TY - JOUR
T1 - Enhanced Proton-Selective Hybrid Polybenzimidazole/Perfluorosulfonic Acid Membranes for Acid Recovery from Lithium Battery Leachate Using Electrodialysis
AU - Golubenko, Daniil
AU - Petukhov, Dmitrii
AU - Al-Juboori, Raed A.
AU - Varghese, Sabu
AU - Johnson, Daniel
AU - Hilal, Nidal
N1 - Publisher Copyright:
© 2025 The Authors. Published by American Chemical Society.
PY - 2025
Y1 - 2025
N2 - Proton-selective membranes present a promising solution for improving the efficiency and sustainability of acid recovery in the hydrometallurgical recycling of lithium-ion batteries (LIBs). This study introduces a hybrid cation exchange membrane developed by in situ modification of a commercial perfluorosulfonic acid (PFSA) membrane with polybenzimidazole (PBI) for efficient acid recovery using electrodialysis (ED). The modified membranes demonstrated exceptional proton selectivity and stability, achieving selectivity ratios of 770 (H+/Li+) and 606 (H+/Co2+), surpassing reported values in the literature. In 150 min of electrodialysis, the optimum membrane composite (PFSA-113_PBI-3%) achieved up to 80% acid recovery from synthetic leachates containing H+, Li+, Mn2+, Co2+, and Ni2+. Outstanding separation factors of up to 86 for H+/Li+ and 104 for H+/d-Metal2+, alongside a current efficiency of 95%, were also obtained with the optimum membrane. The enhanced proton selectivity was attributed to the hydrogen-bond networks and ionic interactions resulting from salt bridges between PBI and polymer acidic groups from the formation of a PBI/PFSA interpolymer complex. This was confirmed through membrane structural analysis using Raman and FTIR spectroscopy, electron microscopy, and small-angle X-ray scattering. The separation mechanism of the modified membrane was found to resemble that of biological membranes, as confirmed through carefully designed methylation tests.
AB - Proton-selective membranes present a promising solution for improving the efficiency and sustainability of acid recovery in the hydrometallurgical recycling of lithium-ion batteries (LIBs). This study introduces a hybrid cation exchange membrane developed by in situ modification of a commercial perfluorosulfonic acid (PFSA) membrane with polybenzimidazole (PBI) for efficient acid recovery using electrodialysis (ED). The modified membranes demonstrated exceptional proton selectivity and stability, achieving selectivity ratios of 770 (H+/Li+) and 606 (H+/Co2+), surpassing reported values in the literature. In 150 min of electrodialysis, the optimum membrane composite (PFSA-113_PBI-3%) achieved up to 80% acid recovery from synthetic leachates containing H+, Li+, Mn2+, Co2+, and Ni2+. Outstanding separation factors of up to 86 for H+/Li+ and 104 for H+/d-Metal2+, alongside a current efficiency of 95%, were also obtained with the optimum membrane. The enhanced proton selectivity was attributed to the hydrogen-bond networks and ionic interactions resulting from salt bridges between PBI and polymer acidic groups from the formation of a PBI/PFSA interpolymer complex. This was confirmed through membrane structural analysis using Raman and FTIR spectroscopy, electron microscopy, and small-angle X-ray scattering. The separation mechanism of the modified membrane was found to resemble that of biological membranes, as confirmed through carefully designed methylation tests.
KW - acid recovery
KW - cation exchange membranes
KW - lithium battery recycling
KW - polybenzimidazole
KW - proton selectivity
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U2 - 10.1021/acsestengg.5c00090
DO - 10.1021/acsestengg.5c00090
M3 - Article
AN - SCOPUS:105004462022
SN - 2690-0645
JO - ACS ES and T Engineering
JF - ACS ES and T Engineering
ER -