Spin-Polarized Oxygen Evolution Reaction Enabled by Chiral Molecules Coupled with Ferromagnetic Electrocatalysts

Journal Article · Thu Dec 11 00:00:00 EST 2025 · ACS Applied Materials & Interfaces

DOI:https://doi.org/10.1021/acsami.5c18273· OSTI ID:3014969

He, Fan ^[1]; Gillette, Eleanor ^[1]; Wang, Xingxing ^[1]; Huxford, Aila ^[1]; Xiao, Chuanxiao ^[2]; Yan, Yong ^[1]; Beard, Matthew ^[3]; Gu, Jing ^[1]

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1. San Diego State University
2. Ningbo Institute of Industrial Technology
3. National Laboratory of the Rockies, Golden, CO (United States)

The discovery of chirality-induced spin selectivity (CISS) revolutionized our understanding of the capabilities of chiral molecules, revealing that chiral molecules can function as spin filters, aligning the spin orientation of electrons when they transmit through them. Recently, CISS has been exploited to direct energy conversion, especially the oxygen evolution reaction (OER). However, despite the remarkable progress that has been achieved, the effect of CISS in influencing the intermediate species formation and changing the rate-determining step (RDS) is still vague. To understand those key reaction mechanism steps, electrocatalysts with distinct magnetic characteristics, ferromagnetic CoFe2O4 and paramagnetic Co3O4, were synthesized. The results show that spin-polarized charge carriers retain their spin alignment when coupled with ferromagnetic CoFe2O4, akin to the behavior observed under a magnetic field. The Tafel analysis and kinetic isotope studies (kinetic isotope effect) suggest that in the absence of chiral molecules, the initial electron transfer step, the formation of O* species, governs the rate-determining step (RDS). However, introducing chiral molecules shifts the RDS to a combination of the first and second electron transfers, leading to the formation of OOH*. This conclusion was further supported by in situ infrared spectroscopy, which shows that l-methionine-modified CoFe2O4 (l-CoFe2O4) promotes the formation of OOH*, a key intermediate for O2 generation. This study highlights the critical role of CISS in affecting the OER mechanism and intermediate species formation.

• Research Organization: National Laboratory of the Rockies (NLR), Golden, CO (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES)
• DOE Contract Number: AC36-08GO28308
• OSTI ID: 3014969
• Report Number(s): NLR/JA-5F00-94442
• Journal Information: ACS Applied Materials & Interfaces, Journal Name: ACS Applied Materials & Interfaces Journal Issue: 51 Vol. 17
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
74 ATOMIC AND MOLECULAR PHYSICS
chirality-induced spin selectivity
electrocatalysis
ferromagnetic and paramagnetic compounds
spin-polarized reactions
water oxidation reaction