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La edición del carboxilo terminal impulsa la divergencia en la biosíntesis de la fasamicina y la antrabensoxocinona
Kai Jiang1,2, Cheng Zhu1, Yan Gao1,2
1State Key Laboratory of Microbial Metabolism and School of Life Sciences and Biotechnology, Shanghai Jiao Tong University, Shanghai 200240, China.
Journal of the American Chemical Society
|July 21, 2025
Resumen
Este estudio revela dos vías distintas para modificar los policetidos aromáticos, la fasamicina (FAS) y la antrabensoxocinona (ABX), a partir de un precursor compartido. Se revelan nuevos mecanismos de edición de grupos carboxilo esenciales para generar diversidad de productos naturales.
Área de la Ciencia:
- La bioquímica
- Productos naturales Química
- Biología estructural
Sus antecedentes:
- Las policetidas aromáticas son diversos productos naturales con actividades biológicas significativas.
- Las variaciones estructurales en estos compuestos surgen de modificaciones en sus marcos centrales.
- Comprender estas modificaciones es clave para desbloquear sus aplicaciones potenciales.
Objetivo del estudio:
- Elucidar las distintas vías de biosíntesis de la (+) / ((-) -antrabenzoxocinona (ABX) y la fasamicina (FAS).
- Identificar los mecanismos moleculares detrás de la protección del grupo carboxilo y la descarboxilación en la biosíntesis de policetidos.
- Para explorar las conexiones evolutivas de las enzimas clave a las familias de proteínas conocidas.
Principales métodos:
- Se utilizó la cristalografía de rayos X para determinar las estructuras de AccS y Abx(+) O.
- Se realizaron estudios de mutagénesis dirigidos al sitio para identificar residuos de enzimas clave.
- Se realizó un análisis comparativo con la familia de proteínas WhiE-ORFI.
Principales resultados:
- Se identificaron dos vías distintas: protección del grupo carboxilo por FasS para la biosíntesis de FAS y descarboxilación por Abx(+) O/Abx(-) O para la biosíntesis de ABX.
- Los principales residuos implicados en la protección del carboxilo y la descarboxilación se identificaron mediante estudios estructurales y de mutagénesis.
- AccS y AbxO estaban vinculados a los terminales N y C de la familia de proteínas WhiE-ORFI.
Conclusiones:
- Este estudio revela nuevas estrategias para la edición del grupo carboxilo terminal en la biosíntesis de productos naturales.
- Los hallazgos proporcionan información sobre la generación de diversidad estructural de policetidos aromáticos.
- Los mecanismos identificados ofrecen objetivos potenciales para la biología sintética y el descubrimiento de fármacos.
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