论文标题
过渡金属单原子催化剂的高通量筛选氮还原反应
High-Throughput Screening of Transition Metal Single-Atom Catalysts for Nitrogen Reduction Reaction
论文作者
论文摘要
将金属作为减少氮反应的催化中心的发现激发了对单原子催化剂的极大热情。但是，可用SAC的活动不佳和选择性低远离工业需求。通过在第一原则计算中，掺杂工程可以有效地调节B-SB单层的NRR性能。特别是，从活性中心的电子结构的角度揭示了活化的N2的起源。在24个过渡金属掺杂剂中，RE@SB和TC@SB表现出最佳的NRR催化性能，具有较低的限制潜力。 RE@SB和TC@SB也可以显着抑制她，并达到100％的高理论法拉达效率。我们的发现不仅加速了氨合成催化剂的发现，而且有助于进一步阐明结构 - 性能相关性。
The discovery of metals as catalytic centers for nitrogen reduction reactions has stimulated great enthusiasm for single-atom catalysts. However, the poor activity and low selectivity of available SACs are far away from the industrial requirement. Through the high throughout first principles calculations, the doping engineering can effectively regulate the NRR performance of b-Sb monolayer. Especially, the origin of activated N2 is revealed from the perspective of the electronic structure of the active center. Among the 24 transition metal dopants, Re@Sb and Tc@Sb showed the best NRR catalytic performance with a low limiting potential. The Re@Sb and Tc@Sb also could significantly inhibit HER and achieve a high theoretical Faradaic efficiency of 100%. Our findings not only accelerate discovery of catalysts for ammonia synthesis but also contribute to further elucidate the structure-performance correlations.
