Abstract Calcite is the most important component of limestone, an essential building material. When adsorbing water, the strength of calcite decreases, resulting in safety problems. Density functional theory (DFT) is widely used to elucidate the adsorption mechanisms of calcite surface at a molecular level. The adsorption structures and energies of H2O on calcite (104) surface were studied systematically for a wide coverage from 0 to 1.0 monolayers. The results show that a hollow site on calcite (104) surface is the most favorable when adsorbing H2O with an energy of 0.89 eV, followed by 0.71 eV at the bridge site and 0.64 eV at the top site, i.e., water molecules are easily adsorbed on calcite surface. Besides, the changes in the atomic structure, density of electronic states, and charge distribution of H2O/calcite (104) system before and after adsorption are discussed in detail for different coverages.

中文翻译：

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不同覆盖率方解石(104)表面H2O吸附的从头算研究

摘要 方解石是石灰石的最重要组成部分，是必不可少的建筑材料。吸水时，方解石的强度降低，造成安全问题。密度泛函理论（DFT）被广泛用于在分子水平上阐明方解石表面的吸附机制。系统地研究了 H2O 在方解石 (104) 表面的吸附结构和能量，覆盖范围从 0 到 1.0 个单层。结果表明，方解石(104)表面的空心位最有利于吸附H2O，能量为0.89 eV，其次是桥位0.71 eV，顶部位0.64 eV，即容易吸附水分子在方解石表面。此外，原子结构的变化，电子态的密度，