摘要
We report the theory-guided design of anatase-supported Nb catalysts for electrochemical N 2 reduction reaction (NRR). Theoretical calculations predict that Nb atoms deliver multi-functional enhancement toward the NRR when incorporated in an anatase TiO 2 (110) catalyst: (1) decreasing the band gap and inducing electrons to promote the conductivity of TiO 2 (110); (2) suppressing the undesired competitive hydrogen evolution reaction; (3) activating the inert Ti sites for N 2 adsorption; (4) enabling fast charge transfer between ∗NNH and the TiO 2 (110) surface; and (5) reducing the energy barrier of the potential-determining ∗N 2 → ∗NNH step, further facilitating NH 3 formation. As a result, our Nb-TiO 2 (110) catalyst exhibits superior activity and selectivity for the NRR, which affords an NH 3 production rate of about 21.3 μg h −1 mg cat −1 and NH 3 faradaic efficiency of ∼9.2% at −0.5 V (versus reversible hydrogen electrode). This study provides insights for the rational design of efficient electrocatalysts for the NRR.