Illinois No．6煤中有机氮和硫赋存形态的研究

Investigation on the Existing Form of Organonitrogen and Organosulfur Compounds in Illinois No.6 Coal

煤中氮和硫是造成环境污染的重要来源,其赋存形态的研究广受关注.选用美国标准煤Illinois No.6煤的溶剂不溶组分(萃余煤)作为反应物,在温和条件下进行加氢热解,对热解产物进行分级萃取,用气相色谱-质谱联用仪分析萃取物的组成.结果表明,非催化加氢热解产物的总萃取率为4.1%,而在Ni的催化作用下,总萃取率高达13.5%;且后者有机氮、硫化物种类(27种)明显多于前者(10种).所检测到的含氮、硫化合物的类型主要包括异氰酸苯酯、异硫氰酸苯酯、苯胺、喹啉、二甲亚砜、硫醇、苯硫酚、硫醚、噻吩和噻蒽.这说明以萃余煤作为反应物,通过温和热解结合分级萃取的策略能够有效地从分子水平上揭示煤中有机氮、硫的赋存形态.

Nitrogen and sulfur in coal are one of the main sources of environment pollution. Much attention has been paid on the existing form of nitrogen and sulfur in coal. The solventinsoluble portion, namely residue, of the argonne premium coal Illinois No. 6 was subjected to mild hydrotreatment. The products derived from hydrotreatment were extracted with different solvents, and the extracts were analyzed by a gas chromatography-mass spectrometer. The results show that the total extract yield is 4.1% for the products from noncatalytic hydrotreat- ment, while that from Ni-catalyzed hydrotreatment can reach 13.5%. A total of twenty-seven organonitrogen and organosulfur compounds （ONCs and OSCs） are detected in the products from Ni-catalyzed hydrotreatment, and are much more than those from noncatalytic one （ten）. The identified ONCs and OSCs mainly include isocyanatobenzene, isothiocyanatobenzene, anilines, quinoline, dimethylsulfoxide, thiols, benzenethiols, sulfides, thiophenes, and thianthrene, which indicate that the strategy combing mild hydrotreatment and fractional extraction is efficient for disclosing the existing form of ONCs and OSCs in coal at the molecular level.