Directed evolution provides insight into conformational substrate sampling by SrtA.

The Sortase family of transpeptidases are found in numerous gram-positive bacteria and involved in divergent physiological processes including anchoring of surface proteins to the cell wall as well as pili assembly. As essential proteins, sortase enzymes have been the focus of considerable interest...

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Main Authors: Muna Suliman, Vishaka Santosh, Tom C M Seegar, Annamarie C Dalton, Kathryn M Schultz, Candice S Klug, William A Barton
Format: Article
Language:English
Published: Public Library of Science (PLoS) 2017-01-01
Series:PLoS ONE
Online Access:https://journals.plos.org/plosone/article/file?id=10.1371/journal.pone.0184271&type=printable
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author Muna Suliman
Vishaka Santosh
Tom C M Seegar
Annamarie C Dalton
Kathryn M Schultz
Candice S Klug
William A Barton
author_facet Muna Suliman
Vishaka Santosh
Tom C M Seegar
Annamarie C Dalton
Kathryn M Schultz
Candice S Klug
William A Barton
author_sort Muna Suliman
collection DOAJ
description The Sortase family of transpeptidases are found in numerous gram-positive bacteria and involved in divergent physiological processes including anchoring of surface proteins to the cell wall as well as pili assembly. As essential proteins, sortase enzymes have been the focus of considerable interest for the development of novel anti-microbials, however, more recently their function as unique transpeptidases has been exploited for the synthesis of novel bio-conjugates. Yet, for synthetic purposes, SrtA-mediated conjugation suffers from the enzyme's inherently poor catalytic efficiency. Therefore, to identify SrtA variants with improved catalytic efficiency, we used directed evolution to select a catalytically enhanced SrtA enzyme. An analysis of improved SrtA variants in the context of sequence conservation, NMR and x-ray crystal structures, and kinetic data suggests a novel mechanism for catalysis involving large conformational changes that delivers substrate to the active site pocket. Indeed, using DEER-EPR spectroscopy, we reveal that upon substrate binding, SrtA undergoes a large scissors-like conformational change that simultaneously translates the sort-tag substrate to the active site in addition to repositioning key catalytic residues for esterification. A better understanding of Sortase dynamics will significantly enhance future engineering and drug discovery efforts.
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spelling doaj-art-76e6f14461e446219b8a4145c14c57ae2025-08-20T02:03:39ZengPublic Library of Science (PLoS)PLoS ONE1932-62032017-01-01128e018427110.1371/journal.pone.0184271Directed evolution provides insight into conformational substrate sampling by SrtA.Muna SulimanVishaka SantoshTom C M SeegarAnnamarie C DaltonKathryn M SchultzCandice S KlugWilliam A BartonThe Sortase family of transpeptidases are found in numerous gram-positive bacteria and involved in divergent physiological processes including anchoring of surface proteins to the cell wall as well as pili assembly. As essential proteins, sortase enzymes have been the focus of considerable interest for the development of novel anti-microbials, however, more recently their function as unique transpeptidases has been exploited for the synthesis of novel bio-conjugates. Yet, for synthetic purposes, SrtA-mediated conjugation suffers from the enzyme's inherently poor catalytic efficiency. Therefore, to identify SrtA variants with improved catalytic efficiency, we used directed evolution to select a catalytically enhanced SrtA enzyme. An analysis of improved SrtA variants in the context of sequence conservation, NMR and x-ray crystal structures, and kinetic data suggests a novel mechanism for catalysis involving large conformational changes that delivers substrate to the active site pocket. Indeed, using DEER-EPR spectroscopy, we reveal that upon substrate binding, SrtA undergoes a large scissors-like conformational change that simultaneously translates the sort-tag substrate to the active site in addition to repositioning key catalytic residues for esterification. A better understanding of Sortase dynamics will significantly enhance future engineering and drug discovery efforts.https://journals.plos.org/plosone/article/file?id=10.1371/journal.pone.0184271&type=printable
spellingShingle Muna Suliman
Vishaka Santosh
Tom C M Seegar
Annamarie C Dalton
Kathryn M Schultz
Candice S Klug
William A Barton
Directed evolution provides insight into conformational substrate sampling by SrtA.
PLoS ONE
title Directed evolution provides insight into conformational substrate sampling by SrtA.
title_full Directed evolution provides insight into conformational substrate sampling by SrtA.
title_fullStr Directed evolution provides insight into conformational substrate sampling by SrtA.
title_full_unstemmed Directed evolution provides insight into conformational substrate sampling by SrtA.
title_short Directed evolution provides insight into conformational substrate sampling by SrtA.
title_sort directed evolution provides insight into conformational substrate sampling by srta
url https://journals.plos.org/plosone/article/file?id=10.1371/journal.pone.0184271&type=printable
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