Multiple transient response methods to identify mechanisms of heterogeneous catalytic reactions

Identification of mechanisms of heterogeneous catalytic reactions is challenging because there are few effective in-situ techniques with which to determine reactive intermediates on surfaces. An effective multiple transient technique consisting of a combination of a broadened pulse with step changes and a sharp isotopic pulse was developed in our group. This technique provides much richer dynamic information than is obtainable from experiments with individual pulses or step changes in reactant concentration. In this Account, we illustrate the method by its application to high-temperature heterogeneous catalytic reactions.