Electrochemical nitrogen reduction reaction (NRR) is becoming increasingly promising alternatively to the traditional Haber-Bosch process but developing efficient electrocatalysts is still a challenge. In this job, we searched that the catalytic performance of Cr₂B₂ for NRR by way of density functional theory (DFT) calculations. We mainly screened out four favorable N₂ adsorbed structures, including N₂ adsorption on the B-B bonds, Cr-B bonds, top site of B and Cr atom. It was found that the largest adsorption energy was −1.235 eV when N₂ was adsorbed on the Cr-B bond in a side-on structure, and has a better excellent NRR catalytic activity with the limiting potential is 0.29 V. The catalytic activity of all structures was better in the alternating mechanism of nitrogen reduction reaction. As the antibonding orbitals approach the Fermi level, the number of electrons in the antibonding orbitals increases. The limiting potential of T_Cr_end can also be reduced from 0.88 V to 0.35 V by NN bond breaking after the second hydrogen, which contribute to the greater NRR performance. We hope that this research will offer a viable strategy for the design of NRR catalysts, and offer a new way of thinking for MBene as a catalyst for NRR.

电化学氮还原反应 (NRR) 替代传统的 Haber-Bosch 工艺变得越来越有前景，但开发高效的电催化剂仍然是一个挑战。在这项工作中，我们通过密度泛函理论（DFT）计算研究了 Cr ₂ B ₂对 NRR的催化性能。我们主要筛选出四种有利的N ₂吸附结构，包括在BB键、Cr-B键、B和Cr原子的顶部位点上的N ₂吸附。发现当 N ₂以侧向结构吸附在Cr-B键上，具有较好的优异NRR催化活性，极限电位为0.29 V。在氮还原反应的交替机制下，所有结构的催化活性均较好。随着反键轨道接近费米能级，反键轨道中的电子数量增加。T _Cr _end的极限电位也可以通过第二个氢后的N N 键断裂从 0.88 V 降低到 0.35 V ，这有助于提高 NRR 性能。我们希望这项研究能为 NRR 催化剂的设计提供一种可行的策略，并为 MBene 作为 NRR 催化剂提供一种新的思路。