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Acidic open-cage solution containing basic cage-confined nanospaces for multipurpose catalysis.
Li, Kang; Wu, Kai; Fan, Yan-Zhong; Guo, Jing; Lu, Yu-Lin; Wang, Yuan-Fan; Maurin, Guillaume; Su, Cheng-Yong.
Affiliation
  • Li K; MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
  • Wu K; MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
  • Fan YZ; MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
  • Guo J; MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
  • Lu YL; MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
  • Wang YF; MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
  • Maurin G; Institut Charles Gerhardt Montpellier, Centre National de la Recherche Scientifique, École Nationale Supérieure de Chimie de Montpellier, Université de Montpellier, Montpellier 34095, France.
  • Su CY; MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
Natl Sci Rev ; 9(5): nwab155, 2022 May.
Article de En | MEDLINE | ID: mdl-35663244
The nanoscale chemical spaces inherent in porous organic/coordination cages or solid/liquid materials have been continuously explored for their nanoconfinement effect on selective adsorption and reaction of small gas or organic molecules. Herein, we aim to rationalize the unconventional chemical reactivities motivated by the cage-confined nanospaces in aqueous solutions, where the robust yet permeable nanospaces defined by the open cages facilitate dynamic guest exchange and unusual chemical reactions. The high positive charges on [(Pd/Pt)6(RuL3)8]28+ nanocages drive imidazole-proton equilibrium to display a significantly perturbed pK a shift, creating cage-defined nanospaces in solution with distinct intrinsic basicity and extrinsic acidity. The supramolecular cage effect plays pivotal roles in elaborating robust solution nanospaces, controlling ingress-and-egress molecular processes through open-cage portals and endowing nanocages with transition-state stabilization, amphoteric reactivities and the phase transfer of insoluble molecules, thus promoting chemical transformations in unconventional ways. Consequently, a wide range of application of cage-confined catalysis with anomalous reactivities may be expected based on this kind of open-cage solution medium, which combines cage nanocavity, solution heterogeneity and liquid-phase fluidity to benefit various potential mass transfer and molecular process options.
Mots clés

Texte intégral: 1 Collection: 01-internacional Base de données: MEDLINE Langue: En Journal: Natl Sci Rev Année: 2022 Type de document: Article Pays d'affiliation: Chine Pays de publication: Chine

Texte intégral: 1 Collection: 01-internacional Base de données: MEDLINE Langue: En Journal: Natl Sci Rev Année: 2022 Type de document: Article Pays d'affiliation: Chine Pays de publication: Chine