Abstract

Nitrate (NO3−) is a ubiquitous contaminant in water and wastewater. Conventional treatment processes such as adsorption and membrane separation suffer from low selectivity for NO3− removal, causing high energy consumption and adsorbents usage. In this study, we demonstrate selective removal of NO3− in an electrosorption process by a thin, porous carbonized eggshell membrane (CESM) derived from eggshell bio-waste. The CESM possesses an interconnected hierarchical pore structure with pore size ranging from a few nanometers to tens of micrometers. When utilized as the anode in an electrosorption process, the CESM exhibited strong selectivity for NO3− over Cl−, SO42−, and H2PO4−. Adsorption of NO3− by the CESM reached 2.4 × 10−3 mmol/m2, almost two orders of magnitude higher than that by activated carbon (AC). More importantly, the CESM achieved NO3−/Cl− selectivity of 7.79 at an applied voltage of 1.2 V, the highest NO3−/Cl− selectivity reported to date. The high selectivity led to a five-fold reduction in energy consumption for NO3− removal compared to electrosorption using conventional AC electrodes. Density function theory calculation suggests that the high NO3− selectivity of CESM is attributed to its rich nitrogen-containing functional groups, which possess higher binding energy with NO3− compared to Cl−, SO42−, and H2PO4−. These results suggest that nitrogen-rich biomaterials are good precursors for NO3− selective electrodes; similar chemistry can also be used in other materials to achieve NO3− selectivity.

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