N self-doped hierarchically porous carbon derived from biomass as an efficient adsorbent for the removal of tetracycline antibiotics

Abstract

In this study, we developed a simple strategy to synthesize a N self-doped hierarchically porous carbon adsorbent (LPC-NC) derived from biomass using potassium oxalate monohydrate and calcium carbonate and remove tetracyclines that are major antibiotics frequently measured in surface water. In the pyrolysis process, the N-enriching lotus seed pots biomass decomposed and formed a porous carbon matrix with self-doped N. The LPC-NC displayed high adsorption amount (506.6 mg/g for tetracycline (TTC) and 445.3 mg/g for oxytetracycline (OTC)), short equilibrium time (30 min) and stable reusability (the decline efficiency<8.0% after five cycles). Batch adsorption experimental and theoretical studies showed that the high adsorption capacity of LPC-NC for tetracyclines was mainly ascribed to the self-doped pyridinic-N species and the adsorption capacity of pyridinic-N species at the edge location was better than that of pyridinic-N species at the vacancy location. Importantly, we believe that the high adsorption performance of LPC-NC for tetracyclines is due to the activation of carbon π electrons by destroying the integrity of conjugation on LPC-NC, thus enhancing the π-π interaction between LPC-NC and tetracyclines. In addition, the results of solid-state nuclear magnetic resonance (NMR) confirmed that the hierarchically porous structure of LPC-NC was conducive to the adsorption of tetracyclines. These insights provide new ideas for the rational design of N-doped carbon-based adsorbents for the efficient removal of tetracyclines.

Keywords: Adsorption; DFT calculations; N self-doped hierarchically porous adsorbent; Nuclear magnetic resonance (NMR) spectroscopy; Tetracyclines.