Molecular engineered palladium single atom catalysts with an M-C1N3 subunit for Suzuki coupling. Issue 18 (4th May 2021)

• Record Type: Journal Article
• Authors: Liu, Jia; Chen, Zhongxin; Liu, Cuibo; Zhang, Bao; Du, Yonghua; Liu, Chen-Fei; Ma, Lu; Xi, Shibo; Li, Runlai; Zhao, Xiaoxu; Song, Jingting; Sui, Xin Zhi; Yu, Wei; Miao, Ling; Jiang, Jianjun; Koh, Ming Joo; Loh, Kian Ping
• Is Part Of: Journal of materials chemistry. Volume 9:Issue 18(2021)
• Page Start: 11427
• Page End: 11432
• Publication Date: 2021-05-04
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d1ta00012h
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : Efficient Suzuki cross-coupling is promoted by ultrathin palladium single atom catalyst with molecularly precise Pd-N3 C1 subunit, which is attributed to a facilitated oxidative addition on electron-rich Pd centers than conventional Pd-N4 coordination. Abstract : Single atom catalysis has emerged as a powerful technique for catalysis due to its outstanding performance and atom economy. Controlling the hybridization of the atom with its environment is crucial in determining the selectivity and/or yield of the reaction. However, the single atom environment is usually ill-defined and hard to predict because the pyrolysis process used in preparing SACs damages the original status of the precursors in the catalyst preparation. A molecular engineering approach to synthesize single atom catalysts (SACs) on a heterogeneous template provides a strategy to make SACs with a highly uniform coordinating environment. Herein, we report the preparation of a molecular engineered Pd single atom catalyst with a pre-defined M-N3 C1 coordination (Pd-N3 C1 -SAC) using a structure-rigid Pd-N3 C1 porphyrin as the precursor, which shows more efficient Suzuki coupling compared with the SAC with Pd-N4 coordination. The origin of the high activity of the Pd-N3 C1 -SAC is revealed through density functional theory calculations, where a lower reaction barrier for the rate-determining oxidative addition is identified.