Govind Rajan Ananth, Silmore Kevin S, Swett Jacob, Robertson Alex W, Warner Jamie H, Blankschtein Daniel, Strano Michael S
Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA.
Lockheed Martin Space, Palo Alto, CA, USA.
Nat Mater. 2019 Feb;18(2):129-135. doi: 10.1038/s41563-018-0258-3. Epub 2019 Jan 14.
The presence of extended defects or nanopores in two-dimensional (2D) materials can change the electronic, magnetic and barrier membrane properties of the materials. However, the large number of possible lattice isomers of nanopores makes their quantitative study a seemingly intractable problem, confounding the interpretation of experimental and simulated data. Here we formulate a solution to this isomer cataloguing problem (ICP), combining electronic-structure calculations, kinetic Monte Carlo simulations, and chemical graph theory, to generate a catalogue of unique, most-probable isomers of 2D lattice nanopores. The results demonstrate remarkable agreement with precise nanopore shapes observed experimentally in graphene and show that the thermodynamic stability of a nanopore is distinct from its kinetic stability. Triangular nanopores prevalent in hexagonal boron nitride are also predicted, extending this approach to other 2D lattices. The proposed method should accelerate the application of nanoporous 2D materials by establishing specific links between experiment and theory/simulations, and by providing a much-needed connection between molecular design and fabrication.
二维（2D）材料中存在扩展缺陷或纳米孔会改变材料的电子、磁性和屏障膜特性。然而，纳米孔大量可能的晶格异构体使得对其进行定量研究成为一个看似棘手的问题，这使得对实验和模拟数据的解释变得混乱。在这里，我们提出了一种解决异构体编目问题（ICP）的方法，结合电子结构计算、动力学蒙特卡罗模拟和化学图论，生成二维晶格纳米孔独特的、最可能的异构体目录。结果与在石墨烯中实验观察到的精确纳米孔形状显示出显著的一致性，并表明纳米孔的热力学稳定性与其动力学稳定性不同。还预测了六方氮化硼中普遍存在的三角形纳米孔，将这种方法扩展到其他二维晶格。所提出的方法应通过在实验与理论/模拟之间建立特定联系，以及通过提供分子设计与制造之间急需的联系，加速纳米多孔二维材料的应用。
