Single-atom transition metal supported on B-doped g-C3N4 monolayer for electrochemical nitrogen reduction

IF 2.9 3区化学 Q3 CHEMISTRY, PHYSICAL

Physical Chemistry Chemical Physics Pub Date : 2024-12-18 DOI:10.1039/d4cp03247k

Huadou Chai, Weiguang Chen, Yi Li, Mingyu Zhao, Jinlei Shi, Yanan Tang, Xianqi Dai

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引用次数: 0

Abstract

Electrochemical reduction of the naturally abundant nitrogen (N2) under ambient conditions is a promising way of ammonia (NH3) synthesis, while the development of a highly active, stable and low-cost catalyst is a challenge for it. Herein, the N2 reduction reaction of TM@g-BC3N4 in electrochemical nitrogen reduction has been systematically investigated by density functional theory (DFT) calculation and compared with that of TM@g-C3N4. It was found that TM atoms are more stable anchored to g-BC3N4 than g-C3N4. The adsorption free energy of N2 molecule on Fe@g-BC3N4 has the greatest change compared with that on Fe@g-C3N4, decreasing by 1.08 eV. The spin charge density around the Fe atom in Fe@g-BC3N4 increases significantly compared with that in Fe@g-C3N4, and the total magnetic moment of the system increases by 3.26 μB. The limiting potential (-0.57 V) of Fe@g-BC3N4 in nitrogen reduction is decreased by 0.06 V compared with that of Fe@g-C3N4 (-0.63 V), and the desorption free energy of ammonia molecules decreases from 1.72 eV to 0.46 eV. Fe atom has higher catalytic activity, ammonia molecule is easier to desorption, nitrogen reduction performance is better. This provides an important reference for the application of g-C3N4-based single atom catalyst in the field of nitrogen reduction.

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支持 B 掺杂 g-C3N4 单层的单原子过渡金属用于电化学氮还原

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来源期刊

Physical Chemistry Chemical Physics 化学-物理：原子、分子和化学物理

CiteScore

5.50

自引率

9.10%

发文量

2675

审稿时长

2.0 months

期刊介绍： Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.