Details

Autor(en) / Beteiligte

• Zheng, Xiaonan
• Liu, Yang
• Yan, Yu
• Li, Xiaoxiao
• Yao, Yuan

Titel

Modulation effect in adjacent dual metal single atom catalysts for electrochemical nitrogen reduction reaction

Ist Teil von

• Chinese chemical letters, 2022-03, Vol.33 (3), p.1455-1458

Ort / Verlag

Elsevier B.V

Erscheinungsjahr

2022

Link zum Volltext

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Nitrogen reduction reaction (NRR) is a clean mode of energy conversion and the development of highly efficient NRR electrocatalysts under ambient conditions for industrial application is still a big challenge. Metal-nitrogen-carbon (M-N-C) has emerged as a class of single atom catalyst due to the unique geometric structure, high catalytic activity, and clear selectivity. Herein, we designed a series of dual metal single atom catalysts containing adjacent M-N-C dual active centers (MN4/M'N4-C) as NRR electrocatalysts to uncover the structure-activity relationship. By evaluating structural stability, catalytic activity, and selectivity using density functional theory (DFT) calculations, 5 catalysts, such as CrN4/M'N4-C (M’ = Cr, Mn, Fe, Cu and Zn), were determined to exhibit the best NRR catalytic performance with the limiting potential ranging from −0.64 V to −0.62 V. The CrN4 center acted as the main catalytic site and the adjacent M'N4 center could enhance the NRR catalytic activity by modulation effect based on the analysis of the electronic properties including the charge density difference, partial density of states (PDOS), and Bader charge variation. This study offers useful insights on understanding the structure-activity relationship of dual metal single atom catalysts for electrochemical NRR. A series of adjacent dual metal single atom catalysts CrN4/M'N4-C (M’ = Cr, Mn, Fe, Cu and Zn) was selected via systematic density functional theory (DFT) calculations, which exhibit high activity for nitrogen reduction reaction (NRR) due to the modulation effect. [Display omitted]