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Nitrogen and phosphorus co-doped porous carbons (NPCs) for peroxydisulfate (PDS) activation towards tetracycline degradation: Defects enhanced adsorption and non-radical mechanism dominated by electron transfer
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2022-11-28 , DOI: 10.1016/j.cej.2022.140615
Minxian Cheng , Yichu Zhang , Bo Lai , Lingzhen Wang , ShengjiongYang , Kailong Li , Dongqi Wang , Yaoguo Wu , Guang-Hao Chen , Jin Qian

Nitrogen and phosphorus co-doped porous carbons (NPCs) were successfully prepared by pyrolysis of the mixture of PANI and phytic acid. The synthesized NPCs exhibited excellent degradation abilities to tetracycline (90.34% within 60 mins). Based on the results of quenching experiments and electron paramagnetic resonance (EPR), metastable reactive complexes mediated electron transfer was the major pathway and singlet oxygen (1O2) played an auxiliary role in the TC degradation. Graphitic N, pyridinic N and defects were identified as the catalytic sites. Linear sweep voltammetry, chronoamperometry tests and electrochemical impedance spectroscopy tests revealed that defects as the active sites to form metastable surface-confined reactive species. The density functional theory (DFT) calculations results indicated that the introduction of phosphorus could promote the peroxydisulfate (PDS) adsorption and activation by adjusting the electron density of the carbon skeleton. This study provides new insights into the designation of metal-free PDS activators towards the high-efficiency removal of contaminants.



中文翻译:

用于过二硫酸盐 (PDS) 活化以降解四环素的氮磷共掺杂多孔碳 (NPC):缺陷增强吸附和电子转移主导的非自由基机制

通过热解 PANI 和植酸的混合物成功制备了氮磷共掺杂多孔碳 (NPC)。合成的 NPC 对四环素表现出优异的降解能力(60 分钟内降解 90.34%)。根据猝灭实验和电子顺磁共振 (EPR) 的结果,亚稳态反应复合物介导的电子转移是主要途径,单线态氧 ( 1 O 2) 在 TC 降解中起辅助作用。石墨氮、吡啶氮和缺陷被确定为催化位点。线性扫描伏安法、计时电流法测试和电化学阻抗谱测试表明缺陷作为活性位点形成亚稳态表面限制的活性物质。密度泛函理论(DFT)计算结果表明,磷的引入可以通过调节碳骨架的电子密度来促进过二硫酸盐(PDS)的吸附和活化。这项研究为指定无金属 PDS 活化剂以高效去除污染物提供了新的见解。

更新日期:2022-12-01
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