Isostructural Nanocluster Manipulation Reveals Pivotal Role of One Surface Atom in Click Chemistry

Chunwei Dong, Ren Wu Huang, Arunachalam Sagadevan, Peng Yuan, Luis Gutiérrez-Arzaluz, Atanu Ghosh, Saidkhodzha Nematulloev, Badriah Alamer, Omar F. Mohammed, Irshad Hussain, Magnus Rueping*, Osman M. Bakr*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

Elucidating single-atom effects on the fundamental properties of nanoparticles is challenging because single-atom modifications are typically accompanied by appreciable changes to the overall particle's structure. Herein, we report the synthesis of a [Cu58H20PET36(PPh3)4]2+ (Cu58; PET: phenylethanethiolate; PPh3: triphenylphosphine) nanocluster—an atomically precise nanoparticle—that can be transformed into the surface-defective analog [Cu57H20PET36(PPh3)4]+ (Cu57). Both nanoclusters are virtually identical, with five concentric metal shells, save for one missing surface copper atom in Cu57. Remarkably, the loss of this single surface atom drastically alters the reactivity of the nanocluster. In contrast to Cu58, Cu57 shows promising activity for click chemistry, particularly photoinduced [3+2] azide-alkyne cycloaddition (AAC), which is attributed to the active catalytic site in Cu57 after the removal of one surface copper atom. Our study not only presents a unique system for uncovering the effect of a single-surface atom modification on nanoparticle properties but also showcases single-atom surface modification as a powerful means for designing nanoparticle catalysts.

Original languageEnglish (US)
Article numbere202307140
JournalAngewandte Chemie - International Edition
Volume62
Issue number37
DOIs
StatePublished - Sep 11 2023

Bibliographical note

Funding Information:
This work was supported by King Abdullah University of Science and Technology (KAUST).

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

Keywords

  • Catalysis
  • Click Chemistry
  • Copper
  • Nanocluster
  • Single-Atom Manipulation

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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