Yuan Shuai, Qin Jun-Sheng, Li Jialuo, Huang Lan, Feng Liang, Fang Yu, Lollar Christina, Pang Jiandong, Zhang Liangliang, Sun Di, Alsalme Ali, Cagin Tahir, Zhou Hong-Cai
Department of Chemistry, Texas A&M University, College Station, TX, 77843-3255, USA.
Department of Materials Science and Engineering, Texas A&M University, College Station, TX, 77843-3003, USA.
Nat Commun. 2018 Feb 23;9(1):808. doi: 10.1038/s41467-018-03102-5.
Crystal engineering of metal-organic frameworks (MOFs) has allowed the construction of complex structures at atomic precision, but has yet to reach the same level of sophistication as organic synthesis. The synthesis of complex MOFs with multiple organic and/or inorganic components is ultimately limited by the lack of control over framework assembly in one-pot reactions. Herein, we demonstrate that multi-component MOFs with unprecedented complexity can be constructed in a predictable and stepwise manner under simple kinetic guidance, which conceptually mimics the retrosynthetic approach utilized to construct complicated organic molecules. Four multi-component MOFs were synthesized by the subsequent incorporation of organic linkers and inorganic clusters into the cavity of a mesoporous MOF, each composed of up to three different metals and two different linkers. Furthermore, we demonstrated the utility of such a retrosynthetic design through the construction of a cooperative bimetallic catalytic system with two collaborative metal sites for three-component Strecker reactions.
金属有机框架（MOF）的晶体工程已能够以原子精度构建复杂结构，但尚未达到有机合成那样的精细程度。具有多种有机和/或无机成分的复杂MOF的合成最终受到一锅法反应中框架组装缺乏控制的限制。在此，我们证明了在简单的动力学指导下，可以以可预测的逐步方式构建具有前所未有的复杂性的多组分MOF，这在概念上模仿了用于构建复杂有机分子的逆合成方法。通过将有机连接体和无机簇随后引入介孔MOF的孔腔中，合成了四种多组分MOF，每种MOF最多由三种不同的金属和两种不同的连接体组成。此外，我们通过构建具有两个协同金属位点的双金属催化体系用于三组分斯特雷克反应，展示了这种逆合成设计的实用性。
