High-throughput screening of highly active and selective single-atom catalysts for ammonia synthesis on WB2 (001) surface

Efficient nitrogen reduction reaction (NRR) under mild conditions remains a long-standing challenge. Single -atom catalysts (SACs) with high utilization, selectivity, and activity have cut a great splash in past years. Here, we showed four (B-1, B-2, W-1, and W-2 terminated) WB2 (001) surfaces are promising alternative sup-ports for low-cost transition metal (TM) SACs toward NRR. After the density-functional-theory (DFT) high -throughput screening, the results show that the single Cr atoms anchored on site 1 of W-1 and W-2 termina-tions serve as the most active catalytic center among all TMs, the limiting potentials of Cr@(W-1@1) and Cr@ (W-2@1) are only-0.28 V and-0.37 V, respectively. Besides, the single V atom anchored on B-1@3 and single Mn atoms anchored on B-2@3 shows the best NRR performances. The limiting potentials of V@(B-1@3) and Mn@(B-2@3) are only around-0.19 V and-0.28 V, respectively. What's more, the excellent selectivities of Cr@ (W-1@1), Cr@(W-1@1), V@(B-1@3), and Mn@(B-2@3) to NRR were further confirmed. This work proposes new single atom-substrate pairs and offers systematical insights into the design scheme for high-efficient NH3 production on WB2 (001) surfaces-supported SACs.

Automated summary

This study demonstrates that four WB2 (001) surfaces can be promising alternative supports for low-cost transition metal SACs in nitrogen reduction reaction (NRR). The optimal active centers of single atom catalysts anchored on different surface positions are identified by density-functional-theory high-throughput screening, and their excellent selectivities in NRR are confirmed.