Enhancing Interface Connectivity for Multifunctional Magnetic Carbon Aerogels: An In Situ Growth Strategy of Metal-Organic Frameworks on Cellulose Nanofibrils

Improving interface connectivity of magnetic nanoparticles in carbon aerogels is crucial, yet challenging for assembling lightweight, elastic, high-performance, and multifunctional carbon architectures. Here, an in situ growth strategy to achieve high dispersion of metal-organic frameworks (MOFs)-anchored cellulose nanofibrils to enhance the interface connection quality is proposed. Followed by a facile freeze-casting and carbonization treatment, sustainable biomimetic porous carbon aerogels with highly dispersed and closely connected MOF-derived magnetic nano-capsules are fabricated. Thanks to the tight interface bonding of nano-capsule microstructure, these aerogels showcase remarkable mechanical robustness and flexibility, tunable electrical conductivity and magnetization intensity, and excellent electromagnetic wave absorption performance. Achieving a reflection loss of -70.8 dB and a broadened effective absorption bandwidth of 6.0 GHz at a filling fraction of merely 2.2 wt.%, leading to a specific reflection loss of -1450 dB mm-1, surpassing all carbon-based aerogel absorbers so far reported. Meanwhile, the aerogel manifests high magnetic sensing sensibility and excellent thermal insulation. This work provides an extendable in situ growth strategy for synthesizing MOF-modified cellulose nanofibril structures, thereby promoting the development of high-value-added multifunctional magnetic carbon aerogels for applications in electromagnetic compatibility and protection, thermal management, diversified sensing, Internet of Things devices, and aerospace. A strategy for in situ growing MOFs on cellulose nanofibrils is proposed to promote interface connectivity. Strong anchoring of MOFs produces a unique structure of nano-capsules tightly embedded in carbon skeletons. The product CoFe/carbon aerogels exhibit exceptional specific reflection loss of -1450 dB mm-1, surpassing all reported carbon aerogels, and demonstrate application potential in thermal management and magnetic sensing. image