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Dr. Chunwei Dong Dr. Ren-Wu Huang Dr. Arunachalam Sagadevan Dr. Peng Yuan Dr. Luis Gutiérrez-Arzaluz Dr. Atanu Ghosh Saidkhodzha Nematulloev Badriah Alamer Prof. Dr. Omar F. Mohammed Prof. Dr. Irshad Hussain Prof. Dr. Magnus Rueping Prof. Dr. Osman M. Bakr 《Angewandte Chemie (International ed. in English)》2023,62(37):e202307140
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. 相似文献
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Saidkhodzha Nematulloev Dr. Arunachalam Sagadevan Badriah Alamer Dr. Aleksander Shkurenko Dr. Renwu Huang Dr. Jun Yin Dr. Chunwei Dong Dr. Peng Yuan Dr. Khursand E. Yorov Azimet A. Karluk Dr. Wasim J. Mir Bashir E. Hasanov Dr. Mohamed Nejib Hedhili Dr. Naveen M. Halappa Prof. Dr. Mohamed Eddaoudi Prof. Dr. Omar F. Mohammed Prof. Dr. Magnus Rueping Prof. Dr. Osman M. Bakr 《Angewandte Chemie (International ed. in English)》2023,62(26):e202303572
Point defects in nanoparticles have long been hypothesized to play an important role in governing the particle's electronic structure and physicochemical properties. However, single point defects in material systems usually exist with other heterogeneities, obscuring the chemical role of the effects. Herein, we report the synthesis of novel atomically precise, copper hydride nanoclusters (NCs), [Cu28H10(C7H7S)18(TPP)3] ( Cu28 ; TPP: triphenylphosphine; C7H7S: o-thiocresol) with a defined defect in the gram scale via a one-pot reduction method. The Cu28 acts as a highly selective catalyst for C−C cross-couplings. The work highlights the potential of defective NCs as model systems for investigating individual defects, correlating defects with physiochemical properties, and rationally designing new nanoparticle catalysts. 相似文献
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