MOE Laboratory of Bioinorganic and Synthetic Chemistry, Lehn Institute of Functional Materials, School of Chemistry , Sun Yat-Sen University , Guangzhou 510275 , China.
State Key Laboratory of Applied Organic Chemistry , Lanzhou University , Lanzhou 730000 , China.
J Am Chem Soc. 2019 Feb 13;141(6):2589-2593. doi: 10.1021/jacs.8b12372. Epub 2019 Jan 30.
We demonstrate herein a facile strategy to engineer versatile catalytically active coordination interspace in the same primitive metal-organic framework (MOF) for variable heterogeneous catalysis. Different functional ligands can be reversibly inserted into and removed from proto-LIFM-28 individually or successively to bring in single or binary catalytic sites for specific reactions and switch the parent MOF to multipurpose catalysts. Alcohol-oxidation, Knoevenagel-condensation, click, acetal, and Baylis-Hillman reactions are achievable through simple exchange of a single catalytic spacer, while sequential or stepwise reactions are designable via selective combination of two catalytic spacers with different functionalities, thus making proto-LIFM-28 a multivariate MOF for multiuse and economic catalysis.
我们在此展示了一种简便的策略,即在同一原始金属-有机骨架(MOF)中构建多功能催化活性配位空间,用于可变的多相催化。不同功能的配体可以单独或连续地可逆地插入和去除原始 LIFM-28 中,从而引入单或双催化位,用于特定反应,并将母体 MOF 转换为多用途催化剂。通过简单交换单个催化间隔物,可以实现醇氧化、Knoevenagel 缩合、点击、缩醛和 Baylis-Hillman 反应,而通过选择性组合具有不同功能的两个催化间隔物,可以设计顺序或逐步反应,从而使原始 LIFM-28 成为用于多功能和经济催化的多元 MOF。