Floating Bimetallic Catalysts for Growing 30 cm‐Long Carbon Nanotube Arrays with High Yields and Uniformity

Abstract Ultralong carbon nanotubes (CNTs) are considered as promising candidates for many cutting‐edge applications. However, restricted by the extremely low yields of ultralong CNTs, their practical applications can hardly be realized. Therefore, new methodologies shall be developed to boost the growth efficiency of ultralong CNTs and alleviate their areal density decay at the macroscale level. Herein, a facile, universal, and controllable method for the in situ synthesis of floating bimetallic catalysts (FBCs) is proposed to grow ultralong CNT arrays with high yields and uniformity. Ferrocene and metal acetylacetonates serve as catalyst precursors, affording the successful synthesis of a series of FBCs with controllable compositions. Among these FBCs, the optimized FeCu catalyst increases the areal density of ultralong CNT arrays to a record‐breaking value of ≈8100 CNTs mm −1 and exhibits a lifetime 3.40 times longer than that of Fe, thus achieving both high yields and uniformity. A 30‐centimeters‐long and high‐density ultralong CNT array is also successfully grown with the assistance of FeCu catalysts. As evidenced by this kinetic model and molecular dynamics simulations, the introduction of Cu into Fe can simultaneously improve the catalyst fluidity and decrease carbon solubility, and an optimal catalytic performance will be achieved by balancing this tradeoff.