Porous three-dimensional (3D) assemblies of nanocarbons with large surface areas and tunable physical properties are attractive for a wide range of applications, such as energy storage electrodes, pollution adsorption, and thermal insulators. However, the full utilization of these materials is impeded by two challenges: forming 3D robust porous network structures that retain the intrinsic properties of the nanocarbon and achieving high shape-tunability to create structures with desired shapes. To address these challenges, gelatins with zwitterionic and hydrogen-bonded helical structure were considered a bio-derived binder to modulate the structural integrity of carbon nanotube (CNT) network which consists of overlapping nanotubes held by weak van der Waals attraction. The resulting CNT/gelatin wet-gels have favorable rheological properties, enabling 3D printing into complex porous architectures. Moreover, the 3D-printed complex wet-gel structure was successfully transformed into elastic and hierarchical porous structures consisting of micro-, meso-, and macro-scale pores with large specific surface areas of ∼988 m² g⁻¹ and excellent mechanical stability without permanent deformation even at 85% compressive strain. The resulting high shape-tunability, high elasticity, and large surface area are attributed to the reinforcement of the existing nanotube cross-linking points strengthened by the gelatin-derived graphitic layer coating without deteriorating the intrinsic properties of CNTs.

具有大表面积和可调物理性质的纳米碳多孔三维 (3D) 组件在广泛的应用中具有吸引力，例如储能电极、污染吸附和热绝缘体。然而，这些材料的充分利用受到两个挑战的阻碍：形成保持纳米碳固有特性的 3D 坚固多孔网络结构，以及实现高形状可调性以创建具有所需形状的结构。为了应对这些挑战，具有两性离子和氢键螺旋结构的明胶被认为是一种生物衍生粘合剂，用于调节碳纳米管 (CNT) 网络的结构完整性，该网络由通过弱范德华引力保持的重叠纳米管组成。所得的 CNT/明胶湿凝胶具有良好的流变特性，使 3D 打印成为复杂的多孔结构。此外，3D 打印的复杂湿凝胶结构成功地转化为弹性和分层多孔结构，由具有~988 m 大比表面积的微观、中观和宏观孔隙组成。²  g ^-1和出色的机械稳定性，即使在 85% 的压缩应变下也不会永久变形。由此产生的高形状可调性、高弹性和大表面积归因于由明胶衍生的石墨层涂层增强的现有纳米管交联点的增强，而不会降低碳纳米管的固有特性。