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Descifrando el mecanismo de tiolactonización en la biosíntesis de la tiolactomicina

Jiawei Guo1,2, Qiaoyu Zhang3, Yang Shen4

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Los investigadores descubrieron cómo se hace la tiolactomicina, un antibiótico dirigido a la síntesis de ácidos grasos bacterianos. La sintetasa peptídica no ribosómica TlnC y la enzima citocromo P450 TlnA trabajan juntas para formar su estructura de anillo única.

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Área de la Ciencia:

  • La bioquímica
  • Enzimología
  • Biosíntesis de productos naturales

Sus antecedentes:

  • La tiolactomicina (1) es un antibiótico prometedor dirigido a la sintasa de ácidos grasos de tipo II bacteriana.
  • La biosíntesis de su anillo único de gamma-tiolactona permanece en gran medida sin aclarar.
  • Comprender esta vía es crucial para el desarrollo de antibióticos y la ingeniería enzimática.

Objetivo del estudio:

  • Elucidar los mecanismos enzimáticos responsables de la biosíntesis del anillo gamma-tiolactona en la tiolactomicina.
  • Identificar las enzimas específicas y sus funciones en la formación de este producto natural único.

Principales métodos:

  • Ensayos bioquímicos en los que se utilizan dominios enzimáticos purificados.
  • Cinética de las enzimas y análisis de los intermedios de reacción.
  • Mutagénesis dirigida al sitio y experimentos de reconstitución in vitro.

Principales resultados:

  • El dominio de condensación y heterociclado (Cy) de la péptido sintetasa no ribosómica TlnC (TlnC_Cy) media una nueva reacción de transferencia de azufre.
  • TlnC_Cy genera un intermediario tiocarboxilato a partir de un precursor de policetido.
  • La enzima del citocromo P450 TlnA actúa como una gamma-tiolactona sintasa, catalizando la ciclización a través de un mecanismo radical.

Conclusiones:

  • Los NRPS TlnC_Cy y P450 TlnA cooperan para ensamblar el anillo gamma-tiolactona de la tiolactomicina.
  • Este estudio revela una estrategia enzimática única para la biosíntesis de gamma-tiolactona.
  • Los hallazgos amplían las capacidades catalíticas conocidas de los dominios NRPS Cy y las enzimas P450.