Research projects within Glover Group

Bioinspired strategies for solar driven generation of fuel and feedstocks

Making energy and chemical resources sustainable, carbon neutral and non-toxic on a global scale is a huge challenge, that we must necessarily realize to mitigate anthropogenic pollution and climate change. The development of catalysts to produce energy storing molecules and/or chemical feedstocks that meet the above requirements would represent a large step in the right direction. Research in the Glover group is aimed at developing new light activated catalyst systems to produce solar fuels and chemical feedstocks. We are further interested in understanding catalysis at the mechanistic level to inform on how best to make new systems more robust and efficient.

Catalysis in Nature is carried out by enzymes where catalyst centers are protected and supported by highly functional protein scaffolds. Nature’s enzymes are not necessarily suited for industrial scale processes; a given enzyme typically operates under a narrow window of conditions to perform a very specific chemical reaction. Our approach hybridizes well-defined de novo proteins with inorganic catalysts and photosensitizers to give an “all-in-one” photocatalyst to target a wide range of chemical reactions such as water oxidation, proton reduction, or carbon dioxide reduction. Use of the well-defined α3 de novo protein scaffold allows us to explore different coordination geometries and tune redox properties of the catalyst center through the use of different natural and unnatural amino acids in the coordination environment. The protein-catalysts are developed to be advantageously: free of noble metals, water soluble and protective against deleterious side chemistry. These properties make such protein-inorganic catalysts more sustainable than the status quo of purely inorganic systems.

The α3 de novo protein hybrids are amenable to detailed structural, electrochemical and transient spectroscopic studies which enable us to detect thermodynamics and kinetics of photoactivated redox events leading up to and during catalysis. These investigations will provide rates and mechanisms for redox events, i.e. electron transfer and proton-coupled electron transfer processes that are at the heart of catalysis. A detailed understanding of these redox processes allows us to make informed modifications to the protein and coordination environment that optimize catalysis.