發(fā)布時(shí)間：2018-04-07 17:47

  本文選題：燃煤產(chǎn)物　切入點(diǎn)：有機(jī)組分　出處：《中國(guó)礦業(yè)大學(xué)》2017年碩士論文

【摘要】：論文首先基于數(shù)理統(tǒng)計(jì)方法歸納總結(jié)了華北、華南部分地區(qū)石炭-二疊紀(jì)煤中REE在不同沉積環(huán)境下的分布特征,在此基礎(chǔ)上,以華南貴州無(wú)煙煤和華北徐州氣煤為研究對(duì)象,通過(guò)酸處理分離出煤有機(jī)組分,同時(shí)使用馬弗爐燃燒和電廠采樣獲取煤的無(wú)機(jī)燃燒產(chǎn)物,再通過(guò)磁選方法獲得燃燒產(chǎn)物中的磁性礦物;使用紅外光譜、X射線衍射、X射線熒光光譜、電感耦合等離子質(zhì)譜、環(huán)境磁學(xué)和電子探針等研究手段,分析煤有機(jī)組分和燃燒產(chǎn)物的化學(xué)組成、稀土元素含量及磁學(xué)參數(shù),以揭示不同沉積環(huán)境煤中稀土元素的地球化學(xué)特征,闡明煤在燃燒過(guò)程中稀土元素的遷移特征及磁學(xué)響應(yīng)。取得如下主要成果和創(chuàng)新性認(rèn)識(shí):(1)探明華北和華南地區(qū)石炭-二疊紀(jì)不同沉積環(huán)境煤中REE的分布規(guī)律同一地區(qū)不同沉積環(huán)境下的煤中REE分布特征整體相似,不同地區(qū)相同沉積環(huán)境下REE分布特征各具差異。接近陸相沉積環(huán)境,煤中REE總含量就越高;越接近海相沉積環(huán)境,煤中輕、重稀土元素分餾就越大,Eu元素的虧損程度會(huì)增強(qiáng),Ce的富集程度相對(duì)降低,直至虧損。煤中REE分布形態(tài)主要受控于陸源物質(zhì),巖漿活動(dòng)會(huì)造成煤中REE相對(duì)富集,輕、重稀土元素分餾程度變高。(2)揭示了煤及其有機(jī)組分中REE的地球化學(xué)差異性特征在成煤階段,煤中有機(jī)和無(wú)機(jī)組分均繼承了物源中REE賦存特征,但無(wú)機(jī)組分比有機(jī)組分更容易受水體環(huán)境的影響。煤樣經(jīng)過(guò)酸處理后,無(wú)機(jī)礦物被溶蝕而有機(jī)質(zhì)基團(tuán)基本未被破壞,且REE的有機(jī)復(fù)合物穩(wěn)定性較高,酸處理后有機(jī)組分中REE得以保留,其分布特征與有機(jī)基團(tuán)種類和相對(duì)含量有關(guān),表現(xiàn)為含碳基團(tuán)較含氫基團(tuán)越多,輕、重稀土元素分餾程度越明顯。煤中有機(jī)和無(wú)機(jī)組分的含量差異是煤樣經(jīng)過(guò)酸處理后REE分布差異的主要原因。(3)探索了原煤及其燃燒產(chǎn)物中REE遷移分配特征燃煤產(chǎn)物基本保留了原煤中REE的分布特征,均為左高右低的Eu元素負(fù)異常的寬緩“V”型曲線,其REE富集程度遠(yuǎn)高于原煤,燃煤產(chǎn)物的底灰中REE富集程度和輕、重稀土元素分餾程度均相對(duì)大于飛灰。原煤中REE向灰分中遷移富集情況各異:原煤中硅酸鹽礦物細(xì)顆粒比重越大,逸散率越高,燃煤產(chǎn)物底灰中輕、重稀土元素分餾程度則越低;原煤中硅酸鹽礦物含量及其細(xì)顆粒比重越大,燃煤產(chǎn)物中無(wú)水石膏、方解石等礦物含量相對(duì)就越高,隨著燃燒溫度升高(700℃→800℃),飛灰中細(xì)顆粒及細(xì)顆粒中Si、Fe、S和P等主量元素含量增加;底灰中無(wú)水石膏等礦物含量相對(duì)降低,硅鋁酸鹽礦物含量相對(duì)升高,REE相對(duì)富集。(4)揭示了燃煤產(chǎn)物中磁性礦物與REE的響應(yīng)關(guān)系燃煤產(chǎn)物中的磁性礦物并非以顆粒分散狀態(tài)出現(xiàn),而是與玻璃質(zhì)礦物相膠結(jié)。磁性礦物在燃燒溫度較低的底灰中形狀不規(guī)則,在高溫飛灰中則顯示為磁珠狀。受“鑭系收縮”效應(yīng)影響,燃煤產(chǎn)物中REE與其低頻磁化率χlf的相關(guān)系數(shù)隨REE的正三價(jià)離子半徑減小而增大。隨著燃燒溫度的升高(700℃→800℃),控溫燃煤產(chǎn)物中Fe元素的逸散率增加,由于Fe元素與REE呈正相關(guān)關(guān)系,其中與HREE的相關(guān)性系數(shù)較高,Fe元素的逸散造成了底灰的磁性礦物中HREE含量的相對(duì)虧損;三價(jià)REE可以置換磁性礦物中的二價(jià)Fe,在磁性礦物中REE含量與二價(jià)Fe含量變化相反,隨著溫度的升高(700℃→1500℃),三價(jià)Fe離子含量降低,二價(jià)Fe離子含量升高,磁性礦物中REE含量相對(duì)降低,其中HREE較原灰分尤其虧損。
[Abstract]:Firstly, based on the method of mathematical statistics summarized in North China, the distribution characteristics of Carboniferous Permian coal in some areas of Southern China - REE in different sedimentary environment, on the basis of this, to Southern China and North Xuzhou Guizhou anthracite coal as the research object, through the acid treatment of isolated coal organic components, at the same time using muffle furnace combustion and power plant sampling the inorganic coal combustion products, to obtain magnetic minerals in combustion products by magnetic separation method; using infrared spectroscopy, X ray diffraction, X ray fluorescence spectrometry, inductively coupled plasma mass spectrometry, environmental magnetism and electronic probe and other research methods, analysis of coal combustion products and organic chemical composition, REE contents and magnetic parameters. In order to reveal the geochemical characteristics of rare earth elements in different sedimentary environment in the coal, migration characteristics and magnetic elucidate coal in the combustion process of rare earth elements in response to the following. The main achievements and innovation of knowledge: (1) study of Carboniferous in Southern China and Northern China in different sedimentary environments of Permian distribution of different sedimentary environment of coal REE in the same area of the coal distribution characteristics of REE are similar, with the same REE distribution characteristics of sedimentary environment in different areas of difference. Close to the continental sedimentary environment in coal REE the total content is higher; more close to the marine sedimentary environment in coal, light, heavy REE fractionation is larger and the degree of loss of Eu element will be enhanced, the enrichment degree of Ce decreased, until the loss. REE in coal distribution is mainly controlled by the source material, magmatic activity will cause the relative enrichment of REE in coal, light and heavy REE fractionation degree becomes higher. (2) the coal and geochemical characteristics of fractions of REE in the coal forming stage, coal in organic and inorganic components were inherited the occurrence characteristics of REE source, but no unit than Set points are more easily affected by water environment. Coal samples after acid treatment, inorganic mineral dissolution and organic groups without destruction, high stability and organic compound REE, after acid treatment of organic components in REE are retained, the distribution and relative content of organic groups and types, performance carbon containing groups containing hydrogen groups is more light and heavy REE fractionation degree is obvious. The organic and inorganic components in coal is the main reason for differences in the content of coal samples after acid treatment REE distribution. (3) to explore the raw coal and its combustion products REE migration distribution characteristics of combustion products to retain the basic distribution characteristics REE in the raw coal, all Eu elements left high right low negative anomaly relief "V" curve, the REE concentration is much higher than that of raw coal, REE enrichment degree of bottom ash combustion products in light and heavy rare earth elements, the degree of fractionation are relatively large To fly ash in coal ash. The migration to REE enrichment in different situations: coal in silicate mineral fine particles of the larger proportion of dissipation rate is high, the product of coal bottom ash light, heavy REE fractionation degree is low; silicate mineral contents in raw coal and fine particles of the larger proportion of anhydrous gypsum coal products. Calcite content is relatively higher, with the increasing of combustion temperature (700 DEG to 800 DEG C), fly ash particles and fine particles of Si, Fe, S and P increased the contents of major elements; the bottom ash and anhydrous gypsum mineral content is relatively low, aluminosilicate mineral salt content increased relatively. The relative enrichment of REE. (4) revealed that magnetic minerals not response between the combustion products of magnetic minerals and REE in the residues in particle dispersion state, phase but with vitreous mineral cementation. The magnetic minerals in the bottom ash low combustion temperature in irregular shape in The high temperature in the fly ash is bead shape. Influenced by the "contraction" effect of lanthanide, Cr3 + ion radius correlation coefficient X LF REE and low frequency magnetic susceptibility in the residues with REE decreases. With the increase of combustion temperature (700 DEG to 800 DEG C), emission of Fe element increased temperature control coal products, because Fe elements are positively correlated with REE, HREE and the correlation coefficient is higher, Fe emission caused by the relative loss of elements of bottom ash in magnetic mineral content of HREE; REE two Fe price of trivalent replacement in magnetic minerals, in magnetic mineral content change of REE and two Fe were opposite price and with the increase of temperature (700 DEG to 1500 DEG C), reduce the content of trivalent Fe ion, Fe ion content increased two relative price, reduce the content of REE in magnetic minerals, which is especially HREE ash loss.

【學(xué)位授予單位】：中國(guó)礦業(yè)大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TQ534;P618.11

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