Direct Imaging of Atomic Permeation Through a Vacancy Defect in the Carbon Lattice.
Direct Imaging of Atomic Permeation Through a Vacancy Defect in the Carbon Lattice.
复制标题
DOI：
10.1002/anie.202010630
复制
发表时间：
2020-12-14
期刊：
影响因子：
--
通讯作者：
Kaiser U
中科院分区：
文献类型：
--
作者：
Cao K;Skowron ST;Stoppiello CT;Biskupek J;Khlobystov AN;Kaiser U
多孔石墨烯作为新一代筛选原子、离子和分子的选择性膜具有广阔的应用前景。然而，通过石墨烯晶格中的缺陷渗透的原子机制仍然不清楚，并且在原子水平上仍然没有观察到。在这里，通过原子分辨率，在真实的时间内，一个接一个地直接观察来自纳米颗粒的钯原子穿过单壁碳纳米管中的缺陷，揭示了原子渗透的关键阶段。在穿过亚纳米孔之前和之后，移动原子和孔周围的悬挂键之间的键合在该过程中起着重要作用。石墨烯晶格的曲率决定性地定义了从凹侧到凸侧的渗透方向，这是由于如通过密度泛函理论计算所证实的弯曲表面处的金属-碳键合的差异，从而证明了多孔碳纳米管用于原子筛分的潜力。这项工作通过原位畸变校正高分辨率透射电子显微镜成像揭示了原子渗透通过石墨烯晶格中的亚纳米孔的机制，突出了移动的原子和亚纳米孔周围的悬挂键之间的化学键合的重要性。这种新的现象和渗透机理可能在多孔石墨烯碳基膜的过滤过程中发挥作用。
Porous graphene has shown promise as a new generation of selective membrane for sieving atoms, ions and molecules. However, the atomistic mechanisms of permeation through defects in the graphenic lattice are still unclear and remain unobserved in action, at the atomic level. Here, the direct observation of palladium atoms from a nanoparticle passing through a defect in a single‐walled carbon nanotube one‐by‐one has been achieved with atomic resolution in real time, revealing key stages of the atomic permeation. Bonding between the moving atom and dangling bonds around the orifice, immediately before and after passing through the subnano‐pore, plays an important role in the process. Curvature of the graphenic lattice crucially defines the direction of permeation from concave to convex side due to a difference in metal‐carbon bonding at the curved surfaces as confirmed by density functional theory calculations, demonstrating the potential of porous carbon nanotubes for atom sieving. This work reveals the mechanism of atomic permeation through a subnano‐pore in graphenic lattice by in situ aberration‐corrected high‐resolution transmission electron microscopy imaging, highlighting the importance of chemical bonding between the mobile atom and dangling bonds around the subnano‐pore. This new phenomenon and permeation mechanism are likely to play a role in the filtration processes by porous graphenic carbon based membranes.
登录
查看更多内容
影响因子：
29.4
作者：
Salzmann, Christoph G.;Llewellyn, Simon A.;Green, Malcolm L. H.
通讯作者：
Green, Malcolm L. H.
DOI：
10.1071/ph850125
发表时间：
1985-01-01
期刊：
AUSTRALIAN JOURNAL OF PHYSICS
影响因子：
--
作者：
WILHELM, HE
通讯作者：
WILHELM, HE
影响因子：
16.6
作者：
Cao K;Zoberbier T;Biskupek J;Botos A;McSweeney RL;Kurtoglu A;Stoppiello CT;Markevich AV;Besley E;Chamberlain TW;Kaiser U;Khlobystov AN
通讯作者：
Khlobystov AN
影响因子：
56.9
作者：
Holt, JK;Park, HG;Bakajin, O
通讯作者：
Bakajin, O
影响因子：
2.8
作者：
Banhart, F;Redlich, P;Ajayan, PM
通讯作者：
Ajayan, PM