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在第三章中已经述及,吐哈盆地在早中侏罗世时,生物已相当繁盛,从本次研究的下中侏罗统发现的大量动植物化石就足以证明这一事实。在本次研究野外实地考察时,时常可以发现露头中保留有植物化石或硅化木,钻孔中揭露的4层主煤层(M1、M2、M3、M4)也是植物繁盛时留下的证据,即使在含铀的砂岩层中也夹有大量煤(或植物)碎屑。
镜下见到氧化带、氧化还原过渡带及还原带样品中的有机质有所不同,图版10 图7(A)为强氧化带岩石中的有机质,可以看到有机质已经被完全降解破坏而呈“流体状”,并渗透到矿物裂隙中。图版10图8(B)为弱氧化带岩石中有机质,有机质已被降解破坏,但仍保留有植物胞腔结构。图版11图1,2(C,D)为氧化还原过渡带和还原带岩石中有机质,可以看到有机质微粒基本保留原样,未被破坏降解。
据研究,吐哈盆地西南部下中侏罗统中以煤为主的有机质属腐殖型有机质,尚处于褐煤阶段,变质程度较低,其中含有较多腐殖质成分(据向伟东,1999)。在这时首先要涉及到腐殖质形成问题,这个问题也关系到吐哈盆地有机质来源问题。
关于腐殖质的形成,是腐殖质化学中很重要一个研究领域,也是一个很复杂的问题,因为它涉及到有关腐殖质的一些重要性质。很多年来,许多学者一直在从事这项研究。最近的研究已经揭示了腐殖质形成的事实。
腐殖质的形成可分成四步(图4—12中1、2、3、4),每一步均代表腐殖质的一个形成阶段,主要阶段已为经典理论,即木质素理论(The lignin theory)所阐述,它是腐殖质形成的第一步。后来很多学者都提出腐殖质形成中包括醌的形成在内的多酚理论(The polyphenol theory),为腐殖质形成的第二至三步。最近的研究发现在自然界中腐殖质的形成还包括第四步,即糖-胺浓缩阶段(Sugar amine condesation)(图4—12)。这四个阶段可以出现于任何种类腐殖质的形成过程中,但其发生的程度和在每一阶段所起的作用可能不同。木质素阶段在湿润的沉积物中占主导地位,而多酚的合成在一些泥炭土壤中相当重要,而在温度、湿度等变动较大的地表,糖-胺浓缩阶段则占主导地位。
多年以来,人们一直认为腐殖质来源于木质素。按照这个理论,木质素未彻底被微生物分解时,残余物变成部分腐殖土。在第一阶段中,木质素的变化包括:脱甲氧基(OCH3),同时产生O—羟基苯;脂肪族链氧化而形成COOH官能团。这个理论的证据是:①木质素和腐殖酸被真菌和细菌降解都相当困难;②二者在酒精和吡啶C5H5N中都部分溶解;③二者在碱中溶解而在酸中沉淀;④二者都含有OCH3官能团;⑤在自然条件下,二者都呈酸性;⑥当木质素在碱液中加热时,会转变成含甲氧基的腐殖酸;⑦腐殖酸和氧化的木质素都有相似的成分。
木质素比其他植物组织更不容易被微生物分解,在自然界需氧来彻底降解。在氧的作用下,木质素被破坏成低分子量产物,利于腐殖质的合成(图4—13)。
在腐殖质形成的第三个阶段,腐殖质的合成中,木质素仍然起着重要作用,但是作用的方式不同,在这里酚醛和酸在微生物破坏木质素阶段被释放出来,经过酶的催化转变成醌,在氨基化合物出现或缺失的情况下聚合而形成类似腐殖质的大分子。
图4—12 腐殖质形成
(据 Stevenson,1982)
图中1、2、3和4为腐殖质形成的4个步骤
在腐殖质形成的第二阶段,多少有些相似于第三阶段,只是多酚从非木质素碳源(纤维素等)被微生物作用而合成。多酚然后在酶催化下氧化成醌而转变为腐殖质。按照现在的观点,木质素来源的醌与微生物合成的醌一起,构成了腐殖质的主要构架。
在腐殖质形成第四个阶段,还原糖和氨基酸随着微生物合成副产品的形成,经催化作用,在中等温度条件下形成含氮聚合物。在自然条件下,这个反应过程相当缓慢。这个阶段的显著特点是在微生物的作用下,产生大量反应体(糖和氨基酸等)。糖-胺浓缩最后的反应包括胺与糖醛基形成氮替代的葡基胺;葡基胺形成氮替代—1氨基—脱氧—2酮 糖;三碳链醛和酮糖的形成,如1羟基—2丙酮(CH3COCH2OH),二乙酰等;以及脱水和形成还原酮、羟甲氧基糠醛。所有这些化合物高度反应并迅速聚合,在氨基化合物出现的条件下形成腐殖酸。
从煤的形成角度分析,腐殖酸是植物残骸在微生物参与下经过复杂的化学和生物分解及合成反应生成的产物。泥炭是植物转变成煤的初始阶段产物。植物残骸在一些微生物的作用下发生氧化分解,改变了原来的形态和结构,变成了含水量很高的棕褐色物质。这种物质称为泥炭或泥煤。这个过程称为泥炭化阶段。在泥炭化阶段,植物残骸中易水解的组分如脂类、半纤维素等发生了深度的分解,同时,分解产物还会互相作用,合成出植物组成中原来没有的腐殖质。植物中比较稳定的物质如脂肪、蜡质和树脂形成了泥炭中的沥青。泥炭中除含有大量的腐殖质和沥青外,仍含有未完全分解的植物残体。所以泥炭中还残留有植物原有的根、茎、叶等组织残体。腐殖质是泥炭有机质中一重要组分,中国泥炭中腐殖质含量一般为20%~40%。泥炭埋于地下后,在温度、压力等作用下,经过地质成岩作用转化为褐煤。
泥炭转化成褐煤以后,后者中一般不再含有未分解的植物组织,而腐殖质继续存在,但由于腐殖质的中性氧原子转变成醇烃基,经脱氧、胶羧基作用,腐殖质酸性降低,开始老化,因此腐殖质含量减少。同时,腐殖酸元素组成也有很大变化,碳含量增加,氧、氢含量减少。
褐煤经高温、高压等地质作用后变成烟煤和无烟煤。这时已经不存在游离腐殖质了。风化煤是由各种煤经地表风化作用而形成的产物。其中也含有腐殖质。
图4—13 有关腐殖质形成的木质素理论示意图
因此,一般随着煤炭变质程度加深,其中腐殖质含量逐渐减少,煤中碳含量增加,氢、氧含量减小,表4—3为不同种煤中腐殖质变化情况。
表4—3 各种煤中腐殖质含量变化情况
(据何立千,2000)
不同来源的腐殖质在结构、组成及性质上都有所不同。
在成岩过程中,由于沉积物的环境条件不同,腐殖质或是被微生物缓慢地作用,或是被变为油母岩或类煤产物。碳化作用起因于微弱附着的多糖和蛋白质残余物,以及侧链和含氧官能团特别是COOH和OH的丢失。这些变化伴随着碳含量的增加和氧含量的减少。其他的变化还包括氮的丢失和在碱液中溶解性的降低。所有抗生物分解的黄腐酸和腐殖酸将最终经成岩作用改变为油母岩和类煤物质。在由黄腐酸和腐殖酸转变到褐煤物质的过程中,首先是COOH基消失,随后是OCH3和C=O基的消失。在黄腐酸、腐殖酸、褐煤中作为COOHO的百分含量变化可见图4—14。
由此可见吐哈盆地西南部的有机质(主要是其中腐殖质)来源于下中侏罗统中埋藏的煤及碎屑。是植物经过漫长的地质历史,在复杂的成煤过程中,由氧化、微生物等作用分解而形成的。
图4—14 形成为COOH的氧的含量
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