Fluorinated amino acids, fAAs, have long attracted interest as non-proteinogenic building blocks that can tune protein stability and introduce 19F NMR handles, but deploying them inside a folded protein's hydrophobic core while preserving function has proven difficult. Replacing core residues with fluorinated analogues changes sidechain volume and polarity simultaneously, and it remained unknown how far a natural core could be repacked with unnatural sidechains before activity collapsed. The combinatorial problem compounds the difficulty: protein sequence space is vast, and experimental screening methods generally lack the throughput to sample all possible permutations of fAA incorporation across even a handful of positions. Genetic code reprogramming combined with mRNA display offers the required throughput in principle, yet prior to this work those methods had not been applied to evolve fAA-containing folded proteins with a defined biological activity.
Researchers in the Suga Group at The University of Tokyo, published in Angewandte Chemie International Edition, addressed this gap with a two-step platform combining genetic code reprogramming, mRNA display-based in vitro selection, and microwave-assisted solid-phase peptide synthesis. The flexible in vitro translation system FIT loaded six chemically distinct fluorinated non-proteinogenic amino acids into a randomized library based on chymotrypsin inhibitor 2, CI2, from barley; mRNA display then selected variants that inhibit chymotrypsin with nanomolar potency, with several more active than the wildtype and thermostabilities of up to 70 °C. The selection is agnostic to the precise structure of variants, so non-native folds could in principle be enriched, and the platform was validated using only CI2 as scaffold and chymotrypsin as target. The hits contain, to the authors' knowledge, the most site-specific fAA incorporations of any genetically encoded sequence with a defined protein fold.
The work demonstrates that substantially remodeling the structural core of a natural protein with non-proteinogenic amino acids need not erase its function, and the authors anticipate the platform will provide a foundation for de novo design of neoproteins with diverse functionalities.