Unveiling the Spin Regulation of Electrocatalytic Nitrogen Reduction on Fe, Ru and Os-Anchored Nitrogen-Doped Graphene

• 1、Chongqing University, Chongqing 401331

Abstract：The theoretical studies of electrocatalytic nitrogen reduction (NRR) have been widely reported before, but the detailed mechanism of the reaction is still unknown. So far, there are few reports about nitrogen reduction changes caused by different spin states of catalysts, so this work mainly report the coordination of four pyridine N and single metal M (M=Fe, Ru, Os) doped monolayers graphene (MN4C), by changing the spin state, then the nitrogen reduction process was calculated by density functional theory. The results show that changing the spin state of the three different metal catalysts can effectively improve the activation degree of the bottom surface, and improve the stability and activity of the adsorbed nitrogen. The activation energy barrier of catalyst RuN4C for nitrogen reduction through alternating paths is the smallest in the low spin state, its limiting potential is -0.58V. In addition, under different spin states of the same metal, higher spin states can effectively inhibit hydrogen evolution reaction, this above content is expected to contribute to the research of nitrogen reduction reaction.

Keywords： Chemistry electrocatalysis transition metal nitrogen-doped graphene nitrogen reduction reaction