PDF(Pubmed)
Abstract：
Combining the physical advantages of two-dimensional (2D) inorganic nanosheets and the modular design and programmed structure of metal-organic frameworks (MOFs), 2D MOFs remain at the forefront of functional material research. Despite tremendous efforts, precise control in the synthesis of 2D nonlayered MOFs with predesigned topology for desired applications remains challenging. Success in the bottom-up synthesis of 2D nonlayered MOFs via ligand exchange motivated us to incorporate partial BTC (BTC = 1,3,5-benzenetricarboxylate) ligand dissociation and CO2 capped coordination into the top-down treatment of bulk Cu-BTC MOF, leading to successful conversion of a 3D nonlayered network to a 2D Cu-based topological structure. Notably, a supercritical CO2-containing solvent mixture is employed to provide the desired defect and coordination engineering. Thus, our work introduces a new top-down concept based on modulated synthesis to fabricate high-quality 2D nonlayered MOFs for the first time.
摘要：
结合了二维（2D）无机纳米片的物理优势以及金属有机框架（MOFs）的模块化设计和编程结构，2DMOFs仍然处于功能材料研究的前沿。尽管付出了巨大的努力,在2D非分层MOFs的合成与所需应用的预先设计的拓扑的精确控制仍然具有挑战性。通过配体交换成功地自下而上地合成2D非层状MOF，促使我们将部分BTC（BTC=1,3,5-苯三羧酸酯）配体解离和CO2封端的配位纳入块状Cu-BTCMOF的自上而下处理中，导致3D非分层网络成功转换为2D基于Cu的拓扑结构。值得注意的是,使用超临界含CO2的溶剂混合物来提供所需的缺陷和协调工程。因此，我们的工作引入了一种基于调制合成的自上而下的新概念，以首次制造高质量的2D非分层MOFs。
