Long‐term chemical durability of borosilicate glasses that makes them a widely accepted form of nuclear waste disposal is achieved through the formation of a porous aluminosilicate gel layer that provides passivity and limits the transport of water to the reaction front. Detailed understanding of the porous silicate gel layer is thus critical in elucidating the corrosion mechanism of these glasses and to design of new glass composition for waste immobilization and other applications. In this paper, we use the diffuse charge reactive potential to generate porous aluminosilicate glass structures with compositions equivalent to the gel layers formed at the glass‐water interface with an aim to understand the processing condition on the microstructure and atomic structure of these systems. We demonstrate the use of the charge scaling techniques is an effective approach to generate these porous structures with controllable pore mophologies. After initial validation of the potentials and calcium aluminosilicate glass structures using neutron diffraction, we created gel structures with compositions similar to well‐known model nuclear waste borosilicate glasses. The porosities and the pore size distribution bear a strong correlation to the processing temperature, as well as to the local atomic structure. Thus, by controlling the processing parameters, the generated porous structures can be customized to closely resemble gel structures due to borosilicate glass corrosion. These results provide insights of the micro‐ and atomic structure features of the porous aluminosilicate glasses and on the optimal procedure to generate porous structures that can be comparable to experimentally observed gel layer structures thus to elaborate on the correlations between the structure and phenomena in glass‐water interactions.

中文翻译：

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反应性分子动力学模拟的纳米多孔硅铝酸盐玻璃的原子和微观结构特征

硼硅酸盐玻璃的长期化学耐用性通过形成多孔的铝硅酸盐凝胶层（可提供钝性并限制水向反应前沿的传输）而实现，从而使其成为广为接受的核废料处置形式。因此，对多孔硅酸盐凝胶层的详细了解对于阐明这些玻璃的腐蚀机理以及设计用于固定废物和其他应用的新型玻璃组合物至关重要。在本文中，我们使用弥散电荷反应势来生成多孔硅铝酸盐玻璃结构，其成分与在玻璃水界面形成的凝胶层相同，目的是了解这些系统的微观结构和原子结构的加工条件。我们证明了使用电荷缩放技术是一种产生具有可控孔学的多孔结构的有效方法。在使用中子衍射对电位和铝硅酸钙玻璃结构进行了初步验证之后，我们创建了具有类似于众所周知的核废硼硅酸盐玻璃模型的凝胶结构。孔隙率和孔径分布与加工温度以及局部原子结构密切相关。因此，通过控制工艺参数，可以定制所产生的多孔结构以使其由于硼硅酸盐玻璃腐蚀而非常类似于凝胶结构。