A remote surface loop modulates core structure and cold activity in phosphopantetheine adenylyltransferase

远程表面环调节磷酸泛酰巯基乙胺腺苷酰转移酶的核心结构和冷活性

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Abstract

Phosphopantetheine adenylyltransferase (PPAT), a key enzyme in the universal Coenzyme A biosynthetic pathway, is essential for cellular metabolism. However, the adaptive mechanisms of PPAT in psychrophilic (cold-adapted) organisms remain poorly understood. Here, we characterize PPAT from the psychrophilic methanotroph Methylocapsa palsarum (MpaPPAT). Sequence analysis identified a unique five-amino-acid insertion (SCRLS) within a surface-exposed loop, a feature conserved among psychrophilic homologues. To investigate its function, we determined the crystal structures of wild-type (WT) MpaPPAT and a loop-deletion mutant (MpaPPAT(Δ67-71)) and performed comparative biochemical analyses. Structurally, MpaPPAT forms a dimer-of-trimers hexamer. Biochemically, WT MpaPPAT maintains high catalytic activity at low temperatures (10-20 °C), whereas the MpaPPAT(Δ67-71) mutant exhibits impaired cold activity. The mutant structure reveals that the deletion of the distant surface loop induces a long-range allosteric change, resulting in a dual impairment: 1) a stabilization and rigidification ("clamping") of the central α-helix 4 (H4) at the hexameric core interface, and 2) a dramatic shift in the central pore's electrostatic potential from positive (WT) to negative (mutant). Our findings reveal that the SCRLS insertion is a critical allosteric modulator that provides a sophisticated dual mechanism for enzymatic cold adaptation. It maintains the conformational flexibility of the hexameric core, preventing the "clamping" effect, and simultaneously ensures a positively charged central channel to electrostatically steer negatively charged substrates (ATP and phosphopantetheine) into the active site, thereby overcoming the kinetic challenges of a low-temperature environment.

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