耗散粒子动力学与可极化ABEEM力场结合模拟嵌段共聚物自组装形态调控

doi:10.7503/cjcu20150552

摘要/Abstract

摘要：

本文采用介观尺度上的耗散粒子动力学与基于ABEEM可极化力场的全原子分子动力学相结合的方式, 从理论上探究了嵌段共聚物结构、对称性、分子组成及温度等对嵌段共聚物最终自组装结构形态的影响. 模拟结果表明, 这些因素均会对嵌段共聚物在选择性溶剂中的最终自组装结构产生一定影响. 这一理论研究为实现可控操纵自组装结构, 提供了有意义的参考.

关键词: 耗散粒子动力学, ABEEM力场, 嵌段共聚物, 囊泡, 胶束, 自组装结构调控

Abstract:

Mesoscopic dissipative particle dynamics(DPD) simulations and all-atom molecular dynamics simulations were combined to investigate the influence of the architecture, symmetry, molecular composition of block copolymers and temperature on final assembled structures of block copolymers. From the simulation results, these factors have an influence on the final assembled structures. This theoretical investigation provides a reference for experiments and practice to manipulate self-assembled structures.

Key words: Dissipative particle dynamics, ABEEM force field, Block copolymer, Vesicle, Micelle, Self-assembly structure control

中图分类号:

O641

TrendMD:

刘林林, 杨忠志. 耗散粒子动力学与可极化ABEEM力场结合模拟嵌段共聚物自组装形态调控. 高等学校化学学报, 2015, 36(11): 2179.

LIU Linlin, YANG Zhongzhi. Self-assembly Morphological Control of Block Copolymers Simulated via the Combination of Dissipative Particle Dynamics and ABEEM Polarizable Force Field^†. Chem. J. Chinese Universities, 2015, 36(11): 2179.

图/表 8

Fig.1 Illustration of coarse-grained mapping of PS290-PI110 diblock copolymer from atomistic to DPD model Every PS and PI particle represents 10 PS and PI monomers, respectively.

Table 1 Flory-Huggins parameters χij obtained from all-atom molecular dynamics simulations

System	χ_ij
PS-PS	0
PS-PI	3.79
PS-n-Heptane	5.00
PI-n-Heptane	0.53

Table 2 Repulsion parameters αij resulted from Flory-Huggins parameters χij

System	α_ij
PS-PS	25.00
PI-PI	25.00
PS-PI	37.40
PI-Heptane	26.73
Heptane-Heptane	25.00
PS-Heptane	41.35

Fig.2 Simulation snapshots of aggregates self-assembled from linear(A) and cyclic PS290-PI110 diblock copolymer(B) in heptane at a certain simulation step(concentration 0.20) t*=104 DPD time steps. (A1) Initial; (A2) 1t*; (A3) 2t*; (A4) 3t*; (A5) 4.8t*; (A6) 100t*. (B1) Initial; (B2) 1t*; (B3) 2t*; (B4) 4t*; (B5) 10t*; (B6) 100t*. Blue: PS segments; orange: PI segments. The solvents(red) are omitted for clarity in most snapshots.

Fig.3 Simulation snapshots of aggregates self-assembled from linear(A) and cyclic symmetric PS200-PI200 diblock copolymer(B) in heptane at a certain simulation step (concentration 0.20) t*=104 DPD time steps. (A1) Initial; (A2) 1t*; (A3) 2t*; (A4) 3t*; (A5) 4.8t*; (A6) 100t*. (B1) Initial; (B2) 1t*; (B3) 2t*; (B4) 4t*; (B5) 10t*; (B6) 100t*. Blue: PS segments; orange: PI segments. The solvents(red) are omitted for clarity in most snapshots.

Fig.4 Simulation snapshots of aggregates self-assembled from PS390-PI240(A) and PS390-PI180 diblock copolymer(B) in heptane at a certain simulation step(concentration 0.22) t*=104 DPD time steps. (A1) Initial; (A2) 1t*; (A3) 2t*; (A4) 4t*; (A5) 8t*; (A6) 100t*. (B1) Initial; (B2) 1t*; (B3) 2t*; (B4) 3.5t*; (B5) 7t*; (B6) 100t*. Blue: PS segments; orange: PI segments. The solvents(red) are omitted for clarity in most snapshots.

Fig.5 Simulation snapshots of aggregates self-assembled from PS200-PI90 diblock copolymer in heptane at the temperature of 1.0 kBT(A) and 1.4 kBT(B) at a certain simulation step(concentration 0.25) t*=104 DPD time steps. (A1), (B1) Initial; (A2), (B2) 1t*; (A3), (B3) 2t*; (A4), (B4) 3t*; (A5), (B5) 11t*; (A6), (B6) 100t*. Blue: PS segments; orange: PI segments. The solvents(red) are omitted for clarity in most snapshots.

Fig.6 Simulation snapshots of aggregates self-assembled from PS200-PI60 diblock copolymer in heptane at the temperature of 1.0 kBT(A) and 1.6 kBT(B) at a certain simulation step(concentration 0.22) t*=104 DPD time steps. (A1) Initial; (A2) 2t*; (A3) 19t*; (A4) 32t*; (A5) 418t*; (A6) 1000t*. (B1) Initial; (B2) 1t*; (B3) 2t*; (B4) 5t*; (B5) 11t*; (B6) 1000t*. Blue: PS segments; orange: PI segments. The solvents(red) are omitted for clarity in most snapshots.

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