Zhang Lili, Xu Ziwei, Feng Tian-Liang, He Maoshuai, Hansen Thomas Willum, Wagner Jakob Birkedal, Liu Chang, Cheng Hui-Ming
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang, 110016, China.
School of Materials Science and Engineering, Jiangsu University, Zhenjiang, 212013, China.
Adv Sci (Weinh). 2023 Dec;10(36):e2304905. doi: 10.1002/advs.202304905. Epub 2023 Oct 28.
The asymmetrical growth of a single-wall carbon nanotube (SWCNT) by introducing a change of a local atomic structure, is usually inevitable and supposed to have a profound effect on the chirality control and property tailor. However, the breaking of the symmetry during SWCNT growth remains unexplored and its origins at the atomic-scale are elusive. Here, environmental transmission electron microscopy is used to capture the process of breaking the symmetry of a growing SWCNT from a sub-2-nm platinum catalyst nanoparticle in real-time, demonstrating that topological defects formed on the side of a SWCNT can serve as a buffer for stress release and inherently break its axis-symmetrical growth. Atomic-level details reveal the importance of the tube-catalyst interface and how the atom rearrangement of the solid-state platinum catalyst around the interface influences the final tubular structure. The active sites responsible for trapping carbon dimers and providing enough driving force for carbon incorporation and asymmetric growth are shown to be low-coordination step edges, as confirmed by theoretical simulations.
通过引入局部原子结构的变化来实现单壁碳纳米管(SWCNT)的不对称生长通常是不可避免的,并且被认为会对手性控制和性能定制产生深远影响。然而,SWCNT生长过程中的对称性破坏仍未得到探索,其在原子尺度上的起源也难以捉摸。在这里,环境透射电子显微镜被用于实时捕捉从亚2纳米铂催化剂纳米颗粒生长的SWCNT对称性破坏的过程,表明在SWCNT侧面形成的拓扑缺陷可以作为应力释放的缓冲,并固有地打破其轴对称生长。原子级细节揭示了管-催化剂界面的重要性,以及界面周围固态铂催化剂的原子重排如何影响最终的管状结构。理论模拟证实,负责捕获碳二聚体并为碳掺入和不对称生长提供足够驱动力的活性位点是低配位台阶边缘。