Robust unsymmetric pincer-type Ru(II) catalyst containing proton-responsive hydroxypyridyl fragment for β-alkylation of secondary alcohols with primary alcohols

Zhang, Lizhu; Shi, Jing; Wang, Xinyi; Xie, Yulian; Li, Zhengyi; Zhai, Qiushi; Yang, Ke; Wang, Xin; X, Sun

doi:10.1016/j.molstruc.2023.135311

Cited by 3 publications

(1 citation statement)

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“…The utilization of alcohols as alkylating agents has gained significant research attention due to their environmentally friendly nature and high atom efficiency. This is because they generate only water as a byproduct. − Numerous expensive precious metal catalysts (e.g., Pt, Ru, and Pd) were employed in this reaction. ,− However, their high cost hinders their extensive application. Consequently, the development of highly efficient nonprecious metals (e.g., Co, Ni, and Fe)-based catalysts for this reaction has emerged as the most urgent priority at present.…”

Section: Introductionmentioning

confidence: 99%

Mechanistic Insights into a Co(II)-Coordinated “Free” Metal Site of 2D Zinc-Based MOFs for β-Alkylation of Secondary Alcohols with Primary Alcohols

Li,

Fu,

Shi

et al. 2023

Inorg. Chem.

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Through in-depth study of the properties and reaction mechanisms of catalysts, it is possible to better optimize catalytic systems and improve reaction efficiency and selectivity. This remains one of the challenges in the field of catalysis. Therefore, the research and design of catalysts play crucial roles in understanding and optimizing catalytic reaction mechanisms. A robust 2D zinc-based MOFs (Zn-HA) supported Co(II) ion catalyst (Zn-HA@Co) has been designed and synthesized via a coordination-assisted strategy for β-alkylation of secondary alcohols with primary alcohols. The characterization demonstrated that the anchoring of Co(II) on Zn-HA via coordination could efficiently enhance the Co(II) ion dispersity and interaction between Co(II) and Zn-HA MOFs. Importantly, the density functional theory results have provided mechanistic insights into the energy of the HOMO and LUMO of the Zn-HA@Co catalyst as well as the energy change of the entire process after interacting with the reactants and the specific energy changes of each orbital. The synthesized Zn-HA@Co MOFs effectively lower the energy barrier of the catalytic reaction process. We expect that our research and design of catalysts will serve as valuable guideline for understanding and optimizing catalytic reaction mechanisms.

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