Interfacial structures and acidity constants of goethite from first-principles Molecular Dynamics simulations

被引：7

作者：

Zhang, Yingchun ^{[1
]}

Liu, Xiandong ^{[1
]}

Cheng, Jun ^{[2
]}

Lu, Xiancai ^{[1
]}

机构：

[1] Nanjing Univ, Sch Earth Sci & Engn, State Key Lab Mineral Deposits Res, Nanjing 210023, Jiangsu, Peoples R China

[2] Xiamen Univ, Coll Chem & Chem Engn, Xiamen 361005, Fujian, Peoples R China

来源：

AMERICAN MINERALOGIST | 2021年 / 106卷 / 11期

基金：

中国国家自然科学基金;

关键词：

Goethite; acidity constant; interfacial structure; first-principles Molecular Dynamics; DENSITY-FUNCTIONAL THEORY; CHROMATE RETENTION MECHANISMS; INTRINSIC PROTON AFFINITY; ATOMIC-SCALE STRUCTURES; REACTIVE SURFACE GROUPS; ALPHA-FEOOH; ORGANIC-MATTER; METAL (HYDR)OXIDES; FE(II) ADSORPTION; ELECTRON-TRANSFER;

D O I：

10.2138/am-2021-7835

中图分类号：

P3 [地球物理学]; P59 [地球化学];

学科分类号：

0708 ; 070902 ;

摘要：

In this paper, we report a first-principles Molecular Dynamics (FPMD) study of interfacial structures and acidity constants of goethite. The pKa values of the groups on (010), (110), and (021) surfaces (space group Pbnm) are derived with the FPMD based vertical energy gap technique. The results indicate that major reactive groups include Fe2OH2 and FeOH2 on (010), FeOH2, Fe3OLH, and Fe3OUH on (110), and FeOhH2 and Fe2OH on (021). The interfacial structures were characterized in detail with a focus on the hydrogen bonding environment. With the calculated pKa values, the point of zero charges (PZCs) of the three surfaces are derived and the overall PZC range of goethite is found to be consistent with the experiment. We further discuss the potential applications of these results in future studies toward understanding the environmental processes of goethite.

引用

页码：1736 / 1743

页数：8

共 50 条

[1] Acidity constants of lumiflavin from first principles molecular dynamics simulations
Kilic, Murat
Ensing, Bernd
[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (35) : 18993 - 19000
[2] Acidity of uranyl(VI) hydrate studied with first-principles molecular dynamics simulations
Buehl, Michael
Kabrede, Hendrik
[J]. CHEMPHYSCHEM, 2006, 7 (11) : 2290 - 2293
[3] Structures and Acidity Constants of Silver-Sulfide Complexes in Hydrothermal Fluids: A First-Principles Molecular Dynamics Study
He, Mengjia
Liu, Xiandong
Lu, Xiancai
Zhang, Chi
Wang, Rucheng
[J]. JOURNAL OF PHYSICAL CHEMISTRY A, 2016, 120 (42): : 8435 - 8443
[4] Surface Acidity and As(V) Complexation of Iron Oxyhydroxides: Insights from First-Principles Molecular Dynamics Simulations
Zhang, Yingchun
Liu, Xiandong
Cheng, Jun
Lu, Xiancai
[J]. Environmental Science and Technology, 2021, 55 (23): : 15921 - 15928
[5] Surface Acidity and As(V) Complexation of Iron Oxyhydroxides: Insights from First-Principles Molecular Dynamics Simulations
Zhang, Yingchun
Liu, Xiandong
Cheng, Jun
Lu, Xiancai
[J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2021, 55 (23) : 15921 - 15928
[6] Anharmonic force constants extracted from first-principles molecular dynamics: applications to heat transfer simulations
Tadano, T.
Gohda, Y.
Tsuneyuki, S.
[J]. JOURNAL OF PHYSICS-CONDENSED MATTER, 2014, 26 (22)
[7] Complex molecular and ionic liquids from first-principles molecular dynamics simulations
Kirchner, Barbara
Firaha, Dzmitry
Holloczki, Oldamur
Thomas, Martin
Sanz, Iris Sancho
[J]. ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2015, 250
[8] Large timesteps in first-principles molecular dynamics simulations
Tsuchida, E
Terakura, K
[J]. JOURNAL OF THE PHYSICAL SOCIETY OF JAPAN, 2001, 70 (03) : 924 - 925
[9] First-principles molecular dynamics simulations in a continuum solvent
Fattebert, JL
Gygi, F
[J]. INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY, 2003, 93 (02) : 139 - 147
[10] Thermal resistance of an interfacial molecular layer by first-principles molecular dynamics
Thuy-Quynh Duong
Massobrio, Carlo
Ori, Guido
Boero, Mauro
Martin, Evelyne
[J]. JOURNAL OF CHEMICAL PHYSICS, 2020, 153 (07):

← 1 2 3 4 5 →