Hyperelasticity of three-dimensional carbon nanotube sponge controlled by the stiffness of covalent junctions

To expand the applications of carbon nanotubes (CNTs) at macroscale, a heteroatom doping technique has been employed to fabricate isotropic 3-D CNT architectures by inducing elbow-like covalent junctions into multiwalled CNTs. As the junctions modify the topology of each CNT by favoring the stable bends in CNTs, junction stiffness and the consequence of junction-related morphology changes in sponge's hyperelasticity remain largely elusive. In this study, two types of 3-D multiwalled CNT sponges were fabricated by inducing boron-doped or nitrogen-doped covalent junctions into CNTs. Hyperelastic properties of the sponges were experimentally quantified as the functions of CNT morphology. A novel microstructure informed continuum constitutive law was developed specifically for such isotropic CNT sponges with junctions. Analyzing the experimental data with the new theory demonstrated that, for the first time, the effective modulus of boron-doped junctions (∼100 GPa) is higher than that of nitrogen-doped junctions (∼20 GPa), and the junction stiffness is a key factor in regulating the hyperelastic compressive modulus of the material. Theoretical analysis further revealed that increased number of junctions and shorter segments on each individual CNT chain would result in stronger hyperelastic 3-D CNT networks. This study has established a fundamental knowledge base to provide guidance for the future design and fabrication of 3-D CNT macrostructures.