Engineering Artificial Metalloenzymes for Selective Catalysis in Complex Media
Abstract
Controlling the selectivity of chemical reactions and conducting these reactions in complex aqueous media, including unprocessed samples from both environmental and human sources, could greatly expand our ability to analyze, utilize, and synthesize chemicals in a non-laboratory setting. Artificial metalloenzymes (ArMs) could achieve these goals by combining the reactivity of synthetic metal catalysts and the adaptability and efficiency of enzymes. This proposal describes the development of ArMs generated from protein or enzyme scaffolds and transition metal-based CH functionalization catalysts bearing reactive anchoring groups. Enclosing these catalysts within structurally defined yet genetically mutable scaffolds will provide exquisite control of their reactivity and tolerance of specific environmental contaminants and bulk media components. The impact of this control on catalysis will be studied, and ArMs will be evolved to promote challenging chemical transformations in complex aqueous media. In addition, a focus on immobilized ArMs containing base metal catalysts will both ensure the low cost and reusability of these systems to enable their use in real -world applications. The proposed ArM technology will impart selectivity to a range of non-biological C-H bond functionalization reactions to facilitate detection, degradation, and utilization of organic compounds in field environments. Focusing in part on immobilized ArMs generated from base metal catalysts will substantially improve the practicality of the proposed ArMs relative to any reported to date. In addition, the ArM platform will provide increased control over the reactivity of base metal complexes and enable assembly of modular flow systems driven by disposable syringes to enable multistep chemical manipulation of target molecules.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- May 07, 2018
- Source ID
- W911NF1810034
Entities
People
- Jared C Lewis
Organizations
- Army Contracting Command
- United States Army
- University of Chicago