Single and double transition metal atoms doped graphdiyne for highly efficient electrocatalytic reduction of nitric oxide to ammonia

[Display omitted] •The NO reduction to NH3 process is constrained by thermodynamic processes on single-atom catalysts (SACs) and electrochemical processes on double-atom catalysts (DACs).•Single Cu atom doped graphdiyne (Cu@GDY) exhibits the optimal NORR catalytic activity with the lowest thermodyna...

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Published in:	Journal of colloid and interface science Vol. 656; pp. 155 - 167
Main Authors:	Wu, Yuting, Lv, Jiarui, Xie, Fengjing, An, RunZhi, Zhang, Jiaojiao, Huang, Hong, Shen, Zhangfeng, Jiang, Lingchang, Xu, Minhong, Yao, Qiufang, Cao, Yongyong
Format:	Journal Article
Language:	English
Published:	United States Elsevier Inc 15-02-2024
Subjects:	Ammonia (NH3) Density functional theory (DFT) Double atom catalysts (DACs) Nitric oxide (NO) Single atom catalysts (SACs) Double atom catalysts (DACs) Ammonia (NH3) Single atom catalysts (SACs) Nitric oxide (NO) Density functional theory (DFT) Ammonia (NH)
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Summary:	[Display omitted] •The NO reduction to NH3 process is constrained by thermodynamic processes on single-atom catalysts (SACs) and electrochemical processes on double-atom catalysts (DACs).•Single Cu atom doped graphdiyne (Cu@GDY) exhibits the optimal NORR catalytic activity with the lowest thermodynamic energy barriers of 0.10 eV.•A catalytic activity relationship is established between the d-band centers of the SACs, DACs and NORR performance.•Thermodynamic and electrochemical processes of NORR are regulated by d-band center of catalysts. The electrocatalytic conversion of nitric oxide (NORR) to ammonia (NH3) represents a pivotal approach for sustainable energy transformation and efficient waste utilization. Designing highly effective catalysts to facilitate the conversion of NO into NH3 remains a formidable challenge. In this work, the density functional theory (DFT) is used to design NORR catalysts based on single and double transition metal (TM:Fe, Co, Ni and Cu) atoms supported by graphdiyne (TM@GDY). Among eight catalysts, the Cu2@GDY is selected as a the most stable NORR catalyst with high NH3 activity and selectivity. A pivotal discovery underscores that the NORR mechanism is thermodynamically constrained on single atom catalysts (SACs), while being governed by electrochemical processes on double atom catalysts (DACs), a distinction arising from the different d-band centers of these catalysts. Therefore, this work not only introduces an efficient NORR catalyst but also provides crucial insights into the fundamental parameters influencing NORR performance.
Bibliography:	ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23
ISSN:	0021-9797 1095-7103
DOI:	10.1016/j.jcis.2023.11.053