Flexible Iron\nClusters Promoting Ammonia Synthesis:\nA Density Functional Theory Prediction

In recent years, significant research has been conducted\non supported\nclusters due to their high dispersion, atomic efficiency, and unsaturated\ncoordination, particularly in ammonia synthesis. This study investigates\nthe catalytic performance of flexible iron clusters embedded in two-dimensional\ncarbon–nitrogen materials for ammonia synthesis. Using density\nfunctional theory and <i>ab initio</i> molecular dynamics\nsimulations, we demonstrate that the structural flexibility of these\nclusters significantly enhances their catalytic activity. The flexibility\ncoefficient, derived from the full width at half maximum of the Fe–Fe\nradial distribution function, is introduced as a novel descriptor\nfor N<sub>2</sub> bond cleavage. Our findings reveal that flexible\nFe clusters adaptively modify their structures during the reaction\nprocess, lowering energy barriers for N<sub>2</sub> activation and\nsubsequent hydrogenation. This study opens new avenues for designing\nadvanced catalytic systems based on structural flexibility to meet\nthe growing demand for sustainable and energy-efficient ammonia production.