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PreprintCC BYChemRxiv

Fundamental Investigations into the Activity and Stability of Iron-Based Bimetallic Catalysts for the Oxygen Evolution Reaction

  • Shayan Hoseini1
  • Foroogh Khezeli1
  • Ashley Head2
  • Craig Plaisance3
  • Theodore Walker1
  1. 1Syracuse University
  2. 2Brookhaven National Laboratory
  3. 3Louisiana State University
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Abstract

Engineering electrocatalyst resistance to degradation in alkaline media remains a major challenge for developing stable, earth-abundant oxygen evolution reaction (OER) anodes. Here, we combined acid–base titration and X-ray fluorescence to quantify Fe dissolution from a series of bimettalic FexMy (oxy)hydroxides deposited on Fe foils (My = Sn, Hf, Mn, Se) at 1.66–2.11 VRHE, showing that apparently stable current densities and cycle voltametery alone can mask significant electrode degradation. After initial restructuring (~2 h), end-of-life anodes showed steady-state dissolution rates of 0.15–0.67 mgFe cm⁻² h⁻¹ near OER onset (~1.75 VRHE). Across alloys, dissolution rates and OER overpotentials correlated with the Fe–My electronegativity difference. Dissolution rates were highest for those alloys where My was less electronegative than Fe, and XPS revealed a more reduced surface with higher concentrations of hydroxoligands. Spin-polarized DFT+U shows Sn reduces neighboring Fe atoms, shifting the potential-limiting OER step to Fe–O* formation, lowering its formation free energy (consistent with a reduced OER overpotential); but elongating Fe-O bonds (perhaps accelerating dissolution). Generalizing these results toward future work, we suggest that the dissolution resistance of FeOOH surfaces may be controlled by alloy-driven modulation of their protonation state (revealed by XPS) and Fe-O bond character (probed by DFT).

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Cite

BibTeXRIS
BibTeX
@misc{hoseini2026fundamental,
  title = {{Fundamental Investigations into the Activity and Stability of Iron-Based Bimetallic Catalysts for the Oxygen Evolution Reaction}},
  author = {Shayan Hoseini and Foroogh Khezeli and Ashley Head and Craig Plaisance and Theodore Walker},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv-2025-4nzrw/v3},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv-2025-4nzrw/v3},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Fundamental Investigations into the Activity and Stability of Iron-Based Bimetallic Catalysts for the Oxygen Evolution Reaction
AU  - Shayan Hoseini
AU  - Foroogh Khezeli
AU  - Ashley Head
AU  - Craig Plaisance
AU  - Theodore Walker
PY  - 2026
DA  - 2026/09/23
PB  - ChemRxiv
DO  - 10.26434/chemrxiv-2025-4nzrw/v3
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv-2025-4nzrw/v3
AB  - Engineering electrocatalyst resistance to degradation in alkaline media remains a major challenge for developing stable, earth-abundant oxygen evolution reaction (OER) anodes. Here, we combined acid–base titration and X-ray fluorescence to quantify Fe dissolution from a series of bimettalic FexMy (oxy)hydroxides deposited on Fe foils (My = Sn, Hf, Mn, Se) at 1.66–2.11 VRHE, showing that apparently stable current densities and cycle voltametery alone can mask significant electrode degradation. After initial restructuring (~2 h), end-of-life anodes showed steady-state dissolution rates of 0.15–0.67 mgFe cm⁻² h⁻¹ near OER onset (~1.75 VRHE). Across alloys, dissolution rates and OER overpotentials correlated with the Fe–My electronegativity difference. Dissolution rates were highest for those alloys where My was less electronegative than Fe, and XPS revealed a more reduced surface with higher concentrations of hydroxoligands. Spin-polarized DFT+U shows Sn reduces neighboring Fe atoms, shifting the potential-limiting OER step to Fe–O* formation, lowering its formation free energy (consistent with a reduced OER overpotential); but elongating Fe-O bonds (perhaps accelerating dissolution). Generalizing these results toward future work, we suggest that the dissolution resistance of FeOOH surfaces may be controlled by alloy-driven modulation of their protonation state (revealed by XPS) and Fe-O bond character (probed by DFT).
ER  -