The two-step strategy screening based high throughput calculation is an effective method to search for highly active single atom catalysts (SACs) for efficient nitrogen reduction reaction (NRR), sharing a common feature of active metal centers MN₄. However, this method faces the lack of descriptor for designing SACs due to limited data. Herein we proposed a robust empirical rule to estimate 312 credible limiting potentials for NRR over 104 C₃N-supported SACs. It is found that the limiting potential scales clearly with the adsorption free energies of two key reaction intermediates (∗N₂H and ∗NH₂), which are significantly dependent on the structure relating descriptor φ, and the activity of SACs with and without N coordination exhibits similar catalytic efficiency. We identified four high-performance SACs having moieties of CrC₂N₂, CrC₄, MnC₄ and OsC₄ with high selectivity towards NRR and competitive limiting potentials of −0.40, −0.45, −0.53 and −0.54 V, respectively. The φ values for these four SACs are around 19–25 which fall within its optimal ranges of 20–25 validating its prediction fidelity. This work broadens the discovery of two-dimensional carbon-nitrides supported SACs free of N coordination towards efficient N₂ reduction and opens a new route of descriptor-guided design of efficient SACs for electrocatalysis process.

基于高通量计算的两步策略筛选是寻找用于高效氮还原反应 (NRR) 的高活性单原子催化剂 (SAC) 的有效方法，具有活性金属中心 MN ₄的共同特征。然而，由于数据有限，该方法面临缺乏设计 SAC 的描述符。在此，我们提出了一个稳健的经验规则来估计 104 个 C ₃ N 支持的 SAC 上NRR 的 312 个可信限制潜力。发现极限电位与两个关键反应中间体（*N ₂ H 和 ∗NH ₂)，这在很大程度上取决于与描述符 φ 相关的结构，并且有和没有 N 配位的 SAC 的活性表现出相似的催化效率。我们确定了具有CRC部分四个高性能的SAC ₂ Ñ ₂，CRC ₄，MNC ₄和OSC ₄具有朝向NRR高选择性和-0.40，-0.45，-0.53和-0.54分别V，有竞争力的限制的电势。这四个 SAC 的 φ 值约为 19-25，落在其 20-25 的最佳范围内，验证了其预测保真度。这项工作拓宽了对二维碳氮化物支持的 SAC 的发现，该 SAC 没有 N 配位，可实现高效的 N ₂ 并为电催化过程中高效 SAC 的描述符引导设计开辟了一条新途径。