Tuning nitrogen reduction reaction activity via controllable Fe magnetic moment: A computational study of single Fe atom supported on defective graphene. (10th September 2018)

• Record Type: Journal Article
• Authors: Guo, Xiangyu; Huang, Shiping
• Is Part Of: Electrochimica acta. Volume 284(2018)
• Page Start: 392
• Page End: 399
• Publication Date: 2018-09-10
• Subjects: Single-atom catalyst -- Nitrogen reduction reaction -- Electrochemical mechanisms -- Density functional theory; Electrochemistry -- Periodicals; Electrochemistry, Industrial -- Periodicals; 541.37
• DOI: 10.1016/j.electacta.2018.07.168
• Languages: English
• ISSNs: 0013-4686

Abstract

Abstract: The design and development of low-cost and highly efficient electrocatalysts for nitrogen reduction reaction is crucial for NH3 synthesis. Herein, by means of comprehensive density functional theory (DFT) calculations and thermodynamic analysis, the catalytic mechanisms of N2 to NH3 conversion on single Fe atom embedded in single vacancy and N-doped graphene are systematically investigated. Significantly, the magnetic moment of Fe atom varies with the coordination of neighboring N atom. An approximately linear scaling is found between the adsorption energy of N atom ( Δ E N* ) and Fe magnetic moment. The increased magnetic moment of Fe atom can strengthen the ΔE N*, and promote the charge transfer between the N2 molecule and substrates, resulting in a substantially lower overpotential for N2 electroreduction. Our results highlight an important role of Fe magnetism in N2 activation, which offers a novel strategy for inspiring the rational design of highly efficient carbon-based materials for N2 fixation and conversion. Graphical abstract: Image 1 Highlights: The catalytic performances of carbon-based Fe single-atom catalysts for nitrogen electroreduction are systematically investigated. A linear relation between the adsorption energy of N atom and the Fe magnetic moment is revealed. The magnetic moment of the supported Fe atom plays an important role in N2 activation.