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Spin-Modulated O₂ Adsorption on Surface-Constructed Metal-Organic Chains.

Yuxuan Lin^1,2, Jinliang Pan¹, Zhiyu Wang³

¹BNLMS, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.

Journal of the American Chemical Society

|January 14, 2026

Summary

This study reveals that high-spin nickel centers preferentially adsorb oxygen molecules compared to low-spin centers. This spin selectivity in oxygen adsorption is crucial for understanding catalytic processes.

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Area of Science:

Surface Science
Catalysis
Quantum Chemistry

Background:

Oxygen adsorption is critical for many catalytic reactions.
The role of catalyst spin states in O2 adsorption mechanisms is not fully understood.
Understanding these mechanisms requires atomic-scale insights.

Purpose of the Study:

To investigate the atomic-scale mechanisms of oxygen adsorption on nickel centers with different spin states.
To compare the O2 affinity of high-spin (NiH) and low-spin (NiL) nickel centers.
To elucidate the influence of electronic structure on selective O2 binding.

Main Methods:

Scanning tunneling microscopy/spectroscopy (STM/STS) for atomic-scale characterization.
Atomic force microscopy (AFM) for comparative analysis.
Density functional theory (DFT) calculations to model electronic interactions.

Main Results:

Direct observation of preferential O2 adsorption at NiH compared to NiL centers.
DFT confirms selectivity originates from distinct d-electron configurations and O2-Ni hybridization.
O2 adsorption at NiH can induce a spin transition in NiL, potentially hindering binding.

Conclusions:

Nickel spin state critically dictates O2 adsorption selectivity at the atomic level.
Microscopic insights into spin-modulated O2 adsorption are provided.
Findings advance the understanding of spin-dependent catalysis.