How hard is mechanism elucidation in catalysis? Combinatorial analysis of C1 chemistry
Most chemical reactions occur over multiple steps whose identity is elucidated by experiment, yielding a reaction mechanism. Knowledge of cognitive science suggests that mechanism elucidation can be viewed as a knowledge-guided search within a combinatorial space. The MECHEM computer program searches this space comprehensively for the simplest plausible mechanisms. We use MECHEM to find mechanisms for Fischer-Tropsch chemistry and CO2 re-forming of methane, both heterogeneous catalytic reactions of current importance. The results reveal hundreds of equally simple mechanisms consistent with evidence. Hence, mechanism elucidation in catalysis is a much harder problem than is ordinarily realized.
Valdes-Perez
RE
Computer Science Department, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, USA. valdes@cs.cmu.edu
Zeigarnik
AV