Au(100)表面亲/疏水性质的密度泛函理论研究

韦涛; 陈建华; 陈晔

doi:10.13779/j.cnki.issn1001-0076.2022.01.001

Au(100)表面亲/疏水性质的密度泛函理论研究

广西大学资源环境与材料学院, 广西南宁 530004

基金项目:
国家自然科学基金(NSFC 51864003)

详细信息

作者简介: 韦涛(1997-), 男, 广西河池人, 硕士研究生, 主要从事矿物处理与加工研究, E-mail: 743277881@qq.com

通讯作者: 陈建华(1971-), 男, 四川西昌人, 教授, 博士生导师, 主要从事浮选理论与工艺、矿物浮选量子化学、矿产资源综合利用等研究, E-mail: jhchen@gxu.edu.cn

中图分类号: TD91;TD953⁺.1

收稿日期: 2022-02-25

刊出日期: 2022-02-25

Density Functional Theory Study on Hydrophilic/hydrophobic Properties of Au (100) Surface

Guangxi University, College of Resources, Environment and Materials, Nanning 530004, Guangxi, China

More Information

Corresponding author: CHEN Jianhua, jhchen@gxu.edu.cn

Received Date: 25 February 2022

Publish Date: 25 February 2022

摘要

摘要:
采用密度泛函理论, 研究了单个、一层、多层(两层、三层)水分子与Au(100)表面的相互作用, 从原子层面上分析Au(100)表面的亲/疏水性质。同时结合分子动力学模拟, 分析水滴在金表面的润湿过程, 进而从介观层面上揭示金表面的亲/疏水性质。结果表明, 单个水分子在Au(100)表面是物理吸附。与单个水分子吸附构型相比, 一层水分子吸附构型中存在层内氢键作用, 多层水分子吸附构型中存在层内氢键和层间氢键作用。随着水分子层数的增多, 多层水分子吸附构型的内层水分子与Au(100)表面原子的平均作用距离呈现逐渐减小的趋势。水滴在金表面的分子动力学模拟结果表明, 有机污染会对金表面的润湿性产生较大影响, 导致金表面呈现一定的疏水性, 而清洁金表面则为亲水性。
- Au(100) /
- 亲/疏水性 /
- 表面 /
- 密度泛函理论 /
- 润湿性
Abstract:
The interaction of single, one layer, multilayer (two layer, three layer) water molecules with Au(100) surface was studied Using density functional theory, and the hydrophilic/hydrophobic properties of Au(100) surface were analyzed at atomic level. In addition, the hydrophilic/hydrophobic properties of the gold surface were revealed from the mesoscopic level through analyzing the wetting process of water droplets on the gold surface by molecular dynamics simulation. The results show that individual water molecules are physically adsorbed on Au(100) surface. Compared with a single water molecule, hydrogen bond interaction exists between one and multiple layers of water molecules, and the adsorption energy of one or multiple layers of water molecules is obviously higher than that of a single water molecule. The adsorption energy increases with the increase of the number of water layers. Molecular dynamics simulation results of water droplets on gold surface show that organic pollution has a great influence on the wettability of gold surface, resulting in a certain hydrophobicity of gold surfacewhile clean gold surface is hydrophilic.
- Au(100) /
- hydrophilic/hydrophobic /
- surface /
- density functional theory /
- wettability

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图 1 Au(100)面的吸附位点

Figure 1.

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图 2 单个水分子在Au(100)面顶位的吸附构型

Figure 2.

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图 3 单个水分子在Au(100)表面顶位吸附前后的态密度

Figure 3.

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图 4 单个水分子在Au(100)表面顶位吸附的电子密度

Figure 4.

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图 5 一层(a)、两层(b)、三层(c)水分子在Au(100)面的吸附构型(紫色虚线表示氢键)

Figure 5.

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图 6 水滴在Au(100)表面清洁及吸附少量甲醛状态下的润湿过程

Figure 6.

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表 1 单个水分子在Au(100)面的吸附能及作用距离

Table 1. Adsorption energy and action distance of a single water molecule on Au(100) surface

吸附构型	吸附位点	E_ads/(kJ·mol^-1)	d_O-Au/Å	d_H-Au/Å
单个水分子	顶位	-11.28	2.564	2.796
单个水分子	桥位	-7.14	3.086	2.809
单个水分子	穴位	-6.40	3.251	2.681

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表 2 水分子的H、O原子和Au(100)表面的Au1原子吸附前后的Mulliken布居

Table 2. Mulliken populations of H and O atoms of water molecules and Au1 atoms before and after adsorption on Au (100) surface

元素	吸附状态	s	p	d	f	total	Charge/e
H1	吸附前	0.48	0.00	0.00	0.00	0.48	0.52
H1	吸附后	0.56	0.00	0.00	0.00	0.56	0.44
H2	吸附前	0.48	0.00	0.00	0.00	0.48	0.52
H2	吸附后	0.56	0.00	0.00	0.00	0.56	0.44
O	吸附前	1.90	5.14	0.00	0.00	7.04	-1.04
O	吸附后	1.87	4.96	0.00	0.00	6.83	-0.83
Au1	吸附前	2.91	6.41	9.68	14.00	33.00	-0.00
Au1	吸附后	2.82	6.48	9.66	14.00	32.96	0.04

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表 3 一层、两层、三层水分子在Au(100)面的作用距离范围及平均作用距离

Table 3. Action distance range and average action distance of water molecules in the first, second and third layers on Au(100) surface

吸附构型	分层	内层水分子的氧与金原子作用距离范围d_O-Au/Å	内层水分子的氧与金原子平均作用距离d_O-Au/Å
一层水分子	一层	3.265~3.692	3.472
两层水分子	内层	2.534~3.668	3.203
三层水分子	内层	2.649~3.675	3.083

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