基于第一性原理的不同结构石墨炔热电输运特性研究

doi:10.11949/0438-1157.20230929

摘要/Abstract

摘要：

石墨炔是一种新兴的二维层状材料，在热电领域具有应用前景。基于第一性原理的计算方法，分别对γ-石墨炔、δ-石墨炔和α-石墨炔的热电输运特性进行深入研究，重点探讨三种不同结构对声子热输运、电子电导和热电优值的影响规律。研究结果表明，γ、δ和α结构的石墨炔在室温下具有较低的热导率，分别为31.19947、13.44974、5.87009 W·m^-1·K^-1，且随温度升高热导率逐渐降低；在电输运方面，三种不同结构的石墨炔在适当载流子掺杂下表现出较高的功率因数，分别为0.135、0.045、0.011 W·m^-1·K^-2；最终获得最大热电优值ZT_max分别约为2.93、2.22、1.67。不同原子结构的石墨炔材料在热、电领域各具优势，在sp杂化碳原子的合理分配下可形成Dirac锥，或可调小带隙，并获得较低的热导率，热电优值最大可达2.93。不同结构的石墨炔材料的热电性能研究，将有助于其在热电领域的应用，并为二维层状碳纳米材料在热电领域的应用提供借鉴和参考。

关键词: 纳米材料, 石墨炔, 热传导, 电导率, 热电优值, 第一性原理, 数值模拟

Abstract:

Graphyne is an emerging two-dimensional layered material with promising applications in the field of thermoelectricity. An objective of this paper is to profoundly investigate the thermoelectric transport properties of γ, δ, and α structured graphyne using first principles calculations. This paper mainly discussed the effect regularities of the three different structures on phonon thermal transport, electronic conductivity, and thermoelectric figure of merit. The results show that graphdiyne with γ, δ and α structures have low thermal conductivity at room temperature, which are 31.19947, 13.44974 and 5.87009 W·m^-1·K^-1, respectively, and the thermal conductivity gradually decreases as the temperature increases. In terms of electrical transport, the three different structures of graphyne demonstrate high power factors under appropriate carrier doping, which are 0.135, 0.045, and 0.011 W·m^-1·K^-2, respectively. Consequently, the maximum thermoelectric figure of merit (ZT_max) was obtained to be about 2.93, 2.22, and 1.67 for each respective structure. The graphyne materials with different atomic structures have their own advantages in the fields of heat and electricity. Under the rational distribution of sp-hybridized carbon atoms, these materials can form Dirac cones or tunable small band gaps, and obtain lower thermal conductivity. The maximum thermoelectric figure of merit can reach 2.93. The thermoelectric performance of graphyne materials with different structures will contribute to their application in the field of thermoelectric, and provide reference and inspiration for the application of two-dimensional layered carbon nanomaterials in the field of thermoelectric.

Key words: nanomaterials, graphyne, heat conduction, conductivity, thermoelectric figure of merit, first principles, numerical simulation

中图分类号:

TB 34

蒋旭浩, 刘远超, 徐一帆, 李耑, 刘新昊, 李梓硕. 基于第一性原理的不同结构石墨炔热电输运特性研究[J]. 化工学报, 2023, 74(12): 5016-5026.

Xuhao JIANG, Yuanchao LIU, Yifan XU, Duan LI, Xinhao LIU, Zishuo LI. Thermoelectric transport properties of graphyne with different structures based on first principles[J]. CIESC Journal, 2023, 74(12): 5016-5026.

图/表 14

图1 γ-石墨炔、δ-石墨炔和α-石墨炔的晶体结构

Fig.1 Crystal structure of γ-graphyne, δ-graphyne and α-graphyne

表1 γ-石墨炔、δ-石墨炔和α-石墨炔的晶格常数

Table 1 Lattice constant of γ-graphyne， α-graphyne and δ-graphyne

石墨炔结构	a/Å	b/Å	c/Å	α/(°)	β/(°)	γ/(°)
γ-石墨炔	6.88968	6.88968	20	90	90	120
δ-石墨炔	9.44480	9.44480	20	90	90	120
α-石墨炔	6.96272	6.96272	12	90	90	120

图2 以第一性原理方法计算石墨炔热电特性技术路线示意图

Fig. 2 Schematic diagram of technology roadmap for calculating thermoelectric characteristics of graphyne by first principles method

图3 γ-石墨炔、δ-石墨炔和α-石墨炔的各声子支对热导率贡献程度

Fig.3 Contribution proportion of phonon branches to the total thermal conductivity of γ-graphyne, δ-graphyne and α-graphyne at different temperatures

图4 γ-石墨炔、δ-石墨炔和α-石墨炔的声子谱

Fig.4 Phonon spectra of γ-graphyne, δ-graphyne and α-graphyne

图5 γ-石墨炔、δ-石墨炔和α-石墨炔随温度变化的热导率

Fig.5 Thermal conductivity of γ-graphyne, δ-graphyne and α-graphyne at different temperatures

图6 不同温度下 γ-石墨炔、δ-石墨炔和α-石墨炔的累积晶格热导率随MFP和频率的变化关系

Fig.6 Cumulative lattice thermal conductivity of γ-graphyne, δ-graphyne and α-graphyne as a function of the mean free path and frequency at different temperatures

图7 γ-石墨炔、δ-石墨炔和α-石墨炔的电子能带结构

Fig.7 Energy band structure of γ-graphyne, δ-graphyne and α-graphyne

图8 γ-石墨炔、δ-石墨炔和α-石墨炔随载流子浓度变化的Seebeck系数

Fig.8 Seebeck coefficients of γ-graphyne, δ-graphyne and α-graphyne as a function of carrier concentration

图9 γ-石墨炔、δ-石墨炔和α-石墨炔在300、500和700 K下的Seebeck系数随载流子浓度的变化

Fig.9 Seebeck coefficients of γ-graphyne, δ-graphyne and α-graphyne at 300, 500 and 700 K as a function of carrier concentration

图10 γ-石墨炔、δ-石墨炔和α-石墨炔随载流子浓度变化的电导率

Fig.10 Conductivity of γ-graphyne, δ-graphyne and α-graphyne as a function of carrier concentration

图11 γ-石墨炔、δ-石墨炔和α-石墨炔在300、500和700 K下的电导率随载流子浓度的变化

Fig.11 Conductivity of γ-graphyne, δ-graphyne and α-graphyne at 300, 500 and 700 K as a function of carrier concentration

图12 低载流子浓度下γ-石墨炔、δ-石墨炔和α-石墨炔的功率因数

Fig.12 Power factors of γ-graphyne, δ-graphyne and α-graphyne at low carrier concentration

图13 γ-石墨炔、δ-石墨炔和α-石墨炔随温度变化的最大热电优值

Fig.13 The maximum ZT values of γ-graphyne, δ-graphyne and α-graphyne at different temperatures

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