First-principles Study on Electronic Structure and Optical Properties of Single Point Defect Graphene Oxide

doi:10.15541/jim20190588

Abstract

Abstract:

In this study, the electronic structure and optical properties of graphene oxide in different structures with single point defect are studied under local density of states approximation and generalized gradient approximation by first-principles calculations based on the density functional theory. The results show that four models are mechanically stable, among which the oxide graphene containing unsaturated oxygen atoms shows an important application potential in water cracking and catalysis. The calculated band structures and partial-wave density of states show that the model containing unsaturated oxygen atoms exhibits indirect band gap, while other models exhibit direct band gap, and the doping type and band gap values vary with different models. The absorption spectrum of graphene oxide is anisotropic, and the absorption edge moves to the near-UV and visible region in the direction perpendicular to the plane. The optical absorption coefficient containing sp ³ hybrid is slightly higher than that containing sp ² hybrid, suggesting that the carbon-oxygen double bond and hanging bond have important influence on the absorption spectrum.

Key words: first-principles calculation, graphene oxide, optical property, band, absorbance

CLC Number:

O649

LIN Qimin, CUI Jiangong, YAN Xin, YUAN Xueguang, CHEN Xiaoyu, LU Qichao, LUO Yanbin, HUANG Xue, ZHANG Xia, REN Xiaomin. First-principles Study on Electronic Structure and Optical Properties of Single Point Defect Graphene Oxide[J]. Journal of Inorganic Materials, 2020, 35(10): 1117-1122.

Figures/Tables 7

Fig. 1 Different types of graphene oxide structures (a) Graphene oxide adsorbed with hydroxyl; (b) Graphene oxide with single substitution epoxy bond; (c) Graphene oxide with carbon oxygen double bond and sp3 hybrid epoxy bond; (d) Graphene oxide with two carbon-oxygen double bonds and one carbon-oxygen single bond; (e, f) and (e1, f1) Top and side views of the structure in (d) adsorbed with hydrogen on the upper and lower side of the suspended oxygen atom, respectively

Table 1 Bond length in different structures calculated by different pseudopotential functions (nm)

	^*	O₁-C₂	O₂-C₆	O₃-C₁₂
LDA	d₁	0.128	0.128	0.137
	d₂	0.128	0.128	0.136
	e	0.124	0.124	0.138
	f	0.124	0.124	0.137
GGA	d	0.124	0.124	0.133
	e	0.122	0.122	0.139
	f	0.122	0.122	0.138

Table 2 Formation energy with different structures (eV)

^*	(a)	(b)	(c)	(d)	(e)	(f)
LDA	-12.7	-6.1	-6.5	-13.1	-19.6	-18.6

Table 3 Elastic coefficients of graphene oxide with different structures

^*	C₁₁	C₂₂	C₁₂	C₆₆
a	1738.99	1618.45	282.75	1.03
b	1789.57	1761.01	309.15	1.63
c	1607.47	958.73	163.94	0.99
d	2015.11	1405.41	147.00	1.39
e	1968.65	825.43	148.48	-11.90
f	1846.90	710.38	240.54	-8.83

Fig. 2 The charge number of three kinds of different atoms in three structures showing in Fig. 1(d), (e) and (f) (d) Graphene oxide with two carbon-oxygen double bonds and one carbon-oxygen single bond; (e, f) Structure (d) adsorbed with hydrogen on the upper and lower side of the suspended oxygen atom, respectively

Fig. 3 Band structures and density of states (DOS) of different structure models (a) Graphene oxide adsorbed with hydroxyl; (b) Graphene oxide with single substitution epoxy bond; (c) Graphene oxide with carbon oxygen double bond and sp3 hybrid epoxy bond; (d) Graphene oxide with two carbon-oxygen double bonds and one carbon-oxygen single bond; (e,f) Structure (d) adsorbed with hydrogen on the upper and lower side of the suspended oxygen atom, respectively

Fig. 4 Absorption coefficient of different structure models in which (b-g) the absorption coefficient of graphene and structures in Fig. 1(a-f) (a) Graphene; (b) Graphene oxide adsorbed with hydroxyl; (c) Graphene oxide with single substitution epoxy bond; (d) Graphene oxide with carbon oxygen double bond and sp3 hybrid epoxy bond; (e) Graphene oxide with two carbon-oxygen double bonds and one carbon-oxygen single bond; (f, g) Structure (d) adsorbed with hydrogen on the upper and lower side of the suspended oxygen atom, respectively

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