Theoretical study on the catalytic performance of AunPdn (n = 1-4, 10) clusters for the Buchwald-Hartwig reaction.

The C-N coupling reaction, namely the Buchwald-Hartwig coupling reaction, is a pivotal transformation in medicinal chemistry, and thus, the development of efficient catalysts for this process is of great importance. In this study, the catalytic performance of bimetallic AunPdn (n = 1-4, 10) clusters for the Buchwald-Hartwig coupling reaction has been investigated by density functional theory (DFT). Our results demonstrate that the catalytic activity of AunPdn (n = 1-4) clusters gradually increases as the cluster size increases. Hence, the catalytic mechanism of a larger Au10Pd10 cluster for the Buchwald-Hartwig (BH) reaction was further examined, and it was found that Au10Pd10 exhibits excellent catalytic performance for this C-N coupling reaction. The difference in the catalytic activity of these AunPdn (n = 1-4, 10) clusters for the BH reaction has been understood by analyzing their electronic structures and charge transfer. This work provides theoretical insights into the design of bimetallic cluster catalysts for C-N cross-coupling reactions and highlights the potential of such clusters as catalytic platforms with tunable performance for various organic coupling reactions.