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Brownian dynamics simulation of a bonded network of reversibly adsorbed particles: Towards a model of protein adsorbed layers

机译:可逆吸附粒子的键合网络的布朗动力学模拟:建立蛋白质吸附层模型

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We present computer simulations of adsorbed protein monolayers modelled as networks of spherical particles. This network is generated through the formation of flexible bonds between the particles. The particles are attracted to a flat (fluid/fluid) interface by a potential well, which is truncated in one direction (the solution). As a consequence, unbonded particles establish an equilibrium between the bulk solution and the interface, where they become adsorbed. In an adsorbed monolayer consisting of bonded particles, the individual particles still have the freedom to adsorb. However, in this case, the monolayer as a whole does not desorb spontaneously. If such a monolayer is strongly compressed, it forms a far thicker interfacial structure with particles extending several particle diameters into the solution. As the interface is compressed, the interfacial pressure increases initially, but then reaches a maximum value, decreases slightly and levels off. Desorption of particles and their movement away from the (crowded) interface reduces the local repulsive interparticle interactions. Upon re-expansion, the particle network completely returns to its original monolayer structure. However, formation of new bonds between particles during the compression-expansion cycle (reflecting the chemical reactivity of the adsorbed protein) introduces a strong element of irreversibility. In this case, a patchy structure is formed at the interface after the expansion. Finally, the effect of strongly adsorbing displacer particles is explored, which can have a similar influence on the adsorbed monolayer as a compression of the interface.
机译:我们目前的计算机模拟的吸附蛋白单层建模为球形颗粒网络。该网络是通过粒子之间形成柔性键而生成的。粒子被势阱吸引到平坦(流体/流体)界面,势阱在一个方向(溶液)被截断。结果,未结合的颗粒在本体溶液和界面之间建立了平衡,在那里它们被吸附。在由键合颗粒组成的吸附单层中,单个颗粒仍具有吸附的自由度。然而,在这种情况下,单分子层整体上不会自发解吸。如果这样的单层被强烈压缩,则其形成的界面结构要厚得多,并且颗粒的直径会扩展到溶液中。随着界面被压缩,界面压力开始增加,但随后达到最大值,略有下降并趋于平稳。粒子的解吸及其远离(拥挤)界面的运动减少了局部排斥粒子间的相互作用。重新扩展后,粒子网络将完全返回其原始的单层结构。然而,在压缩-膨胀循环期间在颗粒之间形成新的键(反映了所吸附蛋白质的化学反应性)引入了不可逆的强烈因素。在这种情况下,扩展后在界面处会形成斑驳的结构。最后,探讨了强吸附性置换颗粒的作用,它对界面的压缩作用对吸附的单分子层具有相似的影响。

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