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Generación combinatoria de la complejidad por enzimas redox en la biosíntesis de la cetoglobosina A
Kan'ichiro Ishiuchi1, Takehito Nakazawa, Fumitoshi Yagishita
1Department of Pharmaceutical Sciences, University of Shizuoka, Shizuoka 422-8526, Japan.
Journal of the American Chemical Society
|April 25, 2013
Resumen
Este estudio detalla la biosíntesis completa de la chaetoglobosina A, identificando las principales enzimas redox e intermedios. La comprensión de estas vías en Chaetomium globosum ayuda al descubrimiento de productos naturales.
Área de la Ciencia:
- La bioquímica es la bioquímica.
- Biosíntesis de Productos Naturales de Productos Naturales
- Enzimología Enzimología.
Sus antecedentes:
- Las enzimas redox son cruciales para generar complejidad estructural en productos naturales.
- La chaetoglobosina A es un producto natural complejo biosintetizado por una vía híbrida.
- La familia de la chaetoglobosina incluye análogos con diferentes estados de oxidación.
Objetivo del estudio:
- Para dilucidar la vía biosintética completa de la cetoglobosina A de la proximetoglobosina I. Para el estudio de la
- Para identificar las enzimas redox específicas responsables de cada paso de oxidación.
- Para determinar el curso estereoquímico y los intermediarios de la biosíntesis de la chaetoglobosina A.
Principales métodos:
- Se utilizaron cepas de Chaetomium globosum con deleciones en genes de enzimas redox (monooxigenasa dependiente de FAD, citocromo P450s).
- Realizó experimentos de biotransformación in vivo por expresión heteróloga de genes en Saccharomyces cerevisiae.
- Determinó las configuraciones absolutas de cinco intermedios identificados utilizando análisis de la estructura cristalina de rayos X.
Principales resultados:
- Se identificaron cinco nuevos análogos como productos intermedios en la oxidación de la proximaetoglobosina I a la chaetoglobosina A.
- Elucidado la secuencia completa de pasos de oxidación y las enzimas que los catalizan.
- Reveló la promiscuidad de las enzimas redox, lo que lleva a una red de vías y la formación combinatoria de intermedios.
Conclusiones:
- El estudio mapeó con éxito la vía biosintética completa de la chaetoglobosina A.
- Demostró las funciones críticas de las enzimas redox específicas y su promiscuidad en la generación de diversidad estructural.
- El enfoque presentado puede acelerar la aclaración de las vías de biosíntesis para otros productos naturales de hongos.
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