Green synthesis of polymer materials <i>via</i> enzyme- initiated RAFT polymerization

Kumar, Sonu; Gaddala, Raviteja; Thomas, Sabu; Schumacher, Joshua; Schönherr, Holger

doi:10.1039/d4py00294f

Polym. Chem.

2024

DOI: 10.1039/d4py00294f

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Green synthesis of polymer materials via enzyme- initiated RAFT polymerization

Sonu Kumar,

Raviteja Gaddala,

Sabu Thomas

et al.

Abstract: Enzymes are well-known biocatalysts for natural metabolic reactions and synthetic organic reactions. For many decades enzymatic catalysis has been successfully implemented for the in vitro synthesis of polymers and their...

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Cited by 2 publications

References 127 publications

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Catalyzing PET‐RAFT Polymerizations Using Inherently Photoactive Zinc Myoglobin

Anderson,

Gomez,

Zhang

et al. 2024

Angewandte Chemie

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Protein photocatalysts provide a modular platform to access new reaction pathways and affect product outcomes, but their use in polymer synthesis is limited because co‐catalysts and/or co‐reductants are required to complete catalytic cycles. Herein, we report using zinc myoglobin (ZnMb), an inherently photoactive protein, to mediate photoinduced electron/energy transfer (PET) reversible addition‐fragmentation chain transfer (RAFT) polymerizations. Using ZnMb as the sole reagent for catalysis, photomediated polymerizations of N,N‐dimethylacrylamide in PBS were achieved with predictable molecular weights, dispersity values approaching 1.1, and high chain‐end fidelity. We found that initial apparent rate constants of polymerization increased from 4.6×10–5 s−1 for zinc mesoporpyhrin IX (ZnMIX) to 6.5×10–5 s−1 when ZnMIX was incorporated into myoglobin to yield ZnMb, indicating that the protein binding site enhanced catalytic activity. Chain extension reactions comparing ZnMb‐mediated RAFT polymerizations to thermally‐initiated RAFT polymerizations showed minimal differences in block copolymer molecular weights and dispersities. This work enables studies to elucidate how protein modifications (e.g., secondary structure folding, site‐directed mutagenesis, directed evolution) can be used to modulate polymerization outcomes (e.g., selective monomer additions towards sequence control, tacticity control, molar mass distributions).

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Catalyzing PET‐RAFT Polymerizations Using Inherently Photoactive Zinc Myoglobin

Anderson,

Gomez,

Zhang

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

Catalyzing PET‐RAFT Polymerizations Using Inherently Photoactive Zinc Myoglobin

Anderson,

Gomez,

Zhang

et al. 2024

Angew Chem Int Ed

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Green synthesis of polymer materials via enzyme- initiated RAFT polymerization

Abstract: Enzymes are well-known biocatalysts for natural metabolic reactions and synthetic organic reactions. For many decades enzymatic catalysis has been successfully implemented for the in vitro synthesis of polymers and their...

Cited by 2 publications

References 127 publications

Catalyzing PET‐RAFT Polymerizations Using Inherently Photoactive Zinc Myoglobin

Catalyzing PET‐RAFT Polymerizations Using Inherently Photoactive Zinc Myoglobin

Catalyzing PET‐RAFT Polymerizations Using Inherently Photoactive Zinc Myoglobin

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