Tetracycline removal via adsorption and metal-free catalysis with 3D macroscopic N-doped porous carbon nanosheets: Non-radical mechanism and degradation pathway

Recently, metal-based carbon materials have been verified to be an effective persulfate activator, but secondary pollution caused by metal leaching is inevitable. Hence, a green metalfree 3D macroscopic N-doped porous carbon nanosheets (NPCN) was synthesized successfully. The obtained NPCN showed high adsorption capacity of tetracycline (TC) and excellent persulfate (PS) activation ability, especially when calcined at 700 degrees C (NPCN-700). The maximum adsorption capacity of NPCN-700 was 121.51 mg/g by H-bonds interactions. Moreover, the adsorption process followed pseudo-second-order kinetics model and Langmuir adsorption isotherm. The large specific surface area (365.27 mg/g) and hierarchical porous structure of NPCN-700 reduced the mass transfer resistance and increased the adsorption capacity. About 96.39% of TC was removed after adding PS. The effective adsorption of the catalyst greatly shortened the time for the target organic molecules to migrate to the catalyst. Moreover, the NPCN-700 demonstrated high reusability with the TC removal rate of 80.23% after 4 cycles. Quenching experiment and electron paramagnetic resonance (EPR) test confirmed the non-radical mechanism dominated by O-1(2). More importantly, the C = O groups, defects and Graphitic N acted as active sites to generate O-1(2). Correspondingly, electrochemical measurement revealed the direct electron transfer pathway of TC degradation. Finally, multiple degradation intermediates were recognized by the LC-MS measurement and three possible degradation pathways were proposed. Overall, the prepared NPCN had excellent application prospects for removal of antibiotics due to its remarkable adsorption and catalytic degradation capabilities. 2021 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.

Automated summary

The green metal-free 3D macroscopic N-doped porous carbon nanosheets (NPCN) demonstrated high adsorption capacity and excellent persulfate activation ability, making it a promising candidate for antibiotic removal.