期刊
JOURNAL OF MOLECULAR LIQUIDS
卷 325, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.molliq.2020.115183
关键词
DNA nucleobases; DFT calculations; Phosphorene; ALMO-EDA; Adsorption; Intermolecular forces
资金
- CONICYT/FONDECYT [11170289]
- CONICYT/FONDEQUIP [EQM180180]
- Universidad Tecnologica Metropolitana [L318-04]
- NLHPC [ECM-02]
In this study, the uptake of Watson-Crick DNA nucleobases onto metal/metalloid phosphorene nanoflakes was investigated using density functional theory. The results show that the nucleobases form stable complexes with doped-phosphorene through coordinate covalent bonding, with attractive electrostatic interactions being the main driving force. The research suggests the potential use of doped-phosphorene materials for future technologies related to DNA constituents in solution.
In pursuit of novel nanodevices for the manipulation of DNA constituents, layered phosphorene materials have emerged as promising candidates due to their excellent uptake properties, biocompatibility, and in vivo biodegradability. Here, a density functional theory (DFT) study is performed to explore the uptake of Watson-Crick DNA nucleobases onto metal/metalloid phosphorene nanoflakes (MPhos, M=Al, Si, Ti, Cu), providing microscopic insights to understand the molecular structure, adsorption stability, intermolecular forces, and effects on the electronic properties of the formed complexes in solution. Structural/stability analyses show that DNA nucleobases form stable complexes with doped-phosphorene by coordinate covalent bonding (chemisorption) in a mainly stacked adsorption pattern. Solvation effects considerably decrease the adsorption stability onto SiPhos, but (Al, Ti. Cu)Phos nanoflakes show adsorption energies higher than similar to 1 eV, acting as excellent uptake platforms of DNA biomolecules in solution. Binding and energy decomposition analyses (AIM, IGM, ALMO-EDA) reveal that the intermolecular forces (adsorption mechanism) are mainly driven by attractive electrostatic interactions (41-55%) and complemented with a balanced interplay between charge transfer, polarization, and dispersion driving forces. DNA nucleobases also act as n-dopants, inducing charge doping of the MPhos adsorbents. The latter cause considerable variations in the electronic structure of TiPhos and CuPhos nanoflakes. implying potential uses in the sensing of DNA constituents. Furthermore, electron-density and electron delocalization indexes reveal that the aromatic character of nucleobases is not affected upon chemisorption. These results provide an atomistic perspective on the potential use of doped-phosphorene materials for future adsorption, analysis, sensing, and/or resembling technologies of DNA constituents in solution. (C) 2020 Elsevier B.V. All rights reserved.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据