CoNi/MXene@CoNi/MXene microsphere/silicone rubber multilayered composites for ultra-broadband microwave absorption

2D transition metal carbide/nitride (MXene) nanomaterials have prospective applications in high-performance microwave absorption (MA). However, the excessively high permittivity, absence of magnetic loss, and susceptible oxidizability of MXene severely hinder the enhancement of its MA properties. Here, we used a facile organic solution–phase thermal decomposition method to prepare dielectric–magnetic MXene@CoNi nanocomposites with heterojunctions, which can effectively prevent the oxidation of MXene. Subsequently, the MXene@CoNi nanocomposites were integrated with magnetic CoNi alloys, MXene microspheres (MXene MPs), and a silicon rubber (SR) matrix to construct multilayered CoNi/MXene@CoNi/MXene MPs/SR composites by casting and curing. Benefiting from the multilayered structure and complementary effects of the dielectric and magnetic components, the multilayered CoNi/MXene@CoNi/MXene MPs/SR composites composed of matching, absorbing, and reflective layers showed a remarkable minimum reflection loss of −53.3 dB and an ultra-broad effective absorption bandwidth up to 11.12 GHz at a thickness of 2.96 mm. These results demonstrated the developed multilayered composites are promising candidates for high-performance MA. Our study provides new insights into the development of ultra-broadband MXene-based absorbent materials.