dataset for ''Spin-mediated promotion of Co catalysts for ammonia synthesis''

Over the past two decades, there has been a growing interest in developing novel catalysts to enable operation of the Haber-Bosch process under milder conditions. Rational design of a new class of catalysts requires new theory guidance and clear mechanistic understanding. Recently, a spin-mediated promotion mechanism was proposed to activate traditionally unreactive magnetic materials like Co for ammonia synthesis by introducing hetero metal atoms. In this study by combining theory and experiment, we validated this promotion mechanism on a La/Co system. Employing model catalyst studies conducted on Co single crystals and mass-selected Co nanoparticles at ambient pressure, we identified the active site for ammonia synthesis as the B5 site of Co steps with La adsorption. Remarkably, the turnover frequency of 0.47±0.03/s achieved on the La/Co system at 350°C and 1 bar surpasses that of any other model catalyst tested under identical conditions.

在过去二十年中，对于开发新型催化剂以实现哈伯-博世过程在更温和条件下运行的兴趣日益增长。一类新型催化剂的理性设计需要新的理论指导以及清晰的机理理解。近期，一种基于自旋介导的促进机制被提出，通过引入异质金属原子，激活传统上不活泼的磁性材料如Co，以实现氨的合成。在本研究中，通过理论分析与实验的结合，我们对La/Co体系中的这一促进机制进行了验证。在常压下，通过对Co单晶和通过质量选择制备的Co纳米粒子进行的模型催化剂研究，我们确定了氨合成的活性位点是Co台阶上的B5位，伴随La的吸附。令人瞩目之处在于，在350°C和1 bar的条件下，La/Co体系中实现的周转频率0.47±0.03/s超越了在相同条件下测试的所有其他模型催化剂。