Kumar Anjan, Sayyed M I, Sabugaa Michael M, Al-Bahrani Mohammed, Sharma Shilpa, Saadh Mohamed J
Nanotechnology Laboratory, GLA University Mathura-281406 India.
Department of Physics, Faculty of Science, Isra University Amman 11622 Jordan.
RSC Adv. 2023 Apr 24;13(18):12554-12571. doi: 10.1039/d3ra01231j. eCollection 2023 Apr 17.
Density Functional Theory (DFT) was employed to investigate the interaction between cyanogen chloride (ClCN) and the surface of a carbon nanocone (CNC). The findings of this research revealed that pristine CNC is not an ideal material to detect ClCN gas due to its minimal alterations in electronic properties. In order to enhance the properties of carbon nanocones, multiple methods were implemented. These included functionalizing the nanocones with pyridinol (Pyr) and pyridinol oxide (PyrO) as well as decorating them with metals such as boron (B), aluminium (Al) and gallium (Ga). Additionally, the nanocones were also doped with the same third-group metal (B, Al and Ga). The simulation results indicated that doping it with aluminium and gallium atoms yielded promising results. After a comprehensive optimization process, two stable configurations were obtained between the ClCN gas and the CNC-Al, and CNC-Ga structures (configurations S21, and S22) with values of -29.11, and -23.70 kcal mol respectively, using M06-2X/6-311G(d) level. The adsorption of ClCN on CNC-Al and CNC-Ga surfaces leads to a marked alteration in the electrical properties of these structures. Calculations reveal that the energy gap between the Highest Occupied Molecular Orbital (HOMO) and Lowest Unoccupied Molecular Orbital (LUMO) levels ( ) of these configurations increased in the range of 9.03% and 12.54%, respectively, thereby giving off a chemical signal. An analysis conducted by the NCI confirms that there is a strong interaction between ClCN and Al and Ga atoms in CNC-Al and CNC-Ga structures, which is represented by the red color in the RDG isosurfaces. Additionally, the NBO charge analysis reveals that significant charge transfer is present in S21 and S22 configurations (190 and 191 |me|, respectively). These findings suggest that the adsorption of ClCN on these surfaces impacts the electron-hole interaction, which subsequently alters the electrical properties of the structures. Based on the DFT results, the CNC-Al and CNC-Ga structures, which have been doped with aluminium and gallium atoms, respectively, have the potential to serve as good candidates for detecting ClCN gas. Among these two structures, the CNC-Ga structure emerged as the most desirable one for this purpose.
采用密度泛函理论（DFT）研究了氯化氰（ClCN）与碳纳米锥（CNC）表面之间的相互作用。该研究结果表明，原始的CNC并非检测ClCN气体的理想材料，因为其电子性质变化极小。为了增强碳纳米锥的性能，实施了多种方法。这些方法包括用吡啶醇（Pyr）和吡啶醇氧化物（PyrO）对纳米锥进行功能化，以及用硼（B）、铝（Al）和镓（Ga）等金属对其进行修饰。此外，纳米锥还掺杂了相同的第三主族金属（B、Al和Ga）。模拟结果表明，用铝和镓原子对其进行掺杂产生了有前景的结果。经过全面的优化过程，在ClCN气体与CNC - Al和CNC - Ga结构之间获得了两种稳定构型（构型S21和S22），使用M06 - 2X/6 - 311G(d)水平时，其值分别为 - 29.11和 - 23.70 kcal mol⁻¹。ClCN在CNC - Al和CNC - Ga表面的吸附导致这些结构的电学性质发生显著变化。计算表明，这些构型的最高占据分子轨道（HOMO）和最低未占据分子轨道（LUMO）能级之间的能隙（ΔE）分别在9.03%和12.54%的范围内增加，从而发出化学信号。NCI进行的分析证实，在CNC - Al和CNC - Ga结构中，ClCN与Al和Ga原子之间存在强相互作用，这在RDG等值面中以红色表示。此外，NBO电荷分析表明，在S21和S22构型中存在显著的电荷转移（分别为190和191 |me|）。这些发现表明，ClCN在这些表面上的吸附影响了电子 - 空穴相互作用，进而改变了结构的电学性质。基于DFT结果，分别掺杂了铝和镓原子的CNC - Al和CNC - Ga结构有潜力作为检测ClCN气体的良好候选材料。在这两种结构中，CNC - Ga结构成为用于此目的的最理想结构。
