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Triple, Mutually Orthogonal Bioorthogonal Pairs through the Design of Electronically Activated Sulfamate-Containing Cycloalkynes.
Hu, Yun; Roberts, Jessica M; Kilgore, Henry R; Mat Lani, Amirah S; Raines, Ronald T; Schomaker, Jennifer M.
Afiliación
  • Hu Y; Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Roberts JM; Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Kilgore HR; Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
  • Mat Lani AS; Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
  • Raines RT; Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
  • Schomaker JM; Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States.
J Am Chem Soc ; 142(44): 18826-18835, 2020 11 04.
Article en En | MEDLINE | ID: mdl-33085477
Interest in mutually exclusive pairs of bioorthogonal labeling reagents continues to drive the design of new compounds that are capable of fast and predictable reactions. The ability to easily modify S-, N-, and O-containing cyclooctynes (SNO-OCTs) enables electronic tuning of various SNO-OCTs to influence their cycloaddition rates with Type I-III dipoles. As opposed to optimizations based on just one specific dipole class, the electrophilicity of the alkynes in SNO-OCTs can be manipulated to achieve divergent reactivities and furnish mutually orthogonal dual ligation systems. Significant reaction rate enhancements of a difluorinated SNO-OCT derivative, as compared to the parent scaffold, were noted, with the second-order rate constant in cycloadditions with diazoacetamides exceeding 5.13 M-1 s-1. Computational and experimental studies were employed to inform the design of triple ligation systems that encompass three orthogonal reactivities. Finally, polar SNO-OCTs are rapidly internalized by mammalian cells and remain functional in the cytosol for live-cell labeling, highlighting their potential for diverse in vitro and in vivo applications.
Asunto(s)

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Ácidos Sulfónicos / Cicloparafinas Límite: Animals Idioma: En Revista: J Am Chem Soc Año: 2020 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Ácidos Sulfónicos / Cicloparafinas Límite: Animals Idioma: En Revista: J Am Chem Soc Año: 2020 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos