Molecular dynamics simulations of CH4/CO2 hydrates nucleation in kaolinite particles

Li，Yun1,2,3; Zhu，Jinlong2,3,4; Han，Songbai1,2,3; Zhang，Baifa5; Tang，Hui1,2,3; Yuan，Bao6,7; Wang，Pengfei1,2,3; Bao，Wancheng1,2,3; Wang，Xiaomeng1,2,3; Zhao，Yusheng1,2,3,4

2023

10.1016/j.apsusc.2022.154911

APPLIED SURFACE SCIENCE   Impact Factor & Quartile

0169-4332

1873-5584

Nucleation and growth mechanism of CH/CO hydrates has attracted great attention for CH/CO mixed gas separation and CO sequestration. In this study, the nucleation mechanism of CH/CO mixtures forming hydrate with different gas concentrations in the kaolinite (Kln) particles with hydroxyl and siloxane surface contacts was investigated using molecular dynamics simulations. The simulation results showed that CH-occupied 5 cages and CO-occupied 56 cages were initially formed in the bulk-like solution of Kln particles, which was facilitated by the adsorption of CH and CO molecules to form hydrate cages, regardless of the type of surface contacts on the Kln particles. The interaction between the adsorbed CH/CO molecules and the siloxane surface was the main factor that facilitated hydrate nucleation by forming clathrate-like structures. By contrast, the hydroxyl surface made a relatively minor contribution to hydrate nucleation because of the strong hydrogen bonds that formed on its surface. These results suggest that the different surface contacts of Kln particles should be considered a key factor in the nucleation and growth mechanism of CH/CO hydrates in marine sediments. These findings provide molecular insight into the mechanisms of CH/CO mixed gas separation and hydrate-based CO sequestration in Kln-rich sediments.

CH4/CO2 hydrates Kaolinite particles Molecular dynamics simulations Siloxane and hydroxyl surface contacts

SCI

English

Corresponding

National Natural Science Foundation of China["11775011","52106092"] ; China Postdoctoral Science Foundation[2020M682771] ; Guangdong Basic and Applied Basic Research Foundation["2020A1515111124","2022A1515010093"] ; Shenzhen Key Laboratory of Natural Gas Hydrates[ZDSYS20200421111201738] ; Southern Marine Science and Engineering Guangdong Laboratory (Guangzhou)[K19313901]

Chemistry ; Materials Science ; Physics

Chemistry, Physical ; Materials Science, Coatings & Films ; Physics, Applied ; Physics, Condensed Matter

WOS:000868700400003

ELSEVIER

MATERIALS SCIENCE

2-s2.0-85138995784

Scopus

1.Southern Marine Science and Engineering Guangdong Laboratory (Guangzhou),Guangzhou,511458,China
2.Shenzhen Key Laboratory of Natural Gas Hydrates,Southern University of Science and Technology,Shenzhen,518055,China
3.Academy for Advanced Interdisciplinary Studies,Southern University of Science and Technology,Shenzhen,518055,China
4.Department of Physics,Southern University of Science and Technology,Shenzhen,518055,China
5.School of Civil and Transportation Engineering,Guangdong University of Technology,Guangzhou,510006,China
6.Spallation Neutron Source Science Center,Dongguan,523803,China
7.Institute of High Energy Physics,Chinese Academy of Sciences,Beijing,100049,China

Li，Yun,Zhu，Jinlong,Han，Songbai,et al. Molecular dynamics simulations of CH4/CO2 hydrates nucleation in kaolinite particles[J]. APPLIED SURFACE SCIENCE,2023,607.

Li，Yun.,Zhu，Jinlong.,Han，Songbai.,Zhang，Baifa.,Tang，Hui.,...&Zhao，Yusheng.(2023).Molecular dynamics simulations of CH4/CO2 hydrates nucleation in kaolinite particles.APPLIED SURFACE SCIENCE,607.

Li，Yun,et al."Molecular dynamics simulations of CH4/CO2 hydrates nucleation in kaolinite particles".APPLIED SURFACE SCIENCE 607(2023).