Lewis base and as electron donor as reducing agent.The humic acid in organic matter adsorbs uranyl ions and forms complexes to block the migration of uranyl ions to form the initial geological and sedimentary background of uranium deposits; natural gas and petroleum are used as reductants.The active and highly mobile hexavalent uranium is reduced to tetravalent uranium which is difficult to migrate, and the uranium deposit is formed.In order to study the mechanism of reduction and mineralization of natural gas and the law of coordination bond formation of organic matter, the chemical change of the interaction between uranium element and organic matter is reflected by simulating the geochemistry of uranium element.From the theoretical point of view, this paper provides a chemical explanation for the coexistence of uranium and many kinds of energy minerals, thus revealing the interrelation between inorganic and organic minerals.In this paper, the coordination mode and chemical binding ability of oxygen-containing functional groups with uranyl ions in humic acid were deduced by analyzing the crystal structure of aromatic polycarboxylic acids and uranyl ions.According to the temperature of primary fluid inclusions captured by bright calcite, the ore-forming temperature is predicted, and the uranium source in the deeper part of the basin reacts with uranyl ion in the presence of natural gas under simulated geological conditions, and the uranium carrying capacity of natural gas is studied.The coordination polymers were synthesized by the interaction of aromatic organic polycarboxylic acids containing hetero-atoms with uranyl ions under hydrothermal conditions, thus reflecting the chemical coordination ability of oxygen-containing functional groups in humic acids during uranium mineralization.A total of 7 uranyl complexes were grown and their chemical structures were determined by X-ray single crystal diffraction. The chemical structures were characterized by elemental analysis, spectroscopic analysis and thermogravimetric differential thermal analysis (TG-DTA).In the autoclave of high temperature and high pressure designed by ourselves, the natural gas was transported into the aqueous solution of low oxygen and uranium, and the geochemical experiment was carried out to simulate the reduction process of uranium with natural gas under geological conditions.The solid product was separated and verified by X-ray powder diffraction. The main component of the reaction product was hydrate of UO3.The existence of organic matter is beneficial to the dissolution of natural gas. The natural gas is transported into the water-ethanol system with low oxygen and uranium for the simulated reaction. After the crude product is treated by acid hydrolysis, the product is tested by X-ray powder diffraction.The mixed valence uranium oxide (U308) has been obtained.
【學位授予單位】：西北大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：P618.1;P619.14

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