The limited scope of DNA-compatible chemistry restricts the types of chemical features that can be incorporated into DNA-encoded libraries (DELs). Here, a method to synthesize DNAconjugated polycyclic isoxazolidines via a [3+2] nitrone-olefin cycloaddition is described. The reaction is compatible with many olefin-containing substrates and diverse N-alkylhydroxylamines. The ability to perform subsequent DNA ligation and PCR amplification was also confirmed. This methodology facilitates the synthesis of DELs containing topographically complex compounds with underexplored chemical features.
Membraneless organelles are droplets in the cytosol that are regulated by chemical reactions. Increasing studies suggest that they are internally organized. However, how these subcompartments are regulated remains elusive. Herein, we describe a complex coacervate‐based model composed of two polyanions and a short peptide. With a chemical reaction cycle, we control the affinity of the peptide for the polyelectrolytes leading to distinct regimes inside the phase diagram. We study the transitions from one regime to another and identify new transitions that can only occur under kinetic control. Finally, we show that the chemical reaction cycle controls the liquidity of the droplets offering insights into how active processes inside cells play an important role in tuning the liquid state of membraneless organelles. Our work demonstrates that not only thermodynamic properties but also kinetics should be considered in the organization of multiple phases in droplets.
Molecular machines, such as ATPases or motor proteins,
couple the
catalysis of a chemical reaction, most commonly hydrolysis of nucleotide
triphosphates, to their conformational change. In essence, they continuously
convert a chemical fuel to drive their motion. An outstanding goal
of nanotechnology remains to synthesize a nanomachine with similar
functions, precision, and speed. The field of DNA nanotechnology has
given rise to the engineering precision required for such a device.
Simultaneously, the field of systems chemistry developed fast chemical
reaction cycles that convert fuel to change the function of molecules.
In this work, we thus combined a chemical reaction cycle with the
precision of DNA nanotechnology to yield kinetic control over the
conformational state of a DNA hairpin. Future work on such systems
will result in out-of-equilibrium DNA nanodevices with precise functions.
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