Montana State University
The presence of active site clusters resembling mineral motifs has led to several hypotheses regarding the primordial nature of complex metalloenzymes in biology. The active site clusters central to the catalytic activity of these metalloenzymes require a number of accessory proteins to produce, suggesting a complex evolutionary history for these metalloproteins. Thus, experimental investigation of the origins and evolutionary histories of maturation proteins, in addition to the structural proteins, holds tremendous promise for understanding the deep evolutionary history of these complex metalloproteins. Here, we present experimental evidence from two case studies that reveal several potentially unifying themes in metalloenzyme evolution. Collectively, the empirical data from these analyses challenge the paradigm that complex metalloenzymes are primordial in nature and alternatively suggest a stepwise evolutionary history for metalloprotein active site cluster synthesis, resulting in enzymes with altered substrate specificity and/or enhanced catalytic activity.
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