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PreprintCC BYChemRxiv

Ligand Design Principles Enabling High Efficiency Aqueous Iron Electrodeposition at Ambient Temperature

  • Jiang Luo1,2,3
  • Shivam Singh1,2,4
  • Yawei Gao1,2,5,6
  • Huong Nguyen1,2,7
  • Saurabh N. Misal1,2,4,8
  • Xingyi Lyu1,2,7
  • Benjamin Ketter1,2,3,9,10
  • Donghyeon Kang1,2,8
  • Lei Cheng1,2,5,6
  • Tao Li1,2,7,11
  • Jordi Cabana1,2,3,4
  • Justin G. Connell1,2,3,9,10
11 affiliations
  1. 1Center for Steel Electrification by Electrosynthesis (C-STEEL
  2. 2Argonne National Laboratory
  3. 3Materials Science Division
  4. 4University of Illinois Chicago
  5. 5Chemical Sciences Division
  6. 6Oak Ridge National Laboratory
  7. 7Northern Illinois University
  8. 8Applied Materials Division
  9. 9Pritzker School of Molecular Engineering
  10. 10University of Chicago
  11. 11Virginia Polytechnic Institute and State University
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Abstract

Aqueous iron electrodeposition is an attractive route to enabling lower temperature, more modular ironmaking compared to conventional blast furnaces, but existing approaches require extreme pH, elevated temperatures and exhibit low Faradaic efficiency (FE) at elevated current density. A central challenge is the lack of design rules linking electrolyte chemistry to Fe2+ stability, FE and deposit purity. Here we demonstrate that pH-dependent electrolyte stability follows a volcano-type dependence on ligand functional group chemistry that is governed by a competition between metal–ligand complexation and ligand–solvent interactions. We determine α/β-hydroxycarboxylates optimize this balance and identify glycolate as a highly efficient coordinating ligand – enabling dense, ~99% pure iron deposits with >90% FE at thicknesses >100 μm and current densities approaching 1 A cm-2 under benign operating conditions (25ºC and pH 3.5). More broadly, these molecular design principles provide a framework for aqueous electrolyte development that should be transferrable to other electrochemical metal production processes.

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Cite

BibTeXRIS
BibTeX
@misc{luo2026ligand,
  title = {{Ligand Design Principles Enabling High Efficiency Aqueous Iron Electrodeposition at Ambient Temperature}},
  author = {Jiang Luo and Shivam Singh and Yawei Gao and Huong Nguyen and Saurabh N. Misal and Xingyi Lyu and Benjamin Ketter and Donghyeon Kang and Lei Cheng and Tao Li and Jordi Cabana and Justin G. Connell},
  howpublished = {ChemRxiv},
  year = {2026},
  month = oct,
  doi = {10.26434/chemrxiv.15010003/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010003/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Ligand Design Principles Enabling High Efficiency Aqueous Iron Electrodeposition at Ambient Temperature
AU  - Jiang Luo
AU  - Shivam Singh
AU  - Yawei Gao
AU  - Huong Nguyen
AU  - Saurabh N. Misal
AU  - Xingyi Lyu
AU  - Benjamin Ketter
AU  - Donghyeon Kang
AU  - Lei Cheng
AU  - Tao Li
AU  - Jordi Cabana
AU  - Justin G. Connell
PY  - 2026
DA  - 2026/10/06
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15010003/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010003/v1
AB  - Aqueous iron electrodeposition is an attractive route to enabling lower temperature, more modular ironmaking compared to conventional blast furnaces, but existing approaches require extreme pH, elevated temperatures and exhibit low Faradaic efficiency (FE) at elevated current density. A central challenge is the lack of design rules linking electrolyte chemistry to Fe2+ stability, FE and deposit purity. Here we demonstrate that pH-dependent electrolyte stability follows a volcano-type dependence on ligand functional group chemistry that is governed by a competition between metal–ligand complexation and ligand–solvent interactions. We determine α/β-hydroxycarboxylates optimize this balance and identify glycolate as a highly efficient coordinating ligand – enabling dense, ~99% pure iron deposits with >90% FE at thicknesses >100 μm and current densities approaching 1 A cm-2 under benign operating conditions (25ºC and pH 3.5). More broadly, these molecular design principles provide a framework for aqueous electrolyte development that should be transferrable to other electrochemical metal production processes.
ER  -