Microbial fuel cells (MFCs) are emerging technology for wastewater treatment by chemical oxygen demand (COD) reduction and simultaneous bioelectricity production. Fabrication of an effective proton exchange membrane (PEM) is a vital component for MFC performance. In this work, green chitosan-based (CS) PEMs were fabricated with graphene oxide (GO) as filler material (CS-GO) and cross-linked with phosphoric acid (CS-GO-P(24)) or sulfuric acid (CS-GO-S(24)) to determine their effect on PEM properties. Interrogation of the physicochemical, thermal, and mechanical properties of the cross-linked CS-GO PEMs demonstrated that ionic cross-linking based on the incorporation of PO groups in the CS-GO mixed-matrix composites, when compared with sulfuric acid cross-linking commonly used in proton exchange membrane fuel cell (PEMFC) studies, generated additional density of ionic cluster domains, rendered enhanced sorption properties, and augmented the thermal and mechanical stability of the composite structure. Consequently, bioelectricity performance analysis in MFC application showed that CS-GO-P(24) membrane produced 135% higher power density than the CS-GO-S(24) MFC system. Simultaneously, 89.52% COD removal of primary clarifier municipal wastewater was achieved in the MFC operated with the CS-GO-P(24) membrane.
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