Aspects of kerogen oxidative dissolution in subcritical water using oxygen from air

摘要

Society's growing demands on everyday products and materials are increasingly difficult to meet in an environment that seeks to avoid petroleumbased processes. Instead of abandoning fossil materials altogether, more research should be done on their efficient and clean conversion. One option for this is the oxidative dissolution of kerogen in water under conditions that satisfy the subcritical range (T = 150-200 degrees C, pO(2) = 0.5-4 MPa). The resulting mixture contains a substantial amount of various aliphatic carboxylic and dicarboxylic acids. Both batch and semi-continuous processes were set up to find the main factors and optimal conditions for the kerogen dissolution process. The rate of transformation of organic carbon to dissolved organic compounds was mainly influenced by elevated temperature and oxygen partial pressure. To obtain high yields of organic carbon dissolution and to avoid the formation of excess CO2, the oxidation of kerogen should be carried out fast (< 1 h) and under high oxygen pressure. By employing a temperature of 175 degrees C and O-2 pressure of 2 MPa, over 65% of the initial organic carbon dissolves in about one hour. Prolonged reaction times or harsher oxidation conditions resulted in a rapid degradation of dissolved matter and also of the valuable products formed. The organic matter content of the initial oil shale had a direct effect on the further degradation of dicarboxylic acid and consequently on the overall yield. The suitability of using a trickle-bed reactor for kerogen dissolution is discussed in detail on the basis of experimental results.