Boosting electrochemical nitrogen reduction reaction performance of two-dimensional Mo porphyrin monolayers via turning the coordination environment. Issue 7 (15th February 2021)

• Record Type: Journal Article
• Authors: Liu, Shiqiang; Cheng, Zhiwen; Liu, Yawei; Gao, Xiaoping; Tan, Yujia; Ren, Yuanyang; Shen, Zhemin
• Is Part Of: Physical chemistry chemical physics. Volume 23:Issue 7(2021)
• Page Start: 4178
• Page End: 4186
• Publication Date: 2021-02-15
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/d0cp06036d
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : Designing atomically dispersed metal catalysts for the nitrogen reduction reaction (NRR) is an effective approach to achieve better energy conversion efficiencies. Abstract : Designing atomically dispersed metal catalysts for the nitrogen reduction reaction (NRR) is an effective approach to achieve better energy conversion efficiencies. In this study, we designed a series of single molybdenum (Mo) atom-anchored porous two-dimensional Mo porphyrin (2D Mo-Pp) monolayers modified by B, C, O, P and S as efficient NRR catalysts to improve the catalytic performance. We introduced two key parameters, θ (p z orbital filling of heteroatoms) and φ (Bader charge of central Mo atoms). It shows that θ and φ play important roles in nitrogen absorption by analyzing the regression models. In particular, the theoretical results suggested that the 2D Mo-Pp monolayer modified by B has an ultralow limiting potential of 0.35 V and can suppress the hydrogen evolution reaction, making the 2D Mo-Pp monolayer modified by B a promising NRR electrocatalyst with high efficiency and selectivity. This work provides insights into the rational design of the elaborate structure of single-atom catalysts with tunable electrocatalytic activities.