Publication date: 16th April 2014
Merging of molecular and material chemistry yields unique heterogeneous molecular-material catalyst constructs made of earth-abundant elements that are (a) well-defined and tunable at the molecular scale, (b) extremely robust, yet simultaneously (c) highly reactive, which makes them excellent candidates to take on the most challenging catalytic processes. Combining all of these properties in a single functional system has always been a major goal in catalyst development. Recently, this goal has become an important enterprise as we develop catalysts for H2O splitting and CO2 reduction; for effective applications, these reactions need to be performed at a scale that surpasses any other current chemical process.
The cages of a crystalline MOF [e.g. MIL-101(Cr)] were used to cage isolate a highly reactive high-valent Mn-based molecular water-oxidation catalyst. Isolation of only one molecule of catalyst per cage prevented the catalyst’s degradation pathways and allowed the catalyst to oxidize water at one of the fastest rates ever recorded, that lasted for weeks.
We realized that metal-sites, as nodes of a MOF, enjoy orders of magnitude higher resistance towards permanent ligand-displacement (that leads to the degradation of a catalyst). However, at the kinetic scale requiring transient ligand-displacement, the metal site remains as active as its molecular counterpart; this is a necessity for catalytic turnover. This structural bolstering of metal sites as nodes in a MOF has been exploited to develop MOF-based systems for light-driven H2 production.
All our catalyst-constructs are heterogeneous, but with the help of the well-defined nature of the constructs, they could be tuned for further improvement of activity or change of functionality to diversify its application.
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