论文中文题名: | 光-生耦合对神府煤的转化研究 |
姓名: | |
学号: | 06127 |
保密级别: | 公开 |
学科代码: | 081902 |
学科名称: | 矿物加工工程 |
学生类型: | 硕士 |
学位年度: | 2009 |
院系: | |
专业: | |
第一导师姓名: | |
论文外文题名: | Study on Photo-biological Co-conversion of Shenfu Coal |
论文中文关键词: | |
论文外文关键词: | Shenfu coal Bioconversion Humic acid Photo-biological co-conversion |
论文中文摘要: |
煤炭是一种不可再生的碳烃资源,具有特殊的化学结构和特性,其直接能源利用不仅造成严重的环境污染,而且造成这一重要资源的极大浪费。煤的生物转化具有转化条件温和、无污染等优点,是煤炭科学技术研究的新领域。提高煤的生物转化率和产物选择性是煤生物转化研究热点之一。因此,采用光-生耦合的方法对煤进行转化,达到提高煤的生物转化率和产物选择性的目的。
以神府煤为研究对象,用神府煤洗煤废水中优选出的粗壮串珠霉(Monilia crassa Sh.Et Dodge)、黄绿青霉(Penicillium citreo-viride Biourge)和黄杆菌属(Flavobacterium Bergey et al,1923.97),对不同光氧化程度的神府煤进行转化。用FTIR和GC/MS分析了生物转化产物结构,研究了光-生耦合转化的协同效应。进一步结合煤基腐殖酸、萘(NAP)和4,4,-二羟基二苯基丙烷(BPA)的生物转化研究结果,提出了光-生耦合转化机理。
在光氧化装置中,对煤样进行紫外光氧化预处理研究。结果表明,光氧化6h和4h的神府煤(SFC)的腐殖酸的产率分别为10.91%和2.35%。光氧化4h和8h神府镜煤(V-SFC)的腐殖酸的产率分别为5.30%和1.33%。
用焦磷酸钠碱液对光氧化6h和4h的SFC及4h和8h的V-SFC抽提后的残渣在液体无机盐培养基中进行微生物转化。结果表明,光氧化6h神府煤,用粗壮串珠菌经8天生物转化后,总转化率为39.72%,生物转化残煤的腐殖酸的总产率为35.54%;光氧化8h神府镜煤,经黄杆菌属生物转化8天后,总转化率为30.80%,生物转化残煤的腐殖酸的总产率为23.71%。由此可见,神府煤经光氧化与生物耦合转化之间存在协同效应。
FTIR表征了SFC和V-SFC经光-生耦合转化后水溶性产物和残煤结构。结果发现,SFC经转化后,芳环含量减少,同时脂肪链和含氧官能团增加;V-SFC转化后,含氧官能团的数量增加。微生物转化光氧化SFC和V-SFC的水溶性产物、碱沉淀产物和碱可溶性产物中主要含有羟基、酰胺-N-O-、CH-(CH3)、醚等官能团。
用丙酮和四氢呋喃(THF)对光-生耦合转化神府煤的残渣进行抽提,GC/MS表征了残渣的结构。原煤经光-生耦合转化后的丙酮可溶物中含量最多的为1-甲基-4-[(4-丙基)]乙炔基苯,其次为惹烯。丙酮抽提后的残煤经THF抽提后,含量最多的为二(2-乙基己基)邻苯二甲酸酯,其次为邻苯二甲酸二丁酯。原煤的溶剂可溶物中不含以上四种物质。
对模型化合物和光氧化煤基腐殖酸进行生物转化,分析了模型化合物及光氧化煤基腐殖酸转化后的组成、结构及机理。基于以上实验结果,提出了神府煤的光-生耦合转化机理。
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论文外文摘要: |
Coal is a non-renewable hydrocarbon resource, and it is special chemical structure and characteristics. The direct application of coal not only brought environmental pollution seriously, but also led to wasting resources extremely. Bioconversion of coal has some advantages, such as milder condition and no pollution. It was new field of sciences. One of research focus was increasing bioconversional yield and choosing products. In order to improving bioconversional yield and choosing products, the coal was conversed by photo oxidation coupling with bioconversion.
Taking Shenfu coal as participarts, different photo-oxidazed SFC was bioconversed by Monilia crassa Sh.Et Dodge, Penicillium citreo-viride Biourge and Flavobacterium Bergey et al,1923.97 which were extracted from Shenfu coal-washing waste water. Photo-biological co-conversion and the structure of bioconversion products were studied using FTIR and GC/MS. Further based on the experimental results that bioconversion of coal cased humic ,NAP and BPA. The mechanism of photo-biological co-conversional coal was proposed.
Coal was pretreated by UV-photocatalytic oxidation in fixed bed photo-oxidation reactor. The results showed that the humic acid content of SFC photo-oxidazed for 6h was up to 10.91%,and 4h was up to 2.35%. The humic acid content of V-SFC photo-oxidazed for 4h was up to 5.30%, and 8h was up to 1.33%.
The SFC photo-oxidazed for 6h and 4h .The V-SFC photo-oxidazed for 4h and 8h .The photo-oxidazed coal was extracted by sodium pyrophosphate alkali liquid. The residues were bioconversed in inorganic salts liquid medium. The results showed that SFC was conversed by photo-oxidazed for 6h coupling of Monilia crassa Sh.Et Dodge for 8 days, the total conversion yield was 39.72%, the yield of humic acid was up to 35.54% ,and V-SFC was conversed by photo-oxidazed for 8h coupling of Flavobacterium Bergey et al,1923.97 for 8 days, the total conversion yield was 30.80%,the yield of humic acid was up to 23.71%. It has coordination effect that photo-oxidation coupling with bioconversion.
After photo-biological co-conversed, the products structure was characterized by FTIR. It was found that the content of aromatic was decreased, meanwhile the content of fat chains and oxygen-containing functional groups was increased in SFC.About V-SFC, the number of oxygen-containing functional groups was increased. SFC and V-SFC was photo-biological co-conversed, the products of water-soluble, precipitate treated by alkali and alkali soluble mainly contained –OH, amide, -N-O-,CH-(CH3) and ether.
The residues that coal was conversed by photo-biological co-conversion. And the residues were extracted by propanone and THF. The structure of residues was characterized by GC/MS. After photo-biological co-conversion of SFC, the content of Benzene, 1-methyl-4-[(4-propylphenyl)ethynyl]- was maximum, and Phenanthrene, 1-methyl-7- (1-methylethyl) was second for the soluble extracted by propanone. After propanone extraction, the residuals were further extracted by THF. The content of Bis(2-ethylhexyl) phthalate was maximum, and dibutyl phthalate was second for the soluble extracted by THF. The solvent soluble matter of SFC which without photo-biological co-conversion didn’t contain above four compounds.
Model compounds and coal based humic acid were conversed by strains. The composition, structure and mechanism was studied.Base on above experimental results, the photo-biological co-conversional mechanism was presented.
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中图分类号: | TQ530.2 |
开放日期: | 2010-03-19 |