Optimizing Catalysts for Solar Fuel Production: Spectroscopic Characterization of the Key Reaction Intermediates.

摘要

The purpose of this grant was to develop a new and general way to isolate key reaction intermediates in the condensed phase catalytic conversion of carbon dioxide and water into transportable solar fuels. To this end, we designed, constructed and implemented a chemical analysis apparatus to extract homogeneous catalysts from their native solution environment and isolate them for spectroscopic study. This was achieved using an electrospray atmospheric pressure interface to a custom built, multi-stage, cryogenically cooled photofragmentation mass spectrometer. The key advance incorporates a 10K processing stage, which freezes ions into well defined structures and coats them with an inert layer of weakly bound adducts. These cold aggregates were then complexed with target molecules to initiate chemical rearrangements under conditions where the reactions could be arrested prior to completion by rapid evaporation of the cryogenic solvent.