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Development of catalase like nanomaterials for tandem systems in the industrial synthesis of keto acids

Berstler, Calvin Andrew
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Abstract
The pursuit of novel strategies for conducting multi-step chemoenzymatic catalysis within a single reaction vessel remains a challenging undertaking. A chemoenzymatic process represents a distinct category of reactions wherein two or more consecutive transformations take place in a single reaction vessel, and subsequent post-reaction processing is minimized. This process leverages both enzymatic and chemical catalysis to efficiently generate desired products from commercially available starting materials, while removing the need to isolate intermediates. Driven by emerging techniques for designing biosynthetic materials that employ enzymes and inorganic species within single-pot systems, innovative use of catalytically active mesoporous nanomaterials as enzyme supports has potential to significantly enhance the overall performance and capabilities of the combined catalysts. In this work, we investigate material properties that influence the catalytic activity of metal phosphate materials. Specifically, we focus on further understanding the structure-function relationship of these materials which have catalase-like activity by synthesizing bulk and mesoporous cobalt phosphate materials with varying levels of crystallinity and surface areas. Catalases, which are known for their proficiency in decomposing hydrogen peroxide in biological systems, are used in a wide range of applications such as in medicine, catalysis, and environmental remediation. Our research demonstrates the impact of synthesis and aging temperatures on morphology and material properties of cobalt phosphate materials, as well as the resulting catalytic activity bringing structure-function relationships together. Furthermore, we explore the potential of employing mesoporous cobalt phosphate with enlarged pores and increased surface area as catalysts and stabilizing agents in a chemoenzymatic system to efficiently synthesize keto acids. By encapsulating and covalently immobilizing enzymes such as L-amino acid oxidase or L-glutamate oxidase within the pores of cobalt phosphate materials, we aim to develop a more efficient and recyclable hybrid tandem system that effectively bridges bio- and chemo-catalysis.
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