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A gold nanocluster Au17Cd2(PNP)2(SR)12 (PNP=2,6‐bis(diphenylphosphinomethyl)pyridine, SR=4‐MeOPhS) consisting of an icosahedral Au13 kernel, two Au2CdS6 staple motifs, and two PNP pincer ligands has been designed, synthesized and well characterized. This cadmium and PNP pincer ligand co‐modified gold nanocluster showed high catalytic efficiency in the KA2 reaction, featuring high TON, mild reaction conditions, broad substrate scope as well as catalyst recyclability. Comparison of the catalytic performance between Au17Cd2(PNP)2(SR)12 and the structurally similar single cadmium (or PNP) modified gold nanoclusters demonstrates that the co‐existence of the cadmium and PNP on the surface is crucial for the high catalytic activity of the gold nanocluster. This work would be enlightening for developing efficient catalysts for cascade reactions and discovering the catalytic potential of metal nanoclusters in organic transformations. [ABSTRACT FROM AUTHOR]

Tuning the nanoclusters' compositions and structures is critical for the performance improvement of nanoclusters. Herein, a well-known Au25( SCH2CH2Ph)18 (Au25 for short) nanocluster has been transformed to a rare cadmium doped gold nanocluster [ Au13Cd2( PPh3)6( SC2H4Ph)6( NO3)2] 2Cd( NO3)4 ( Au26Cd5 for short) by peeling and doping. Although Au25 exhibits no catalytic activity toward A3-coupling reaction under the investigated conditions, the novel cadmium doped gold nanocluster Au26Cd5 shows high catalytic activity, as well as good recyclability and substrate tolerance for the same reaction. The high catalytic activity is attributed to the cooperation between the exerted cadmium atoms and the neighbor gold atoms on the surface of Au13 icosahedron. This work has important implication for the tuning of nanoclusters' compositions and structures targeting the improvement of catalytic performance by some unusual but effective strategies. [ABSTRACT FROM AUTHOR]