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

Junjie Li,Mohammad Norouzi Banis,Duojie Wu,Xueliang Sun,Meng Gu,Tsun-Kong Sham,Keegan R Adair,Jun Li,Ya-Fei Jiang,Debora Motta Meira,Ning Chen,Cong-Qiao Xu,Lei Zhang,Weihan Li,Y Zou Finfrock,Kieran Doyle-Davis,Qi Wang,Ruying Li

doi:10.1038/s41467-021-27143-5

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.

Highlights

Single-atom catalysts (SACs) have been applied in many fields due to their superior catalytic performance
We show that this synthesis strategy is general and can be extended to achieve Fe and Ni SACs
After performing one cycle of Pt Atomic layer deposition (ALD) on N-doped carbon nanosheet (NCNS), well-dispersed Pt single atoms were confirmed by HAADF-STEM (Supplementary Fig. 2) and X-ray absorption spectroscopy (XAS) results (Supplementary Fig. 3)[36]

Summary

Introduction

Single-atom catalysts (SACs) have been applied in many fields due to their superior catalytic performance. Pt single atoms on N-doped carbon nanosheets (Pt1/NCNS) as the catalyst to synthesize Co SAC through ALD. The NCNS substrate shows high potential for the synthesis of SACs. After performing one cycle of Pt ALD on NCNS, well-dispersed Pt single atoms were confirmed by HAADF-STEM (Supplementary Fig. 2) and XAS results (Supplementary Fig. 3)[36].

Results

Conclusion