Kowalczyk Piotr, Furmaniak Sylwester, Neimark Alexander V, Burian Andrzej, Terzyk Artur P
School of Mathematics, Statistics, Chemistry, and Physics, Murdoch University, Perth, WA 6150, Australia.
Stanisław Staszic State University of Applied Sciences in Piła, Podchorążych Street 10, 64-920 Piła, Poland.
J Phys Chem A. 2024 Mar 7;128(9):1725-1735. doi: 10.1021/acs.jpca.3c08203. Epub 2024 Feb 26.
Triply periodic minimal surfaces (TPMS) inspired by nature serve as a foundation for developing novel nanomaterials, such as templated silicas, graphene sponges, and schwarzites, with customizable optical, poroelastic, adsorptive, catalytic, and other properties. Computer simulations of reactions on TPMS using reactive intermolecular potentials hold great promise for constructing and screening potential TPMS with the desired properties. Here, we developed an off-lattice, surface-constrained Metropolis Monte Carlo (SC-MMC) algorithm that utilized a temperature quench process. The presented SC-MMC algorithm was used to investigate the process of graphitization reactions on the Schwarz primitive, Schwarz diamond, and Schoen gyroid TPMS, all with a cubic lattice parameter of 8 nm. We show that the optimized carbon TPMS exhibits a low energy, approximately -7.1 eV/atom, comparable to that of graphite and diamond crystals, along with a variety of topological defects. Furthermore, these structures showcase extensive and smooth surfaces characterized by a negative discrete Gaussian curvature, a distinctive feature indicative of an interconnected morphology. They possess specific surface areas of ∼2700 m/g, comparable to graphene, and exhibit a significant porosity of around 90%. The theoretical X-ray correlation functions and nitrogen adsorption isotherms confirm that the constructed TPMS exhibit remarkably similar surface properties, although the pore space topology varies significantly.
受自然启发的三重周期极小曲面（TPMS）为开发新型纳米材料奠定了基础，这些纳米材料包括模板化二氧化硅、石墨烯海绵和黑硅石等，具有可定制的光学、多孔弹性、吸附、催化及其他特性。利用反应性分子间势对TPMS上的反应进行计算机模拟，对于构建和筛选具有所需特性的潜在TPMS具有很大的前景。在此，我们开发了一种利用温度猝灭过程的非晶格表面约束 metropolis 蒙特卡罗（SC-MMC）算法。所提出的SC-MMC算法用于研究施瓦茨原始曲面、施瓦茨菱形曲面和舍恩曲面TPMS上的石墨化反应过程，所有这些曲面的立方晶格参数均为8nm。我们表明，优化后的碳TPMS具有低能量，约为-7.1eV/原子，与石墨和金刚石晶体相当，同时还存在各种拓扑缺陷。此外，这些结构展现出广泛且光滑的表面，其特征为负离散高斯曲率，这是一种表明相互连接形态的独特特征。它们的比表面积约为2700m²/g，与石墨烯相当，孔隙率约为90%。理论X射线相关函数和氮吸附等温线证实，尽管孔隙空间拓扑结构差异很大，但所构建的TPMS表现出非常相似的表面性质。
