@article{Gao2023, 
author = {Ya Gao and Erpeng Wang and Yazhuo Zheng and Jian Zhou and Zhimei Sun},
title = {Hexagonal MBenes-Supported Single Atom as Electrocatalysts for the Nitrogen Reduction Reaction},
year = {2023},
journal = {Energy Material Advances},
volume = {4},
pages = {0039},
url = {https://www.sciopen.com/article/10.34133/energymatadv.0039},
doi = {10.34133/energymatadv.0039},
abstract = {The electrocatalytic nitrogen reduction reaction (NRR) is currently constrained by sluggish reaction kinetics and poor selectivity because of the difficulties in activating inert N≡N triple bonds and the existence of competing hydrogen evolution reaction (HER). Therefore, electrocatalysts with high activity, selectivity, and stability are highly desired. Herein, by means of first-principles calculations, we investigated the electrocatalytic NRR performance of a series of transition metal atoms (e.g., 3d, 4d, and 5d) embedded in defective hexagonal MBene nanosheets [h-Zr(Hf)2B2O2] and identified that h-Zr(Hf)2B2O2 could be an excellent platform for electrocatalytic NRR. On the basis of our proposed screening criteria, 16 candidates are efficiently selected out from 50 systems, among which, Zr2B2O2-Cr stands out with high selectivity to NRR against HER and the ultralow limiting potential (−0.10 V). The value is much lower than that of the well-established stepped Ru(0001) surface (−0.43 V). The origin of the high activity toward NRR is attributed to the synergistic effect of the single atom (SA) and the M atoms in the substrate. More impressively, a composition descriptor is further proposed on the basis of the inherent characteristics of the catalysts [number of valence electrons of SA and electronegativity of the SA and Zr(Hf) atoms], which helps to better predict the catalytic performance. Our work not only contributes to the development of highly efficient NRR electrocatalysts but also extend the application of h-MBenes in electrocatalysis.}
}