Solution‐Processable Metal‐Organic Framework Featuring Highly Tunable Dynamic Aggregation States

Abstract The limited processability of metal‐organic frameworks (MOFs) is hindered flexibility in the manipulation of their aggregation state and applications. Therefore, achieving highly processable MOFs is of great significance but a challenging goal. Herein, a facile strategy is presented for achieving the construction of solution‐processable Mg‐based MOF, NKU‐Mg‐1 , allowing for dynamic control of the aggregation state through dynamic self‐assembly (DySA) process and reversible circularly polarized luminescence (CPL) switcher modulation. Notably, micron‐sized crystals of NKU‐Mg‐1 can be readily dispersed in water to form nano‐sized colloids, triggered by the dynamic COO‐Mg coordination bonding interruption by the competitive H 2 O‐Mg bonding. Accordingly, the aggregation state of the colloid MOF can be readily tuned from 50–80 nm up to 1000 nm, in turn enabling control of aggregation‐dependent emission. Specially, the solid‐phase aggregation can be controlled via structural transitions between 3D NKU‐Mg‐1‐rec‐1 and 2D NKU‐Mg‐1‐rec‐2 nano‐crystals, as confirmed by 3D electron diffraction. Furthermore, benefiting from its highly dynamic tunable aggregation nature, the rational incorporation of the chiral module confers significant CPL activity (g lum up to 0.01). Importantly, controllable dynamic aggregation enables reversible switching of the CPL activity by precisely regulating the aggregation states. The solution‐processable and dynamic aggregation‐tunable features endow it highly promising for applications.