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Catálisis de boro en una enzima diseñadora

Lars Longwitz1, Reuben B Leveson-Gower1, Henriëtte J Rozeboom2

  • 1Stratingh Institute for Chemistry, University of Groningen, Groningen, The Netherlands.

Nature
|May 8, 2024
PubMed
Resumen

Los científicos crearon una nueva enzima diseñadora utilizando la expansión del código genético. Esta enzima incorpora una fracción de ácido borónico, permitiendo nuevas reacciones químicas y logrando una alta enantioselectividad para varios sustratos.

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Área de la Ciencia:

  • La bioquímica
  • Biología sintética
  • Química orgánica

Sus antecedentes:

  • Las enzimas son cruciales para la producción química sostenible, pero tienen mecanismos de reacción limitados.
  • La expansión de las capacidades enzimáticas requiere la incorporación de funcionalidades no biológicas.
  • El biocatálisis actual está limitado por la estrecha gama de reacciones enzimáticas naturales.

Objetivo del estudio:

  • Para crear una enzima genéticamente codificada con una actividad organocatalítica no natural.
  • Desarrollar una enzima diseñadora capaz de reacciones más allá del alcance de la naturaleza.
  • Demostrar el potencial de la expansión del código genético para el biocatálisis programable.

Principales métodos:

  • Expansión del código genético para incorporar un ácido borónico en una proteína.
  • Evolución dirigida para mejorar la actividad enzimática y la selectividad.
  • Cristalografía de rayos X, HRMS y espectroscopia de RMN 11B para el análisis estructural y mecanicista.

Principales resultados:

  • Se sintetizó y codificó genéticamente con éxito una nueva enzima que contiene ácido bórico.
  • La enzima catalizó la resolución cinética de las hidroxicetonas a través de la formación de oximas.
  • La evolución dirigida produjo una variante con enantioselectividades similares a las enzimas naturales.
  • El modo de activación único de la enzima fue confirmado estructuralmente y espectroscópicamente.

Conclusiones:

  • La expansión del código genético permite la creación de enzimas diseñadoras con grupos catalíticos xenobióticos.
  • Las enzimas que contienen boro pueden acceder a nuevos mecanismos de reacción no alcanzables por las enzimas naturales.
  • Este enfoque abre nuevas vías para el biocatálisis enantioselectivo y el diseño de enzimas programables.