Atomic Edge-Guided Polyethylene Crystallization on Monolayer Two-Dimensional Materials
Atomic Edge-Guided Polyethylene Crystallization on Monolayer Two-Dimensional Materials
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DOI：
10.1021/acs.macromol.1c01978
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发表时间：
2022-01
期刊：
影响因子：
5.5
通讯作者：
Dong Zhou;M. Fuentes-Cabrera;Akash Singh;R. Unocic;J. Carrillo;Kai Xiao;Yumeng Li;Bo Li
中科院分区：
文献类型：
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作者：
Dong Zhou;M. Fuentes-Cabrera;Akash Singh;R. Unocic;J. Carrillo;Kai Xiao;Yumeng Li;Bo Li
在这里，我们结合联合收割机的二维（2D）材料（MoSe 2）具有良好定义的原子边缘配置与从头算和原子分子动力学（MD）模拟研究如何原子边缘与聚乙烯（HDPE）链在稀溶液组装过程中相互作用的先进合成。我们的研究结果表明，钼封端的锯齿形（Mo-ZZ）的边缘作为首选的成核网站和强烈的相互作用与HDPE链。HDPE链与Mo-ZZ边缘平行排列，并形成垂直于边缘的薄片阵列。有趣的是，观察到原子边缘配置显着改变这种相互作用。同一块MoSe 2在不同棱边的情况下，不同棱边处的结晶差异明显。通过对HDPE链段正构烷烃（n= 5和25）与MoSe_2的从头算和分子动力学模拟，发现MoSe_2的原子结构影响其与正构烷烃链的相互作用.根据Mo-ZZ边缘优先成核原理，通过形成具有平行原子台阶的多层MoSe 2，可以实现HDPE层片的可控长程取向。这项研究开辟了一条通往原子水平理解聚合物-2D纳米材料相互作用的途径。它还弥合了原子级和远程介观结构之间的差距，并引入了一种新的远程结构控制策略。
Here, we combine an advanced synthesis of two-dimensional (2D) materials (MoSe2) having well-defined atomic edge configurations withab initioand atomistic molecular dynamics (MD) simulations to study how atomic edges interact with polyethylene (HDPE) chains in a dilute solution assembly process. Our results reveal that Mo-terminated zigzag (Mo-ZZ) edges act as preferred nucleation sites and strongly interact with HDPE chains. The HDPE chains align in parallel with the Mo-ZZ edges and form arrays of lamellae that are perpendicular to the edges. Interestingly, atomic edge configurations are observed to dramatically change such interactions. The crystallization discrepancy at different edges was demonstrated on the same piece of MoSe2with different types of edges. Theab initioand MD simulations betweenn-alkane (n= 5 and 25), a segment of HDPE, and MoSe2suggest that the atomic structures of MoSe2can affect their interactions withn-alkane chains. Following the Mo-ZZ edge preferred nucleation principle, controlled long-range alignment of HDPE lamellae can be realized by creating multilayer MoSe2with parallel atomic steps. This research opens a pathway toward an atomic level understanding of polymer–2D nanomaterial interactions. It also bridges the gap between atomic-level and long-range mesoscopic structures and introduces a novel strategy for long-range structural control.