Ultraflexible Ultrathin 3D/1D Hierarchical Interpenetrating Ni-MOF/CNT Buckypaper Composites: Microstructures and Microwave Absorption Properties

Metal–organic frameworks (MOFs) have attracted attention due to their designable structures. However, recently reported MOF microwave-absorbing materials (MAMs) are dominated by powders. It remains a challenge to design MOF/carbon nanotube (CNT) composite structures that combine the mechanical properties of self-supporting flexibility with excellent microwave absorption. This work involves the hydrothermal approach to grow Ni-MOF of different microstructures in situ on the CNT monofilament by adjusting the molar ratio of nickel ions to organic ligands. Subsequently, an ultraflexible self-supporting Ni-MOF/CNT buckypaper (BP) is obtained by directional gas pressure filtration technology. The BP porous skeleton and the Ni-MOF with a unique porous structure provide effective impedance matching. The CNTs contribute to the conduction loss, the cross-scale heterogeneous interface generated by Ni-MOF/CNT BP provides rich interfacial polarization loss, and the porous structure complicates the microwave propagation path. All factors work together to give Ni-MOF/CNT BP an excellent microwave absorption capacity. The minimum reflection losses of Ni-MOF/CNT BPs decorated with granular-, hollow porous prism-, and porous prism-shaped Ni-MOFs reach −50.8, −57.8, and −43.3 dB, respectively. The corresponding effective absorption bandwidths are 4.5, 6.3, and 4.8 GHz, respectively. Furthermore, BPs show remarkable flexibility as they can be wound hundreds of times around a glass rod with a diameter of 4 mm without structural damage. This work presents a new concept for creating ultraflexible self-supported MOF-based MAMs with hierarchical interpenetrating porous structures, with potential application advantages in the field of flexible electronics.