Density functional theory was employed to investigate the (111), (200), (210), (211) and (220) surfaces of CoS₂. The surface energies were calculated with a sulfur environment using first-principle-based thermodynamics. It is founded that surfaces with metal atoms at their outermost layer have higher energy. The stoichiometric (220) surface terminated by two layer of sulfur atoms is most stable under the sulfur-rich condition, while the non-stoichiometric (211) surface terminated by a layer of Co atoms has the lower energy under the sulfur-poor environment. The electric structure results show that the front valence electrons of (200) surface are active, indicating that there may be some active sites on this face. There is an energy gap between the stoichiometric (220) and (211), which has low Fermi energy, indicating that their electronic structures are dynamically stable. Spin-polarized bands are calculated on the stoichiometric surfaces, and these two (200) and (210) surfaces are predicted to be noticeably spin-polarized. The Bravais–Friedel–Donnay–Harker (BFDH) method is adopted to predict crystal growth habit. The results show that the most important crystal planes for the CoS₂ crystal growth are (111) and (200) planes, and the macroscopic morphology of CoS₂ crystal may be spherical, cubic, octahedral, prismatic or plate-shaped, which have been verified by experiments.

采用密度泛函理论研究CoS ₂的(111)、(200)、(210)、(211)和(220)表面。使用基于第一原理的热力学在硫环境下计算表面能。研究发现，最外层有金属原子的表面具有较高的能量。以两层硫原子封端的化学计量（220）表面在富硫条件下最稳定，而以一层Co原子封端的非化学计量（211）表面在贫硫环境下能量较低。电性结构结果表明(200)面的正面价电子活跃，表明该面上可能存在一些活性位点。化学计量的(220)和(211)之间存在能隙，其费米能量较低，表明它们的电子结构是动态稳定的。在化学计量表面上计算自旋极化带，预计这两个 (200) 和 (210) 表面具有明显的自旋极化。采用 Bravais-Friedel-Donnay-Harker (BFDH) 方法来预测晶体生长习性。结果表明，CoS ₂晶体生长最重要的晶面是(111)和(200)面，CoS ₂晶体的宏观形貌可以是球形、立方形、八面体、棱形或板形，已被通过实验验证。