论文标题
通过聚合物中有理设计的组对MXENE的强烈调节和功能化：一项理论研究
Strongly Modulated Exfoliation and Functionalization of MXene with Rational Designed Groups in Polymer: A Theoretical Study
论文作者
论文摘要
随着新兴的原子超薄金属化合物，由于表面终止丰富和高金属电导率，MXENES对催化剂和纳米电子应用显示出巨大的希望。但是，层间粘附和遭受环境干扰的趋势显着限制了它们的耐力和效率。通过进行第一原理计算，我们在本文中探索了通过聚合物对MXENE的表面钝化和去角质，这些聚合物已在实验上证明可以促进性能。九种单体与典型的MXENE TI3C2T2（T = NONE，O，F，OH，F0.5O0.5）作为原型复合材料，分别探索了与能量和化学氧化还原相关的吸附和电荷转移。我们的工作表明，裸Ti3c2 mxene具有强大的裂解和分解单体的能力。表面功能化的TI3C2F2，TI3C2FO和TI3C2O2仅通过范德华力与单体具有弱结合，而Ti3c2（OH）2（OH）2也表现出对某些单体的结合增强的结合。单体中的特定官能团，例如卤素，硫和羟基或相对平面的芳族结构，在很大程度上有助于吸附。我们揭示通过聚合物的功能化将通过MXENES中的界面电荷转移改变载体的密度。虽然裸露的TI3C2和TI3C2（OH）2向聚合物捐赠电子，而Ti3c2f2，Ti3C2FO和Ti3C2O2则获得了从聚合物转移的少量电子，这取决于多组群的类型。不同单体的电荷转移和去角质能的各种能力意味着设计聚合物以去角质去角质并调节载体密度，这非常需要改变电导率，介电性能和促进耐力。
As emerging atomically ultrathin metal compounds, MXenes show great promise for catalysts and nanoelectronics applications due to the abundant surface terminations and high metallic conductivity. However, the tendency of the interlayer adhesion and suffering from environmental disturbances significantly limit their endurance and efficiency. Herein via conducting first-principles calculations, we explore surface passivation and exfoliation of MXene via polymers which have been experimentally proven to promote the performance. Nine kinds of monomers together with the typical MXene Ti3C2T2 (T= None, O, F, OH, F0.5O0.5) as prototype composites are explored with respect to the adsorption and charge transfer associated with energetics and chemical redox, respectively. Our work shows that naked Ti3C2 MXene has a strong ability to cleave and decompose the monomers. Surface functionalized Ti3C2F2, Ti3C2FO, and Ti3C2O2 have a weak binding with monomers through only van der Waals force, whereas Ti3C2(OH)2 also exhibits strengthened binding for some monomers. Specific functional groups in the monomer, such as the halogen, sulfur, and hydroxyl groups or a relatively planar aromatic structure, largely contribute to the adsorption. We reveal that the functionalization through polymer would alter the carriers' density via interfacial charge transfer in MXenes. While the naked Ti3C2 and Ti3C2(OH)2 donate electrons to the polymers, the Ti3C2F2, Ti3C2FO, and Ti3C2O2 receive small amounts of electrons transferred from the polymer, highly depending on the types of the monomers. The varying ability of charge transfer and exfoliation energy of different monomers implies great flexibility for designing polymers to exfoliate the MXene and modulate the carrier densities which is highly desired for altering conductivity, dielectric properties, and promoted endurance.
