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A fundamental study of K sub 2 CO sub 3 -catalysis of hydrogasification of carbon and the role of oxygen in the catalysis

Thesis/Dissertation ·
OSTI ID:5004526
In this work fundamental experimental kinetic studies of K{sub 2}CO{sub 3}-catalyzed and non-catalyzed hydrogasification of carbon blacks at 700-865 C and 500 psi hydrogen pressure have been conducted to gain more insight into the role of K{sub 2}CO{sub 2} and oxygen complexes. In these studies, the effects of different catalyst loadings on hydrogasification rate, potassium loss at high temperature, the nature of oxygen complexes in carbon black, and effects of oxygen chemisorption at 400 and 800 C and/or degassing at 1000 C on non-catalyzed and the catalyzed hydrogasification have been investigated. From the effect of various oxygen surface groups on rate of hydrogasification, it is postulated that oxygen groups thermally desorb from the carbon surface and create nascent active sites which act as active sites for hydrogasification, hence enhancing the reactivity of the carbon. K{sub 2}CO{sub 3} catalytic activity and potassium losses are influenced by the nature of oxygen surface groups. The formation of stable and active potassium-containing species via interaction of K{sub 2}CO{sub 3} and oxygen complexes leads to reduced potassium losses and enhanced hydrogasification rates. The interaction of K{sub 2}CO{sub 3} with carbonyl groups forms both stable and active species. Interaction with basic oxygen complexes, which are relatively inactive in uncatalyzed hydrogasification, form active but unstable intermediate species. Interaction with acidic complexes is not well characterized from the experiments. Degassing removes non-basic groups and thermally anneals the nascent active sites, resulting in reduced gasification rate and increased potassium.
Research Organization:
Michigan State Univ., East Lansing, MI (USA)
OSTI ID:
5004526
Country of Publication:
United States
Language:
English