Developing highly efficient and nonprecious electrocatalysts for oxygen-involving energy conversion reactions is crucial for the development of clean and sustainable energy technologies. Herein, the intrinsic relationship between the atomic structure and the catalytic activity of Ni₃S₂ was investigated based on density functional theory. It was found that the Ni₃S₂ (100) surface exhibits promising bifunctional catalytic activity towards the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER). The ORR catalytic activity of Ni₃S₂ (100) can be enhanced by the doping of Cu, and the OER catalytic activity of Ni₃S₂ (100) can be improved by the doping of Se. Furthermore, a descriptor derived from the electron affinity was developed, which correlate Ni₃S₂ microstructures with their catalytic activities. This study provides a systematic understanding to the intrinsic activity of transition metal sulfides, paving the way to the rational design and development of advanced electrocatalysts for renewable energy technology.

为涉及氧气的能量转换反应开发高效且非贵重的电催化剂对于清洁和可持续能源技术的发展至关重要。在此，基于密度泛函理论研究了原子结构与Ni ₃ S ₂催化活性之间的内在关系。发现Ni ₃ S ₂ (100) 表面对氧还原反应(ORR) 和析氧反应(OER) 表现出良好的双功能催化活性。Ni的ORR催化活性₃小号₂（100）可以通过Cu的掺杂来增强，并且Ni的OER催化活性₃小号₂(100) 可以通过 Se 的掺杂得到改善。此外，还开发了一种源自电子亲和势的描述符，它将 Ni ₃ S ₂微观结构与其催化活性相关联。该研究为过渡金属硫化物的内在活性提供了系统的理解，为合理设计和开发用于可再生能源技术的先进电催化剂铺平了道路。