Emergence
of a Negative Activation Heat Capacity during
Evolution of a Designed Enzyme
Posted on 2019-07-18 - 19:17
Temperature influences the reaction
kinetics and evolvability of
all enzymes. To understand how evolution shapes the thermodynamic
drivers of catalysis, we optimized the modest activity of a computationally
designed enzyme for an elementary proton-transfer reaction by nearly
4 orders of magnitude over 9 rounds of mutagenesis and screening.
As theorized for primordial enzymes, the catalytic effects of the
original design were almost entirely enthalpic in origin, as were
the rate enhancements achieved by laboratory evolution. However, the
large reductions in ΔH⧧ were
partially offset by a decrease in TΔS⧧ and unexpectedly accompanied by a negative
activation heat capacity, signaling strong adaptation to the operating
temperature. These findings echo reports of temperature-dependent
activation parameters for highly evolved natural enzymes and are relevant
to explanations of enzymatic catalysis and adaptation to changing
thermal environments.
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Bunzel, H. Adrian; Kries, Hajo; Marchetti, Luca; Zeymer, Cathleen; R. E. Mittl, Peer; Mulholland, Adrian J.; et al. (2019). Emergence
of a Negative Activation Heat Capacity during
Evolution of a Designed Enzyme. ACS Publications. Collection. https://doi.org/10.1021/jacs.9b02731