posted on 2024-01-23, 18:47authored byMingxin Qin, Lanlan Chen, Wenhua Zhang, Jinlong Yang
The catalytic activity of single-atom catalysts (SACs)
is crucially
affected by the actual ligand configurations under the reaction condition;
thus, carefully considering the reaction condition is crucial for
the theoretical design of SACs. With single metal atoms supported
by g-C3N4 as a model system, a self-consistent
screening framework is proposed for the theoretical design of SACs
with respect to the nitrogen reduction reaction (NRR). Pourbaix diagrams
are constructed on the basis of various co-adsorption configurations
of N2, H, and OH. Possible stable configurations containing
N2 under the expected reaction condition are considered
to obtain the limiting potential of NRR, and the stability of the
configuration at the calculated UL is
rechecked. With this framework, AC stacking of double-layer g-C3N4-supported Nb and AA stacking and AB stacking
of double-layer g-C3N4-supported W are predicted
to exhibit superior NRR activity with UL values of −0.36, −0.45, and −0.52 V, respectively.
This procedure can be widely applied to the screening of SACs for
electrocatalytic reactions.