RGO/Al复合材料界面性质第一性原理研究

doi:10.15541/jim20210438

无机材料学报 ›› 2022, Vol. 37 ›› Issue (6): 651-659.DOI: 10.15541/jim20210438 CSTR: 32189.14.10.15541/jim20210438

所属专题：【材料计算】计算材料(202409)

RGO/Al复合材料界面性质第一性原理研究

孙铭(), 邵溥真, 孙凯, 黄建华, 张强(), 修子扬(), 肖海英, 武高辉

哈尔滨工业大学材料科学与工程学院, 哈尔滨 150001

收稿日期:2021-07-12 修回日期:2021-11-02 出版日期:2022-06-20 网络出版日期:2021-12-16
通讯作者: 张强, 教授. E-mail: zhang_tsiang@hit.edu.cn;
修子扬, 副教授. E-mail: xiuzy@hit.edu.cn
作者简介:孙铭(1998-), 女, 硕士研究生. E-mail: s1257973295@163.com
基金资助:
国家自然科学基金(52071117);国家自然科学基金(51771063);黑龙江省杰出青年科学基金(JQ2021E002)

First-principles Study on Interface of Reduced Graphene Oxide Reinforced Aluminum Matrix Composites

SUN Ming(), SHAO Puzhen, SUN Kai, HUANG Jianhua, ZHANG Qiang(), XIU Ziyang(), XIAO Haiying, WU Gaohui

School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China

Received:2021-07-12 Revised:2021-11-02 Published:2022-06-20 Online:2021-12-16
Contact: ZHANG Qiang, professor. E-mail: zhang_tsiang@hit.edu.cn;
XIU Ziyang, associate professor. E-mail: xiuzy@hit.edu.cn
About author:SUN Ming (1998–), female, Master candidate. E-mail: s1257973295@163.com
Supported by:
National Natural Science Foundation of China(52071117);National Natural Science Foundation of China(51771063);Heilongjiang Provincial Science Fund for Distinguished Young Scholars(JQ2021E002)

摘要/Abstract

摘要：

本研究采用基于密度泛函理论的第一性原理方法, 在广义梯度近似下, 分别建立了具有不同碳氧比的“铝/氧化石墨烯/铝(Al/GO/Al)”界面模型以及含缺陷“Al/GO/Al”三层界面模型。探讨了含氧官能团和单空位缺陷、双空位缺陷以及拓扑缺陷对还原氧化石墨烯增强铝基复合材料界面性质的影响。研究结果表明: 在“Al/GO/Al”界面模型中, 环氧基优于碳原子而与铝原子产生明显的电荷交互作用, 氧原子净电荷为-0.98 e, 铝原子净电荷为0.46 e, 环氧基有利于复合材料中还原氧化石墨烯与铝基体之间的界面结合。当缺陷存在时, 含缺陷的“Al/GO/Al”界面模型中缺陷处碳原子净电荷在-0.05 e至-0.38 e区间, 环氧基与碳原子之间存在较弱的相互作用, 与铝原子间相互作用明显较强。环氧基抑制了空位缺陷处碳原子与铝原子之间的反应, 可保护含空位还原氧化石墨烯中碳原子结构的完整性。本研究可为开发高性能Al/GO/Al基复合材料提供理论指导。

关键词: 第一性原理, 还原氧化石墨烯/铝复合材料, 氧化石墨烯/铝界面模型, 界面性质

Abstract:

An “aluminum/graphene oxide/aluminum (Al/GO/Al)” interface model with different carbon/oxygen ratio or with different defects was established. Effects of oxygen-containing functional groups and different defects on the interface of reduced graphene oxide/aluminum composites was studied using first principle method based on density functional theory (DFT). The results show that the epoxy group is better than carbon atom to produce obvious charge interaction with aluminum atom in the interface model of Al/GO/Al. The net charge of oxygen atom is -0.98 e while aluminum atom is 0.46 e, which is conducive to the interfacial bonding between reduced graphene oxide (RGO) and aluminum matrix in composites. When the defects exists, the net charge of carbon atoms at the defects in the Al/GO/Al interface model is in the range of -0.05 e to -0.38 e. Interaction between epoxy group and carbon atoms is weak, while interaction between epoxy group and aluminum atoms is significantly intensified. The existence of epoxy group can inhibit reaction between carbon atom and aluminum atom in the vacancy defects, and protect integrity of carbon structure in RGO with vacancy defects. Therefore, this research may provide theoretical guidance for development of high-performance Al/GO/Al matrix composites.

Key words: first principle, reduced graphene oxide/aluminum composite, graphene oxide/aluminum interface model, interface property

中图分类号:

TB331

孙铭, 邵溥真, 孙凯, 黄建华, 张强, 修子扬, 肖海英, 武高辉. RGO/Al复合材料界面性质第一性原理研究[J]. 无机材料学报, 2022, 37(6): 651-659.

SUN Ming, SHAO Puzhen, SUN Kai, HUANG Jianhua, ZHANG Qiang, XIU Ziyang, XIAO Haiying, WU Gaohui. First-principles Study on Interface of Reduced Graphene Oxide Reinforced Aluminum Matrix Composites[J]. Journal of Inorganic Materials, 2022, 37(6): 651-659.

图/表 14

图1 GO(Gr)原子模型与Al/GO(Gr)/Al界面模型

Fig. 1 GO(Gr) atomic model and Al/GO(Gr)/Al interface model (a) Gr atom model; (b-e) GO atomic models with C/O ratios of 24 : 1, 12 : 1, 8 : 1, and 6 : 1, respectively; (f) Al/Gr/Al interface model; (g-j) Al/GO/Al interface models with C/O ratios of 24 : 1, 12 : 1, 8:1, and 6 : 1, respectively

图2 含缺陷GO原子模型与含缺陷Al/GO/Al界面模型

Fig. 2 GO atom model and Al/GO/Al interface model both with defects (a) GO with single-vacancy defect; (b) GO with double-vacancy defect; (c) GO with Stone-Wales defect; (d) Al/GO/Al interface model with single-vacancy defect; (e) Al/GO/Al interface model with double- vacancy defect; (f) Al/GO/Al interface model with Stone-Wales defect

图3 不同原子层数对应Al表面模型的表面能

Fig. 3 Surface energy of Al surface model corresponding to different atomic layers

表1 Al/GO(Gr)/Al界面能量计算结果

Table 1 Calculation results of energy at the interface of Al/GO(Gr)/Al interface model

Interface model	E_Al/GO(Gr)/Al/eV	W_ad/(J·m^-2)	E_int/(J·m^-2)
Al/Gr/Al	-7790.9254	2.1894	-2.1918
Al/GO(1)/Al	-8230.1766	2.8727	-3.2239
Al/GO(2)/Al	-8668.9362	3.5572	-4.1941
Al/GO(3)/Al	-9108.2092	4.2686	-5.2290

图4 Al/GO(Gr)/Al界面模型的计算能量随环氧基数量的变化

Fig. 4 Energy calculation of Al/GO(Gr)/Al interface model according to the epoxy number

图5 不同Al/GO(Gr)/Al界面模型中不同原子PDOS曲线

Fig. 5 PDOS curves of C (a), Al (b) and O (c) atoms in different Al/GO(Gr)/Al interface models

表2 Al/Gr/Al界面模型Mulliken布居分析

Table 2 Mulliken populations of Al/Gr/Al interface model

Atom	Location	s	p	Charge/e
Al	Interface	1.28	1.70	0.02
C	Interface	1.05	2.98	-0.03

表3 Al/GO/Al界面模型Mulliken布居分析

Table 3 Mulliken populations of Al/GO/Al interface model

Atom	Location	s	p	Charge/e
Al	Location 1	1.04	1.50	0.46
Al	Location 2	1.28	1.70	0.02
O	Interface	1.88	5.10	-0.98
C	Interface	1.05	2.97	-0.03

图6 Al/Gr/Al (a)与Al/GO/Al (b)差分电荷密度

Fig. 6 Electron density difference of Al/Gr/Al (a) and Al/GO/Al (b)

图7 含缺陷Al/GO/Al界面模型能量计算

Fig. 7 Energy calculation of Al/GO/Al interface model with defects SW: Stone-Wales; SV: Single-vacancy; DV: Double-vacancy

图8 不同缺陷Al/GO/Al界面模型中不同原子PDOS曲线

Fig. 8 PDOS for different atoms in Al/GO/Al interface models with different defects (a) PDOS for Al atom; (b) PDOS for C atom; (c) PDOS for O atom

图9 含缺陷的Al/GO/Al差分电荷密度

Fig. 9 Electron density difference of Al/GO/Al with different defects (a, b) Single-vacancy defect in YZ direction; (c, d) Single-vacancy defect in vertical Z direction; (e, f) Double-vacancy defect in YZ direction; (g, h) Double-vacancy defect in vertical Z direction; (I, j) Stone-Wales defect in YZ direction; (k, l) Stone-sWales defect in vertical Z direction

表4 含缺陷Al/GO/Al布居分析

Table 4 Mulliken populations of Al/GO/Al with defects

Model	Atom	Position	s	p	Charge /e
SV	Al	Al1	1.05	1.47	0.48
		Al2	1.02	1.58	0.41
		Al3	1.22	1.65	0.13
	O	O	1.87	5.12	-0.99
	C	C1	1.24	3.13	-0.38
	C	C2-C3	1.10-1.19	2.97-2.91	-0.07- -0.10
DV	Al	Al1	1.05	1.47	0.48
		Al2	1.22	1.63	0.15
		Al3	1.22	1.71	0.07
	O	O	1.87	5.12	-0.99
	C	C1	1.20	2.94	-0.14
	C	C2-C4	1.06-1.18	2.99-2.91	-0.05- -0.09
SW	Al	Al1	1.05	1.45	0.50
		Al2	1.07	1.60	0.33
		Al3	1.22	1.68	0.10
	O	O	1.87	5.12	-0.99
	C	C1	1.15	3.09	-0.24
	C	C2	1.08	3.04	-0.12

图10 含缺陷的GO原子模型和相应的差分电荷密度

Fig. 10 GO atom model with defects (a-c) and corresponding electron density difference (d-f) at the interface of Al/GO/Al model (a, d) Single-vacancy; (b, e) Double-vacancy; (c, f) Stone-Wales defects

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RGO/Al复合材料界面性质第一性原理研究

First-principles Study on Interface of Reduced Graphene Oxide Reinforced Aluminum Matrix Composites

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