Supporting Information

Distribution and mobility of crude oil-brine in clay mesopores:

Insights from molecular dynamics simulations

Lihu Zhang†, Xiancai Lu‡*, Xiandong Liu†, Qin Li†, Yongxian Cheng†, Qingfeng Hou
∥ , Jingong Cai§

† State Key Laboratory for Ore Deposits Research, School of Earth Sciences and

Engineering, Nanjing University, Nanjing Jiangsu, 210023, P. R. China

‡ Key Lab of Surficial Geochemistry of Ministry of Education, School of Earth Sciences

and Engineering, Nanjing University, Nanjing Jiangsu, 210023, P. R. China

∥ State Key Laboratory of Enhanced Oil Recovery, Research Institute of Petroleum

Exploration and Development, China National Petroleum Corporation (CNPC), Beijing

100083, People’s Republic of China

§ Tongji University, State Key Lab Marine Geology, Shanghai 200092, P. R. China.

*Corresponding author:

Prof. Xiancai Lu, School of earth sciences and engineering, Nanjing University,

Nanjing, Jiangsu Province, 210023, China

Email: xcljun@nju.edu.cn

Tel: 86-25-89681065
Figure S1. The mean square displacement (MSD) of each oil component in the mesopore of model-H (upper) and model-L (lower).
Figure S2. The masscenter trajectories and mean square displacement (MSD) of carbazoles in representative aggregates/clusters in the mesopore of model-H (right)

and mode-L (left). The unwrapped x-coordinates (a1, b1, c1, d1,e1 and f1) and y-coordinates (a2, b2, c2, d2, e2 and f2) are employed for the sake of continuity. The

horizontal dashed lines in (a3,b3 and c3) approximatively correspond to the position of oil/brine interfaces of model-H, and the ends of vertical axis in (d3, e3, and f3)

correspond to the position of pore walls of model-L. The diffusion coefficient (D) of each aggregate/cluster was averaged based on the corresponding molecules.
Figure S3. Number density profiles of hydrocarbon (a), organic acid (b), carbazole (c), and thioether

(d) along z-direction in model-H under EMD and NEMD simulations. The hydrogen atoms in all

organics were excluded in the calculation of z-density profiles. The ends of horizontal axis of z-

density profiles correspond to the position of the porewalls.

Figure S4. Number density profiles of hydrocarbon (a), organic acid (b), carbazole (c), and thioether

(d) along z-direction in model-L under EMD and NEMD simulations. The hydrogen atoms in all

organics were excluded in the calculation of z-density profiles. The ends of horizontal axis of z-

density profiles correspond to the position of the porewalls.

Figure S5. The distribution probability of end-to-end distance of four straight chain hydrocarbons

in model-H and model-L under EMD and NEMD simulations. end-to-end distance means the

distance between the head and tail carbon atom of targeted molecule.
Table S1. Detailed components of brine and crude oil in model-H and model-L. The amount of each oil component is listed in parenthesis.

composition model-H model-L molecular structure

H2O 30000 2500
Na+ 300 191
brine
Ca2+ 90 7
Cl- 300 25

C12H26(80), C23H48(85),
Chain hydrocarbons C16H34(210), C20H42(170),
C13H28(80), C15H32(170), C19H40(80)

Naphthenic hydrocarbons C14H28(105), C13H26(325), C16H30(265)

oil C13H20(265), C16H20(220),

Aromatic hydrocarbons
C17H24(50), C16H18(55)
C10O2H20(55), C11O2H20(260),
Organic acids
C12O2H22(160)
carbazole C21NH27(50)

thioether C21SH44(70)