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Dominación de los dicalcogenuros: aislamiento, caracterización y reactividad de los aniones perselenuro, persulfuro,

Keyan Li¹, Lev N Zakharov¹, Michael D Pluth¹

¹Department of Chemistry and Biochemistry, Materials Science Institute, Knight Campus for Accelerating Scientific Impact, and Institute of Molecular Biology, University of Oregon, Eugene, Oregon 97403-1253, United States.

Journal of the American Chemical Society

|June 9, 2023

Resumen

Los investigadores sintetizaron y caracterizaron nuevos aniones de persulfuro, perselenuro, tioselenuro y selenosulfuro. Estos aniones dicalcogénidos estables ofrecen nuevos conocimientos sobre las vías de señalización biológica que involucran especies reactivas de azufre y selenio.

Área de la Ciencia:

* Química inorgánica
* Química bioorgánica
* Química orgánica

Sus antecedentes:

* Las especies reactivas de azufre (RSS) y las especies reactivas de selenio (RSeS) son cruciales en la señalización biológica a través del sulfuro de hidrógeno (H2S) y el selenuro de hidrógeno (H2Se).
* Los aniones diclorenuro se proponen como intermedios transitorios en varias transformaciones bioquímicas.

Objetivo del estudio:

* Para lograr la síntesis selectiva, el aislamiento y la caracterización de los aniones de persulfuro, perselenuro, tioselenuro y selenosulfuro.
* Investigar la reactividad fundamental de estas nuevas especies de dicalcogenuros.
* Aclarar sus características estructurales y de reactividad relevantes para los sistemas biológicos.

Principales métodos:

* Síntesis de aniones dicalcogénidos mediante la reducción del azufre elemental (S8) o del selenio (Se) utilizando tiolato de bencilo de potasio o selenolato.
* Confirmación estructural mediante cristalografía de rayos X.
* Caracterización espectroscópica, incluida la espectroscopia de RMN en estado de solución 1H, 13C y 77Se.

Principales resultados:

* Síntesis y aislamiento exitosos de aniones estables de persulfuro ([BnSS]-), perselenuro ([BnSeSe]-), tioselenuro ([BnSSe]-), y selenosulfuro ([BnSeS]-).
* La cristalografía de rayos X y la espectroscopia de RMN confirmaron las estructuras químicas de los dicalcogenidos aislados.
* Reactividad demostrada incluyendo reducción a EPPh3 o HE-/H2E y reacción con cianuro para formar ECN-.

Conclusiones:

* El estudio proporciona aniones dicalcogénidos estables y accesibles estéricamente análogos a la cisteína.
Se obtuvieron nuevos conocimientos sobre las propiedades estructurales y de reactividad de estos aniones.
* Los hallazgos avanzan en la comprensión de las funciones de los dicalcogenuros en los procesos biológicos, incluida la posible participación en vías de desintoxicación como la enzima rodanesa.

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