Controlling solvation in conducting redox polymers for selective electrochemical separation of nitrate from wastewater

Shao-Wei Tsai, Alexandra Zagalskaya, Yurui Li, Ching-Yu Chen, Marcos Felipe Calegari Andrade, Riccardo Candeago, James F. Browning, A. Robert Hillman, Roland D. Cusick, Tuan Anh Pham and Xiao Su ()
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Shao-Wei Tsai: University of Illinois Urbana-Champaign, Department of Chemical and Biomolecular Engineering
Alexandra Zagalskaya: Livermore, Quantum Simulations Group, Materials Science Division, Lawrence Livermore National Laboratory
Yurui Li: University of Illinois Urbana-Champaign, Department of Civil and Environmental Engineering
Ching-Yu Chen: University of Illinois Urbana-Champaign, Department of Chemical and Biomolecular Engineering
Marcos Felipe Calegari Andrade: Livermore, Quantum Simulations Group, Materials Science Division, Lawrence Livermore National Laboratory
Riccardo Candeago: University of Illinois Urbana-Champaign, Department of Chemical and Biomolecular Engineering
James F. Browning: Oak Ridge National Laboratory, Neutron Scattering Division
A. Robert Hillman: University of Leicester, School of Chemistry
Roland D. Cusick: University of Illinois Urbana-Champaign, Department of Civil and Environmental Engineering
Tuan Anh Pham: Livermore, Quantum Simulations Group, Materials Science Division, Lawrence Livermore National Laboratory
Xiao Su: University of Illinois Urbana-Champaign, Department of Chemical and Biomolecular Engineering

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Selective capture of nitrate from wastewater is crucial for ensuring safe drinking water and promoting resource circularity. This study investigated alkylated polyaniline redox polymers as highly-selective electrosorbents to address this challenge. By controlling polymer solvation properties through synthetic functionalization, poly(N-methylaniline) (PNMA) achieves a nitrate uptake of up to 1.38 mmol g−1-polymer and a separation factor of 7 over chloride. Poly(N-butylaniline) (PNBA) further enhances selectivity, achieving a separation factor beyond 14 due to increased hydrophobicity. The mechanisms underlying this selectivity are investigated using ab initio molecular dynamics (AIMD) and in-situ electrochemical quartz crystal microbalance (EQCM) studies, which reveal that hydrophobicity reduces chloride binding. A technoeconomic analysis indicates that methylation on PANI reduces nitrate removal costs by 50% compared to non-functionalized PANI, due to enhanced selectivity and uptake, and decreased energy consumption. PNMA electrodes demonstrate practical nitrate selectivity over 20 versus chloride in real wastewater, while avoiding sulfate binding. This study highlights the potential of controlling solvation at electroactive polymers to enhance nitrate selectivity, offering a promising design path for redox-mediated electrochemical separations.

Date: 2025
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DOI: 10.1038/s41467-025-64895-w

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