One‐Pot Synthesis of Conductive Metal–Organic Framework@polypyrrole Hybrids with Enhanced Electromagnetic Wave Absorption Performance

Rational heterostructure design can bring interfacial polarization relaxation to significantly enhance the electromagnetic wave (EMW) absorption performance. However, intelligently building a homogeneous heterostructure with superior EMW absorption properties remains a great challenge. Herein, a typical conductive metal–organic framework Cu 3 (HHTP) 2 (hexahydroxytriphenylene, HHTP) is delicately packed onto a polypyrrole (PPy) conductive polymer surface via a one‐step in situ polymerization approach. Results show that Cu 3 (HHTP) 2 is well packed on the PPy surface to form an elegant Cu 3 (HHTP) 2 @PPy hybrids interfacial microstructure with a unique superiority regarding EMW absorption compared with single components of PPy and Cu 3 (HHTP) 2 . Interestingly, the interfacial microstructure of Cu 3 (HHTP) 2 @PPy hybrids can be tuned by adjusting the composition of the PPy and Cu 3 (HHTP) 2 , resulting in the improvement of impedance matching, conductive loss, and enhancement of interfacial polarization relaxation, endowing the optimization of the EM wave absorption properties of the Cu 3 (HHTP) 2 @PPy. The broad effective absorption bandwidth covers a range as broad as 6.68 GHz (11.00–17.68 GHz), which is higher than most reported metal‐organic frameworks (MOFs) and conductive polymer‐based EM absorbing materials. Herein, new insight for developing highly efficient EMW absorption materials through hybridized interfacial microstructure engineering is provided.