Inspired by the densely covered capillary structure inside a dog's nose, we report an artificial nanostructure, i. e., poly(sodium p-styrenesulfonate)-functionalized reduced graphene oxide nanoscrolls (PGNS), with high structural perfection and efficient gas sensing applications. A facile supramolecular assembly is introduced to functionalize graphene with the functional polymer, combined with the lyophilization technique to massively transform the planar graphene-based nanosheets to nanoscrolls. Detailed characterizations reveal that the bioinspired nanoscrolls exhibit a wide-open tubular morphology with uniform dimensions that is structurally distinct from the previously reported ones. The detailed morphologies of the graphene-based nanosheets in each scrolling stage during lyophilization are monitored by cryo-SEM. This unravels an asymmetric polymer-induced graphene scrolling mechanism including the corresponding scrolling process, which is directly presented by molecular dynamics simulations. The fabricated PGNS sensors exhibit superior gas sensing performance with reliable repeatability, excellent linear sensibility, and, especially, an ultrahigh response ( R/ R = 5.39, 10 ppm) toward NO. The supramolecular assembly combined with the lyophilization technique to fabricate PGNS provides a strategy to design biomimetic materials for gas sensors and chemical trace detectors.

Because of the combined advantages of both porous materials and two-dimensional (2D) graphene sheets, superior mechanical properties of three-dimensional (3D) graphene foams have received much attention from material scientists and energy engineers. Here, a 2D mesoscopic graphene model (Modell. Simul. Mater. Sci. Eng. 2011, 19, 054003), was expanded into a 3D bonded graphene foam system by utilizing physical cross-links and van der Waals forces acting among different mesoscopic graphene flakes by considering the debonding behavior, to evaluate the uniaxial tension behavior and fracture mode based on in situ SEM tensile testing (Carbon 2015, 85, 299). We reasonably reproduced a multipeak stress-strain relationship including its obvious yielding plateau and a ductile fracture mode near 45° plane from the tensile direction including the corresponding fracture morphology. Then, a power scaling law of tensile elastic modulus with mass density and an anisotropic strain-dependent Poisson's ratio were both deduced. The mesoscopic physical mechanism of tensile deformation was clearly revealed through the local stress state and evolution of mesostructure. The fracture feature of bonded graphene foam and its thermodynamic state were directly navigated to the tearing pattern of mesoscopic graphene flakes. This study provides an effective way to understand the mesoscopic physical nature of 3D graphene foams, and hence it may contribute to the multiscale computations of micro/meso/macromechanical performances and optimal design of advanced graphene-foam-based materials.