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Trifunctional cobalt single-atom catalyst with axial chloride coordination to achieve efficient methylamine electrosynthesis: a constant-potential DFT study
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DOI：10.1039/d6ta01804a.png)
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Abstract
En 中文
Electrochemical methylamine synthesis from nitrate (NO3-) and carbon dioxide (CO2) offers a promising approach for sustainable methylamine production, but progress remains limited due to the sluggish C-N coupling process and the lack of effective catalysts. For this purpose, a system with efficient trifunctionality, i.e., NO3- reduction, CO2 reduction and crucial C-N coupling sites, is essential for efficient methylamine production on single-atom catalysts (SACs). Through a systematic investigation by performing constant-potential density functional theory calculations, axially chlorine-coordinated Co single-atom catalysts anchored on graphene (CoN4(Cl)@G) with outstanding trifunctionality are identified from among a series of TMN4(Cl)@G and TMN4@G (TM = Fe, Co, Ni) systems. Furthermore, a distinct C-N coupling mechanism, namely, the direct coupling of the migration-capable CO species with the *NH2 intermediate to form the key precursor *NH2CO (*NH2-CO -> *NH2CO), is evidenced to be both thermodynamically and kinetically feasible (with a low energy barrier of 0.48 eV). Consequently, this work presents a practical strategy for methylamine synthesis starting from graphene-supported single-atom sites, and also advances mechanistic insight into C-N bond formation.
Keywords:
OXYGEN REDUCTION
MECHANISM
CO2
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9.5
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