Tetracycline removal via adsorption and metal-free catalysis with 3D macroscopic N-doped porous carbon nanosheets: Non-radical mechanism and degradation pathway |
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Authors: | Yaqian Shen Ke Zhu Dongdong He Jin Huang Hongmei He Lele Lei Wenjin Chen |
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Institution: | School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China |
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Abstract: | Recently,metal-based carbon materials have been verified to be an effective persulfate acti-vator,but secondary pollution caused by metal leaching is inevitable.Hence,a green metal-free 3D macroscopic N-doped porous carbon nanosheets (NPCN) was synthesized success-fully.The obtained NPCN showed high adsorption capacity of tetracycline (TC) and excellent persulfate (PS) activation ability,especially when calcined at 700 ℃ (NPCN-700).The maxi-mum 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 adsorp-tion 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.More-over,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 102.More importantly,the C =O groups,defects and Graphitic N acted as active sites to generate 102.Correspondingly,electrochemical mea-surement 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 degrada-tion capabilities. |
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Keywords: | 3D macroscopic N-doped porous carbon nanosheets Tetracycline Adsorption and metal-free catalysis Singlet oxygen |
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