For the solar-powered water splitting reaction to proceed efficiently, new classes of light-absorbing sensitizers and hydrogen evolution catalysts are required. We have developed numerous molecular compositions based exclusively on coordination compound sensitizers and catalysts capable of reducing protons to hydrogen in pure water and water-rich solvent mixtures using visible light. In addition to the design, synthesis, and characterization of various molecules that serve either as sensitizers or catalysts in these solar energy conversion schemes, we have developed new apparatus' for parallel high-throughput screening of these photocatalytic compositions, monitoring pressure, GC, and MS in real-time throughout the time course of the photoreactions. This combinatorial approach to solar fuels photocatalysis has already led to significant understanding and optimization of numerous hydrogen-producing compositions, permitting us to focus on the best systems for detailed transient absorption and IR mechanistic studies. This presentation will highlight advances incorporating all first-row transition metal complexes, based on a recently developed class of Cu(I) sensitizers exhibiting unprecedented excited state lifetimes working in concert with Co(III) hydrogen evolution catalysts, as well as champion compositions functioning in pure water based on new classes of Ru(II) and Ir(III) sensitizers and Co(II) polypyridyl catalysts. Details related to the transient spectroscopy of these molecular catalytic systems will be presented.

Homogeneous approaches to solar hydrogen photocatalysis

248th National Meeting (2014)

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