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The establishment of covalent junctions between carbon nanotubes (CNTs) and the modification of their straight tubular morphology are two strategies needed to successfully synthesize nanotube-based three-dimensional (3D) frameworks exhibiting superior material properties. Engineering such 3D structures in scalable synthetic processes still remains a challenge. This work pioneers the bulk synthesis of 3D macroscale nanotube elastic solids directly via a boron-doping strategy during chemical vapour deposition, which influences the formation of atomic-scale “elbow” junctions and nanotube covalent interconnections. Detailed elemental analysis revealed that the “elbow” junctions are preferred sites for excess boron atoms, indicating the role of boron and curvature in the junction formation mechanism, in agreement with our first principle theoretical calculations. Exploiting this material’s ultra-light weight, super-hydrophobicity, high porosity, thermal stability, and mechanical flexibility, the strongly oleophilic sponge-like solids are demonstrated as unique reusable sorbent scaffolds able to efficiently remove oil from contaminated seawater even after repeated use.

We have developed a rational strategy for creating the 3D pillared vertically aligned carbon nanotube (VACNT)-graphene architectures by intercalated growth of VACNTs into thermally expanded highly ordered pyrolytic graphite (HOPG). By controlling the fabrication process, the length of the VACNT pillars can be tuned. In conjunction with the electrodeposition of nickel hydroxide to introduce the pseudocapacitance, these 3D pillared VACNT–graphene architectures with a controllable nanotube length were demonstrated to show a high specific capacitance and remarkable rate capability, and they significantly outperformed many electrode materials currently used in the state-of-the-art supercapacitors.

The creation of three-dimensionally engineered nanoporous architectures via covalently interconnected nanoscale building blocks remains one of the fundamental challenges in nanotechnology. Here we report the synthesis of ordered, stacked macroscopic three-dimensional (3D) solid scaffolds of graphene oxide (GO) fabricated via chemical cross-linking of two-dimensional GO building blocks. The resulting 3D GO network solids form highly porous interconnected structures, and the controlled reduction of these structures leads to formation of 3D conductive graphene scaffolds. These 3D architectures show promise for potential applications such as gas storage; CO2 gas adsorption measurements carried out under ambient conditions show high sorption capacity, demonstrating the possibility of creating new functional carbon solids starting with two-dimensional carbon layers.

Optoelectronic performance of metal nanowire networks are dominated by junction microstructure and network configuration. Although metal nanowire printings, such as silver nanowires (AgNWs) or AgNWs/semiconductor oxide bilayer, have great potential to replace traditional ITO, efficient and selective nanoscale integration of nanowires is still challenging owing to high cross nanowire junction resistance. Herein, pulsed laser irradiation under controlled conditions is used to generate local crystalline nanojoining of AgNWs without affecting other regions of the network, resulting in significantly improved optoelectronic performance. The method, laser-induced plasmonic welding (LPW), can be applied to roll-to-roll printed AgNWs percolating networks on PET substrate. First principle simulations and experimental characterizations reveal the mechanism of crystalline nanojoining originated from thermal activated isolated metal atom flow over nanowire junctions. Molecular dynamic simulation results show an angle-dependent recrystallization process during LPW. The excellent optoelectronic performance of AgNW/PET has achieved Rs ∼ 5 Ω/sq at high transparency (91% @λ = 550 nm).