Electrochemical nitrogen reduction reaction on anchored SnS2 nanosheets with TM2 dimers

Abstract

The design of efficient, high-stability nitrogen fixation catalysts remains a great challenge to achieve electrochemical nitrogen reduction reaction (NRR) under ambient conditions. Herein, the high-throughput first-principles calculations are performed to obtain potential electrochemical NRR catalysts from transition metal (TM) dimers anchored on SnS₂ nanosheets. The selected W₂/SnS₂ behaves as a promising NRR candidate possessing -0.27 V limiting potential and 0.81 eV maximum kinetic potential, and it exhibits the adsorption advantages of *N₂ over other small molecules (*H₂O, *O, *OH, *H). More importantly, the moderate d orbital valence electron number and electronegativity of TM atom could obtain better NRR activity, and a new descriptor φ considering the effects of coordination environments and adsorbates is proposed to achieve the fast pre-screening among various candidates. This work presents practical insights into the fast screening of TM₂/SnS₂ candidates for efficient nitrogen fixation and further streamlining the design of electrochemical NRR catalysts.

Keywords: Density functional theory; High-throughput screening; Nitrogen reduction reaction; SnS(2) nanosheets; TM(2) dimers.