Temperature-programmed simulation experiments of saturated hydrocarbons with calcium sulfate and element sulfur were compared in this study. Based on the variation analysis of the yields and evolvement features of gas...Temperature-programmed simulation experiments of saturated hydrocarbons with calcium sulfate and element sulfur were compared in this study. Based on the variation analysis of the yields and evolvement features of gaseous hydrocarbon (C1-C5) and inorganic gaseous CO2, H2 and H2S, the reaction mechanisms were analyzed and discussed. In the calcium sulfate-saturated hydrocarbon system, H2S was produced by a small quantity, which indicates this reaction belongs to the low-degreed thermal sulfate reduction (TSR) and is featured of self-pyrolysis. In the sulfur-saturated hydrocarbon system, the heated sulfur becomes sulfur radical, which has strong catalysis capability and can fasten the cracking of C―H bond in the alkyl group in the saturated hydrocarbons. As a result, the cracking of C―H bond leads to the yields enhancement of CO2 and H2, and at the same time, H2S was produced since the cracked hydrogen can be instantly combined with sulfur radical. Therefore, this reaction in the sulfur-hydrocarbon system belongs to the catalysis of sulfur radical. Furthermore, the promoted pyrolysis effects of C6+ hydrocarbons by sulfur radical in the low-temperature stage in the sul- fur-hydrocarbon system, together with the consumption effects of gaseous hydrocarbon in the high-temperature stage in the calcium-hydrocarbon system, result in the crossed phenomenon of the gaseous hydrocarbon yields curves.展开更多
基金Supported by National Basic Research Program of China (Grant No. 2006CB701404)CAS Innovation Project (Grant No. KZCX2-YW-114-1)+1 种基金National Natural Science Foundation of China (Grant No. 40873032)the Earmarked Fund of the State Key Laboratory of Organic Geochemistry (Grant No. SKLOG2008A01)
文摘Temperature-programmed simulation experiments of saturated hydrocarbons with calcium sulfate and element sulfur were compared in this study. Based on the variation analysis of the yields and evolvement features of gaseous hydrocarbon (C1-C5) and inorganic gaseous CO2, H2 and H2S, the reaction mechanisms were analyzed and discussed. In the calcium sulfate-saturated hydrocarbon system, H2S was produced by a small quantity, which indicates this reaction belongs to the low-degreed thermal sulfate reduction (TSR) and is featured of self-pyrolysis. In the sulfur-saturated hydrocarbon system, the heated sulfur becomes sulfur radical, which has strong catalysis capability and can fasten the cracking of C―H bond in the alkyl group in the saturated hydrocarbons. As a result, the cracking of C―H bond leads to the yields enhancement of CO2 and H2, and at the same time, H2S was produced since the cracked hydrogen can be instantly combined with sulfur radical. Therefore, this reaction in the sulfur-hydrocarbon system belongs to the catalysis of sulfur radical. Furthermore, the promoted pyrolysis effects of C6+ hydrocarbons by sulfur radical in the low-temperature stage in the sul- fur-hydrocarbon system, together with the consumption effects of gaseous hydrocarbon in the high-temperature stage in the calcium-hydrocarbon system, result in the crossed phenomenon of the gaseous hydrocarbon yields curves.