A general strategy for preparing pyrrolic-N4 type single-atom catalysts via pre-located isolated atoms

Junjie Li, Ya-fei Jiang, Qi Wang, Cong-Qiao Xu, Duojie Wu, Mohammad Norouzi Banis, Keegan R. Adair, Kieran Doyle-Davis, Debora Motta Meira, Y. Zou Finfrock, Weihan Li, Lei Zhang, Tsun-Kong Sham, Ruying Li, Ning Chen (), Meng Gu (), Jun Li () and Xueliang Sun ()
Additional contact information
Junjie Li: University of Western Ontario
Ya-fei Jiang: Southern University of Science and Technology
Qi Wang: Southern University of Science and Technology
Cong-Qiao Xu: Southern University of Science and Technology
Duojie Wu: Southern University of Science and Technology
Mohammad Norouzi Banis: University of Western Ontario
Keegan R. Adair: University of Western Ontario
Kieran Doyle-Davis: University of Western Ontario
Debora Motta Meira: Science Division, Canadian Light Source Inc.
Y. Zou Finfrock: Science Division, Canadian Light Source Inc.
Weihan Li: University of Western Ontario
Lei Zhang: University of Western Ontario
Tsun-Kong Sham: University of Western Ontario
Ruying Li: University of Western Ontario
Ning Chen: Science Division, Canadian Light Source Inc.
Meng Gu: Southern University of Science and Technology
Jun Li: Southern University of Science and Technology
Xueliang Sun: University of Western Ontario

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Single-atom catalysts (SACs) have been applied in many fields due to their superior catalytic performance. Because of the unique properties of the single-atom-site, using the single atoms as catalysts to synthesize SACs is promising. In this work, we have successfully achieved Co1 SAC using Pt1 atoms as catalysts. More importantly, this synthesis strategy can be extended to achieve Fe and Ni SACs as well. X-ray absorption spectroscopy (XAS) results demonstrate that the achieved Fe, Co, and Ni SACs are in a M1-pyrrolic N4 (M= Fe, Co, and Ni) structure. Density functional theory (DFT) studies show that the Co(Cp)2 dissociation is enhanced by Pt1 atoms, thus leading to the formation of Co1 atoms instead of nanoparticles. These SACs are also evaluated under hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), and the nature of active sites under HER are unveiled by the operando XAS studies. These new findings extend the application fields of SACs to catalytic fabrication methodology, which is promising for the rational design of advanced SACs.

Date: 2021
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DOI: 10.1038/s41467-021-27143-5

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