几何尺寸及缺陷对石墨炔纳米带热输运特性的影响

doi:10.11949/0438-1157.20230242

摘要/Abstract

摘要：

基于分子动力学模拟方法，对石墨炔纳米带（GYNR）的热输运特性进行了深入研究，重点探讨了几何尺寸、缺陷类型及缺陷的位置（水平方向和垂直方向、苯环与乙炔链）和排列方式等对声子热输运的影响规律，揭示并分析了其声子热输运调控机理。研究结果表明，理想GYNR的热导率仅为18.22 W/（m·K），且相比于石墨烯，GYNR随尺寸增大热导率仅升至21.37 W/（m·K），对几何尺寸依赖较小；对于缺陷类型，空位缺陷的存在相比于氮掺杂对热导率抑制更强，可低至9.19 W/（m·K）；对于缺陷位置，位于苯环上或靠近纳米带边界时相比于炔链热导率更低；多个缺陷若以平行分布相比于三角形结构分布可获得更低的热导率，低于8.00 W/（m·K）。研究结果可以为石墨炔材料在纳米器件的热电领域开发、应用及调控等方面提供理论支持和参考。

关键词: 石墨炔纳米带, 纳米材料, 热传导, 几何尺寸, 缺陷, 分子模拟

Abstract:

Based on the molecular dynamics simulation method, the thermal transport properties of graphyne nanoribbons (GYNR) are profoundly studied, focusing on the influence of geometrical dimensions, defect type and defect position (horizontal and vertical directions, benzene ring and acetylene chain), and arrangement on the phonon thermal transport, etc., and the regulation mechanism of the phonon thermal transport is revealed and analyzed. The research results show that the ideal thermal conductivity of GYNR is only 18.22 W/(m·K). Compared with graphene, the thermal conductivity of GYNR only rises to 21.37 W/(m·K) with the increase of size. The thermal conductivity of GYRN is less dependent on the geometry size. For defect types, the thermal conductivity is suppressed more strongly in the presence of vacancy defects than nitrogen doping, which can be as low as 9.19 W/(m·K). For the location of defects, the thermal conductivity is lower when the defects are located on the benzene ring or near the nanoribbon boundary compared to the alkyne chain. If multiple defects are distributed in parallel, the thermal conductivity can lower than 8.00 W/(m·K) compared with the triangular structure distribution. The results can provide theoretical support and reference for the development, application and regulation of graphyne materials in the thermoelectric field of nano-devices.

Key words: graphyne nanoribbons, nanomaterials, heat conduction, geometrical dimensions, defect, molecular simulation

中图分类号:

TB 34

刘远超, 蒋旭浩, 邵钶, 徐一帆, 钟建斌, 李耑. 几何尺寸及缺陷对石墨炔纳米带热输运特性的影响[J]. 化工学报, 2023, 74(6): 2708-2716.

Yuanchao LIU, Xuhao JIANG, Ke SHAO, Yifan XU, Jianbin ZHONG, Zhuan LI. Influence of geometrical dimensions and defects on the thermal transport properties of graphyne nanoribbons[J]. CIESC Journal, 2023, 74(6): 2708-2716.

图/表 17

图1 6×6×1石墨炔超胞

Fig.1 Schematic diagram of 6×6×1 super cell of graphyne

图2 不同空位缺陷位置的ZGYNR

Fig.2 ZGYNR with different vacancy defect locations

表1 不同长度和宽度的AGYNRs

Table 1 AGYNRs with different lengths and widths

宽4.12 nm		长14.39 nm
长度/nm	原子数	宽度/nm	原子数
14.39	1538	4.12	1538
22.41	2498	6.68	2458
34.53	3858	9.25	3378
44.51	4978	11.82	4298
53.07	5938

图3 AGYNR结构示意图

Fig.3 Schematic diagram of AGYNR structure

图4 有缺陷的AGYNR

Fig.4 Defective AGYNR

图5 模拟过程

Fig.5 Simulation process

图6 ZGYNR轴向温度分布

Fig.6 Axial temperature distribution of ZGYNR

图7 AGYNR热导率随长度变化关系

Fig.7 Influence of length change on thermal conductivity of AGYNR

图8 AGYNR热导率随宽度变化关系（300 K）

Fig.8 Influence of width change on thermal conductivity of AGYNR（300 K）

图9 AGYNR热导率-温度曲线

Fig.9 Thermal conductivity-temperature curves of AGYNR

图10 AGYNR长度-热导率的倒数拟合曲线

Fig.10 Inverse fitting curve of length-thermal conductivity of AGYNR

图11 热导率随X轴空位缺陷位置变化关系（固定缺陷在Y轴Y=1.374 nm）

Fig.11 Change of thermal conductivity with the position of vacancy defect on X-axis (fixed defect on Y-axis Y=1.374 nm)

图12 热导率随X轴上空位缺陷位置变化关系（固定四组缺陷位于不同Y轴位置）

Fig.12 Change of thermal conductivity with the position of vacancy defect on X-axis (the fixed four groups of defects are located in different Y-axis positions)

图13 热导率随Y轴空位缺陷位置变化关系（固定缺陷在X轴X=0.621 nm）

Fig.13 Change of thermal conductivity with the position of Y-axis vacancy defect (fixed defect in X-axis X=0.621 nm)

图14 热导率随Y轴空位缺陷位置变化关系（固定六组缺陷位于不同X轴位置）

Fig.14 Change of thermal conductivity with the position of vacancy defect on Y-axis (the fixed six groups of defects are located in different X-axis positions)

图15 不同缺陷位置的GYNR热导率-温度特性曲线

Fig.15 Thermal conductivity-temperature characteristic curves of GYNR with different defect locations

图16 不同缺陷排布的GYNR热导率-温度特性曲线

Fig.16 Thermal conductivity-temperature characteristic curves of GYNR with different defect arrangements

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