Hinge-shift mechanism as a protein design principle for the evolution of β-lactamases from substrate promiscuity to specificity

TEM-1 β-lactamase degrades β-lactam antibiotics with a strong preference for penicillins. Sequence reconstruction studies indicate that it evolved from ancestral enzymes that degraded a variety of β-lactam antibiotics with moderate efficiency. This generalist to specialist conversion involved more t...

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Detalhes bibliográficos
Autores: Modi, Tushar, Risso, Valeria A., Martínez-Rodríguez, Sergio, Gavira Gallardo, J. A., Mebrat, Mubark D., Van Horn, Wade D., Sanchez-Ruiz, Jose M., Banu Ozkan, S.
Tipo de documento: artigo
Estado:Versão publicada
Data de publicação:2021
País:España
Recursos:Consejo Superior de Investigaciones Científicas (CSIC)
Repositório:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/265220
Acesso em linha:http://hdl.handle.net/10261/265220
Access Level:Acceso aberto
Palavra-chave:Amino Acid Sequence
Beta-Lactamases
Catalytic Domain
Computational Biology
Escherichia coli
Evolution, Molecular
Molecular Dynamics Simulation
Penicillins
Protein Conformation
Substrate Specificity
Descrição
Resumo:TEM-1 β-lactamase degrades β-lactam antibiotics with a strong preference for penicillins. Sequence reconstruction studies indicate that it evolved from ancestral enzymes that degraded a variety of β-lactam antibiotics with moderate efficiency. This generalist to specialist conversion involved more than 100 mutational changes, but conserved fold and catalytic residues, suggesting a role for dynamics in enzyme evolution. Here, we develop a conformational dynamics computational approach to rationally mold a protein flexibility profile on the basis of a hinge-shift mechanism. By deliberately weighting and altering the conformational dynamics of a putative Precambrian β-lactamase, we engineer enzyme specificity that mimics the modern TEM-1 β-lactamase with only 21 amino acid replacements. Our conformational dynamics design thus re-enacts the evolutionary process and provides a rational allosteric approach for manipulating function while conserving the enzyme active site.