Non-bonding interaction of dual atom catalysts for enhanced oxygen reduction reaction

Mohsen Tamtaji, Qiuming Peng, Tongchao Liu, Xue Zhao, Zhihang Xu, Patrick Ryan Galligan, Md Delowar Hossain, Zhenjing Liu, Hoilun Wong, Hongwei Liu, Khalil Amine, Ye Zhu, William A. Goddard, Wenting Wu, Zhengtang Luo

Research output: Journal article publicationJournal articleAcademic researchpeer-review

20 Citations (Scopus)


We demonstrate the design of graphene-supported dual atom catalysts (DACs) for the four-electron oxygen reduction reaction (ORR), by utilizing the non-bonding interaction of counterpart metals (M) that synergistically tune the electronic properties and catalytic activity of the Fe active site in FeMN6-DAC and FeMN8-DAC systems, where M stands for Fe, Co, Ni, Cu, and Zn. More specifically, for Fe-M distances below 15 Å, the non-bonding interaction is significant, making the system act as the DAC. We predicted that FeNiN6-DAC and FeNiN8-DAC exhibit a low ORR overpotential (ηORR) of 0.28 V and 0.47 V, respectively, which are at the summits of volcano plots. This low ηORR originates from the high Bader charge transfer coupled with high spin density at the Fe site in both the FeNiN6-DAC and FeNiN8-DAC systems, which weakens the adsorption of OH* intermediate while enhancing its desorption to H2O. Guided by these density functional theory (DFT) computational results, we synthesized FeCoN8-DAC and FeNiN8-DAC along with N-doped graphene and confirmed their structures with scanning transmission electron microscopy (STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption near-edge structure (XANES), extended X-ray absorption fine structure (EXAFS), and electron spin resonance (ESR). We verify experimentally the catalytic activities and find that FeNiN8-DAC has the low experimental overpotential of 0.39 V with a Tafel slope of 47 mVdec−1. Based on these results, we propose a DFT-guided strategy to tune the charge transfer and spin population of the active site toward designing DACs for electrochemical ORR.

Original languageEnglish
Article number108218
JournalNano Energy
Publication statusPublished - Apr 2023


  • Descriptor
  • DFT
  • Electrocatalyst
  • Overpotential
  • Spin state

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • General Materials Science
  • Electrical and Electronic Engineering


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