Three-dimensional molecular geometry of PEG hydrogels by an “expansion-contraction” method through Monte Carlo simulations
Three-dimensional molecular geometry of PEG hydrogels by an “expansion-contraction” method through Monte Carlo simulations
复制标题
DOI：
10.1007/s10118-015-1620-4
复制
发表时间：
2015-03
影响因子：
4.3
通讯作者：
Aokai Zhang;Jun Ling;Yu-wei Sun;G. Fu
中科院分区：
文献类型：
--
作者：
Aokai Zhang;Jun Ling;Yu-wei Sun;G. Fu
使用三维 (3-D) 粗粒度蒙特卡罗算法来模拟铜 (I) 催化叠氮化物-炔环加成 (CuAAC) 形成的溶胀水凝胶的构象。该模拟由三个连续步骤组成，包括扩散、交联和松弛。立即模拟多功能反应位点的交联，然后进行快速交联。为了探索该方法的有效性，制备并表征了具有三功能和四功能反应位点（分别为 G3 和 G4）的原始聚乙二醇（PEG）水凝胶。模拟数据与实验结果（例如交联之间的 PEG 长度、孔体积和孔半径分布）非常吻合，表明建模算法的有效性。 G3 和 G4 网络中计算的 PEG 长度很接近（约 4.6 nm）。水凝胶网络的 3D 视觉拓扑结构表明，“理想”水凝胶远非立方体、菱形或任何明确的规则重复细胞结构。
Three-dimensional (3-D) coarse-grained Monte Carlo algorithms were used to simulate the conformations of swollen hydrogels formed by copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC). The simulation consists of three successive steps including diffusion, cross-linking and relaxation. The cross-linking of multifunctional reaction sites is simulated instantly followed by fast crosslinking. In order to explore the validity of this approach pristine poly(ethylene glycol) (PEG) hydrogels with tri- and tetra-functional reaction sites (G3 and G4 respectively) were prepared and characterized. The data from the simulations were found to be in good agreement with experimental results such as PEG lengths between crosslinks, pore volume and pore radius distribution, indicating the validity of the modeling algorithm. The calculated PEG lengths in G3 and G4 networks are close (≈ 4.6 nm). The 3-D visual topological structure of the hydrogel network suggests that the “ideal” hydrogel is far from cubic, diamond or any well defined structures of regular repeating cells.