Rational design of model Pd(ii)-catalysts for C-H activation involving ligands with charge-shift bonding characteristics.
作者信息
Ma Dongxia, Zhang Congjie, Chen Zhe-Ning, Xu Xin
机构信息
Key Laboratory of Macromolecular Science of Shaanxi Province, School of Chemistry & Chemical Engineering, Shaanxi Normal University, Xi'an, 710062, China.
Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, MOE Laboratory for Computational Physical Science, Department of Chemistry, Fudan University, Shanghai, 200433, China.
出版信息
Phys Chem Chem Phys. 2017 Jan 18;19(3):2417-2424. doi: 10.1039/c6cp06215f.
In this work, five new palladium(ii) complexes have been designed as the model catalysts for methane to methyl trifluoroacetate conversion. All these compounds are analogues of the well-established (bis-NHC)PdBr complex (NHC, N-heterocyclic carbenes), derived by complexing the palladium(ii) metal ion with the derivatives of bis-2-borabicyclo[1.1.0]but-1(3)-ene (bis-2BB) ligands using the sp carbons. Our density functional theory calculation results suggest that the (bis-2BB)PdBr catalysts outperform the popular (bis-NHC)PdBr complex in the desired catalytic process, and further reveal that the charge-shift bonding in the bis-2BB ligands contributes to the improved catalytic performance. These findings may spark new ideas for experimental design of more efficient organometallic catalysts for C-H bond activation and functionalization.
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