Revealing the impact of interlayer structural ordering in graphene confined membranes for efficient water treatment

CK Mao and L Chen and CX Hong and HZ Guo and XD Zhang and J Wang and HY Shao and G Xu, CHEMICAL ENGINEERING JOURNAL, 521, 166801 (2025).

DOI: 10.1016/j.cej.2025.166801

Two-dimensional catalytic membranes achieve efficient water purification technology by leveraging their unique confined structure to enhance reaction efficiency between reactive species and pollutants. However, the influence of ordered interlayer structure in 2D confined membranes on pollutant removal remains unclear. In this study, a series of 2D membranes with varying interlayer ordering degrees were fabricated by vacuum-filtrating GO@Cox nanosheets containing different crystalline layers of GO. Catalytic experiments revealed that membranes with higher interlayer ordering achieved nearly 100 % tetracycline (TC) removal across diverse environments under an ultralow peroxymonosulfate (PMS) dosage (0.025 mM). Electron paramagnetic resonance (EPR) analysis demonstrated that the ordered interlayer structures significantly promoted the conversion of PMS to long-lived singlet oxygen (1O2), thereby improving oxidant utilization efficiency. Through density functional theory and molecular dynamics simulations, we identified that ordered interlayer structures primarily enhance PMS activation efficiency by strengthening electron transfer between GO@Cox and PMS. Simultaneously, the ordered interlayer structures elevate the transmembrane potential energy barrier for pollutants to intensify interactions between reactive species and contaminants, ultimately boosting pollutant removal. This work systematically elucidates the critical role of interlayer structural ordering in governing catalytic water treatment performance of 2D membranes, providing new insights for designing high-performance nanomembrane materials.

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