A simple descriptor for the nitrogen reduction reaction over single atom catalysts

Abstract

The performance of supported catalysts is largely decided by metal-support interactions, which is of great significance for the rational design of catalysts. However, how to quantify the structure-activity relationship of supported catalysts remains a great challenge. In this work, taking MoS₂ and WS₂ supported single atom catalysts (SACs) as prototypes, a simple descriptor, namely, effective d electron number (labeled as <i>Φ</i>), is constructed to quantitatively describe the effect of metal-support interaction on the nitrogen reduction reaction (NRR) activity. This descriptor merely consists of intrinsic properties of the catalyst (including the number of d electrons, electronegativity of the metal atoms and generalized electronegativity of the substrate atoms) and can accurately predict the limiting potential (<i>U</i>_L) for the NRR, with no need for any density functional theory calculations. Moreover, this descriptor possesses superb expansibility that can be applied to other materials, including other metal dichalcogenide (MoSe₂, MoTe₂, WSe₂, WTe₂ and NbS₂) and even MXene (V₂CO₂, Ti₂CO₂ and Nb₂CO₂)-supported SACs. On this basis, a fast screening of excellent NRR catalysts among these systems is performed and three promising NRR catalysts (<i>i.e.</i> Mo@WTe₂, Mo@V₂CO₂ and Re@NbS₂) are successfully selected with <i>U</i>_L as low as -0.32, -0.24 and -0.31 V, respectively. This work offers new opportunities for advancing the rapid discovery of high-efficiency NRR catalysts, and the design principle is expected to be widely applicable to other catalytic systems and beyond.