Supracluster Assembly of Archimedean Cages with 72 Hydrogen Bonds for the Aldol Addition Reaction

© 2023 Wiley-VCH GmbH..

Clusters that can be experimentally precisely characterized and theoretically accurately calculated are essential to understanding the relationship between material structure and function. Here, we propose the concept of "supraclusters", which aim to connect "supramolecules" and "suprananoparticles" as well as reveal the unique assembly behavior of "supraclusters" with nanoparticle size at the molecular level. The implementation of supraclusters is full of challenges due to the difficulty in satisfying the ordered connectivity of clusters due to their abundant and dispersed hydrogen bonding sites. By solvothermal synthesis under a high catechol (H2 CATs) content, we successfully isolated a series of triangular {Al6 M3 } cluster compounds possessing brucite-like structural features. Interestingly, eight {Al6 M3 } clusters form 72-fold strong hydrogen bonding truncatedhexahedron Archimedean {Al6 M3 }8 supracluster cage (abbreviated as H-tcu). Surprisingly, the solution stability of the H-tcu was further proved by electrospray ionization mass spectrometry (ESI-MS) characterization. Therefore, it is not difficult to explain the reason for assembly of H-tcu into edge-directed and vertex-directed isomers. These porous supraclusters can be obtained by scale-up synthesis and exhibit a noticeable catalysis effect towards the condensation of acetone and p-nitrobenzaldehyde. As an intermediate state of supramolecule and suprananoparticle, the supracluster assembly can enrich the cluster chemistry and bring new structural types.

Medienart:

E-Artikel

Erscheinungsjahr:

2023

Erschienen:

2023

Enthalten in:

Zur Gesamtaufnahme - volume:62

Enthalten in:

Angewandte Chemie (International ed. in English) - 62(2023), 49 vom: 04. Dez., Seite e202309971

Sprache:

Englisch

Beteiligte Personen:

Liu, Ya-Jie [VerfasserIn]
Su, Hai-Feng [VerfasserIn]
Sun, Yi-Fan [VerfasserIn]
Wang, San-Tai [VerfasserIn]
Zhang, Cheng-Yang [VerfasserIn]
Fang, Wei-Hui [VerfasserIn]
Zhang, Jian [VerfasserIn]

Links:

Volltext

Themen:

Catalysis
Cluster Science
Hierarchical Assembly
Journal Article
Supracluster
Zeolite

Anmerkungen:

Date Revised 27.11.2023

published: Print-Electronic

Citation Status PubMed-not-MEDLINE

doi:

10.1002/anie.202309971

funding:

Förderinstitution / Projekttitel:

PPN (Katalog-ID):

NLM363695648