The increased recognition that molecular species do not always remain homogeneous under catalytic conditions, instead depositing on the electrode surface, has brought new attention to the challenge of differentiating homogeneous or heterogeneous catalysis.  In some cases, molecular “catalysts” are revealed to be pre-catalysts, undergoing chemical transformations to form heterogeneous electroactive species that are often no longer molecular in nature. Other catalysts undergo changes in solubility upon reduction and/or protonation, aggregating and adhering to the electrode surface while maintaining the integrity of their molecular core. Using case studies, this talk will discuss how electrochemical methodologies and surface analytical techniques can be leveraged to elucidate the mechanisms by which coordination complexes undergo transformations to yield heterogeneous species. From these data, we can begin to pinpoint the parameters that govern electrochemical deposition of heterogeneous materials and reveal the mechanisms by which molecular precursors transform into surface-adsorbed species.

Interplay between homogeneous coordination complexes and surface-adsorbed films in fuel-production catalysis

2019 Spring National Meeting

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