本文選題：模擬煤矸石自燃　切入點：多環(huán)芳烴　出處：《太原理工大學》2015年碩士論文　論文類型：學位論文

【摘要】：煤矸石是煤礦生產(chǎn)的副產(chǎn)品，大量的煤矸石經(jīng)過長時間的堆積發(fā)生自燃現(xiàn)象，產(chǎn)生有毒有害氣體多環(huán)芳烴。多環(huán)芳烴的生成與煤矸石內(nèi)部因素和外部自燃條件有密切的關(guān)系，為了研究不同變質(zhì)程度煤層夾矸中多環(huán)芳烴的含量，以及煤矸石在自燃過程中外部條件對多環(huán)芳烴生成的影響，本文以山西太原西山馬蘭礦、屯蘭礦、杜兒坪礦、西銘礦和山西晉城古書院礦的地下巷道煤矸石為研究對象，采用索氏提取和高效液相色譜（HPLC）等測試方法，討論不同變質(zhì)程度煤層夾矸中16種US EPA多環(huán)芳烴(PAHs)的含量特征；此外，在詳細分析自然環(huán)境中煤矸石山自燃環(huán)境的基礎(chǔ)上，于實驗室固定床管式爐上模擬煤矸石自燃，分析PAHs的生成途徑，探討不同溫度和通氣量對PAHs生成的影響，，結(jié)果表明： （1）變質(zhì)程度不同的煤層夾矸中含有的PAHs種類不同，但都含有萘和苯并[a]蒽，都不含有苯并[a]芘和茚并[1,2,3-cd]芘；隨著變質(zhì)程度的增強，PAHs的總含量和毒性都先增大，再減小，中高等變質(zhì)程度的煙煤夾矸中PAHs的含量最多，毒性最強，無煙煤的煤層夾矸中PAHs的含量最少，毒性最弱。西銘礦、屯蘭礦和杜兒坪礦煤矸石中的PAHs環(huán)數(shù)分布廣，且高環(huán)PAHs所占比例相對較多。 （2）煤矸石自燃產(chǎn)生的PAHs總量和種類都大于未自燃前煤矸石中含有的PAHs，且自燃過程中PAHs的分布符合分餾效應(yīng)，即模擬實驗分析得的PAHs主要以LPAHs為主，自燃殘余樣品中PAHs以4環(huán)PAHs為主，同時檢測到了5環(huán)和6環(huán)PAHs。煤矸石發(fā)生自燃后產(chǎn)生的PAHs毒性增強，且低溫環(huán)境下自燃生成的PAHs的毒性大于高溫環(huán)境。 （3）煤矸石自燃產(chǎn)生的PAHs以低環(huán)為主，在自燃過程中，較低溫度下（≤450℃）氧化產(chǎn)生的PAHs大于較高溫度（≥550℃）燃燒產(chǎn)生的PAHs，但高溫環(huán)境燃燒產(chǎn)生的PAHs種類多，HPAHs所占的比例相對較大。 （4）煤矸石在較低空氣流速下自燃，各溫度階段產(chǎn)生的PAHs變化相對比較平緩，在較高的空氣流速下自燃，低溫段的PAHs生成量遠遠大于高溫段PAHs生成量，且各溫度段的PAHs生成量變化相對比較劇烈。 （5）煤矸石發(fā)生自燃產(chǎn)生的萘（NaP）、菲（PhA）含量增多，低分子量多環(huán)芳烴占有絕對優(yōu)勢，且萘/菲基本都大于15，表明煤矸石自燃產(chǎn)生的PAHs來自于造巖源中大分子有機質(zhì)分子鍵的斷裂，但在高溫環(huán)境下高溫縮合或環(huán)化作用有所增強。
[Abstract]:Coal gangue is a by-product of coal mine production. After a long period of accumulation of coal gangue, a large number of coal gangue occur spontaneous combustion phenomenon, producing toxic and harmful gas polycyclic aromatic hydrocarbons. The generation of polycyclic aromatic hydrocarbons (PAHs) is closely related to the internal factors and external spontaneous combustion conditions of coal gangue. In order to study the content of polycyclic aromatic hydrocarbons (PAHs) in coal gangue with different metamorphic degrees and the influence of external conditions of coal gangue on the formation of PAHs in the process of spontaneous combustion of coal gangue, this paper deals with the formation of PAHs in Xishan Ma Lan Mine, Tunlan Mine and Duerping Mine in Taiyuan, Shanxi Province. Coal gangue in underground roadway of Ximing Mine and Guyuan Mine of Jincheng City, Shanxi Province was studied. The content characteristics of 16 kinds of US EPA polycyclic aromatic hydrocarbons (PAHs) in coal gangue with different metamorphism degree were discussed by Soxhlet extraction and HPLC (High performance liquid Chromatography). Based on the detailed analysis of the spontaneous combustion environment of coal gangue in the natural environment, this paper simulates the spontaneous combustion of coal gangue in a fixed bed tube furnace in laboratory, analyzes the way of PAHs formation, and discusses the influence of different temperature and ventilation on the formation of PAHs. The results show that:. (1) the coal bed gangue with different degree of metamorphism contains different kinds of PAHs, but all of them contain naphthalene and benzo [a] anthracene, neither of them contain benzo [a] pyrene or ninhydro [1o _ 2o _ 3-cd] pyrene. With the increase of metamorphism degree, the total content and toxicity of PAHs increase first, then decrease, The content of PAHs in gangue of bituminous coal of middle and higher metamorphism degree is the highest and the toxicity is the strongest, the content of PAHs in gangue of anthracite coal seam is the least and the toxicity is the weakest. The number of PAHs ring in coal gangue of Ximing, Tunlan and Duerping mines is widely distributed. And the proportion of high ring PAHs is relatively high. (2) the total amount and type of PAHs produced by spontaneous combustion of coal gangue is larger than that contained in coal gangue before spontaneous combustion, and the distribution of PAHs in the process of spontaneous combustion accords with fractionation effect, that is, the PAHs obtained by simulation experiment is mainly LPAHs. The main PAHs in the autoignition residual samples was 4-ring PAHs. At the same time, 5 rings and 6 rings of PAHs were detected. The toxicity of PAHs produced by spontaneous combustion of coal gangue was enhanced, and the toxicity of PAHs generated by spontaneous combustion at low temperature was higher than that in high temperature environment. 3) the PAHs produced by spontaneous combustion of coal gangue is mainly low ring, and in the process of spontaneous combustion, The PAHs produced by oxidation at lower temperature (鈮

本文編號：1645984