High-Throughput Screening of Synergistic Transition Metal Dual-Atom Catalysts for Efficient Nitrogen Fixation.

Lv, Xingshuai; Wei, Wei; Huang, Baibiao; Dai, Ying; Frauenheim, Thomas · Nano Lett · 2021

basic_science · Level V

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Abstract

Great enthusiasm in single-atom catalysts (SACs) for the nitrogen reduction reaction (NRR) has been aroused by the discovery of metal-N<sub><i>x</i></sub> as a promising catalytic center. However, the poor activity and low selectivity of available SACs are far away from the industrial requirement. Through the first-principles high-throughput screening, we find that Fe-Fe distributed on graphite carbon nitride (Fe<sub>2</sub>/<i>g</i>-CN) can manipulate the binding strength of the target reaction species (compromises the ability to adsorb N<sub>2</sub>H and NH<sub>2</sub>), therefore achieving the best NRR performance among 23 transition metal (TM) centers. Our results show that Fe<sub>2</sub>/<i>g</i>-CN achieves a high theoretical Faradaic efficiency of 100% and, impressively, the lowest limiting potential of -0.13 V. Particularly, multiple-level descriptors shed light on the origin of NRR activity, achieving a fast prescreening among various candidates. Our predictions not only accelerate discovery of catalysts for ammonia synthesis but also contribute to further elucidate the structure-performance correlations.