Leveraging Triphenylphosphine-Containing Polymers to Explore Design Principles for Protein-Mimetic Catalysts DOI Creative Commons
Matthew A. Sanders, Supraja S. Chittari,

Jack R. Foley

и другие.

Опубликована: Апрель 15, 2024

Complex interactions between non-coordinating residues are significant yet commonly overlooked components of macromolecular catalyst function. While these have been demonstrated to impact binding affinities and catalytic rates in metalloenzymes, the roles similar structural elements synthetic polymeric catalysts remain underexplored. Using a model Suzuki-Miyuara cross-coupling reaction, we performed series systematic studies probe interconnected effects metal-ligand cross-links, electrostatic interactions, local rigidity polymer catalysts. To achieve this, novel bi-functional triphenylphosphine acrylamide (BisTPPAm) monomer was synthesized evaluated alongside an analogous monofunctional (TPPAm). In copolymer catalysts, increased initial reaction were observed for copolymers untethered by Pd complexation (BisTPPAm-containing) as compared Pd-cross-linked (TPPAm-containing). Further, incorporating through secondary structure-like revealed nonmonotonic relationships composition rate, demonstrating potential tunable behavior sphere interactions. Finally, rigorous cheminformatics featurization strategies statistical modeling, quantitated chemical descriptors substrate conditions on performance. Collectively, results provide insights into composition, structure, function protein-mimetic copolymers.

Язык: Английский

Leveraging Triphenylphosphine-Containing Polymers to Explore Design Principles for Protein-Mimetic Catalysts DOI Creative Commons
Matthew A. Sanders, Supraja S. Chittari,

Jack R. Foley

и другие.

Опубликована: Апрель 15, 2024

Complex interactions between non-coordinating residues are significant yet commonly overlooked components of macromolecular catalyst function. While these have been demonstrated to impact binding affinities and catalytic rates in metalloenzymes, the roles similar structural elements synthetic polymeric catalysts remain underexplored. Using a model Suzuki-Miyuara cross-coupling reaction, we performed series systematic studies probe interconnected effects metal-ligand cross-links, electrostatic interactions, local rigidity polymer catalysts. To achieve this, novel bi-functional triphenylphosphine acrylamide (BisTPPAm) monomer was synthesized evaluated alongside an analogous monofunctional (TPPAm). In copolymer catalysts, increased initial reaction were observed for copolymers untethered by Pd complexation (BisTPPAm-containing) as compared Pd-cross-linked (TPPAm-containing). Further, incorporating through secondary structure-like revealed nonmonotonic relationships composition rate, demonstrating potential tunable behavior sphere interactions. Finally, rigorous cheminformatics featurization strategies statistical modeling, quantitated chemical descriptors substrate conditions on performance. Collectively, results provide insights into composition, structure, function protein-mimetic copolymers.

Язык: Английский

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