R eaction rate coefficient of fullerene ( C ) consumption by soot

The reaction of fullerene molecules with soot was studied by contacting sublimed C fullerenes with commercially 60 available carbon black particles at different temperatures in the range 1023–1273 K. Fullerene mass data collected both preand post-reaction were fit to a simple first-order kinetic model and yielded a temperature-dependent reaction rate expression. 28 21 The calculated collision efficiency of the reaction is of the order 10 and the activation energy is |9.8 kcal mol , which would be consistent with a surface diffusion reaction or a heterogeneous reaction. Simple extrapolation of the observed rate to the conditions of a fullerene forming flame would give a consumption rate six orders of magnitude too small to account for the rate of fullerene consumption observed in the post-flame zone of a fullerene-forming benzene /oxygen/argon flame. Extrapolation of the reaction rate to flame conditions also shows that the rate of consumption calculated here is too small to account for observed oscillations in the fullerene concentration profile which can be related to changes in the relative rates of consumption and formation. Calculation of activation energies required for the extrapolation of rates observed here to match those observed in flames yields significantly larger values than those obtained in the present study and are so large as to suggest that mechanisms other than those studied here control fullerenes consumption in flames. Other mechanistic possibilities for the consumption of fullerenes in flames include reactions of fullerenes with other flame species and fullerene–soot reactions in which soot reactivity depends on soot reactions with other flame species.  2003 Elsevier Ltd. All rights reserved.