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Phosphorus doping to enhance the peroxymonosulfate activation efficiency of carbon nitride for degrading tetracycline
Journal of Water Process Engineering ( IF 6.3 ) Pub Date : 2023-06-16 , DOI: 10.1016/j.jwpe.2023.103916
Liquan Wang , Ruyi Li , Yimin Zhang , Baohua Tu , Yuan Zhao , Ting Chen , Yuexiang Gao

Herein, a new type of peroxymonosulfate (PMS) activator—phosphorus-doped carbon nitride (P-C3N4)—was prepared using a one-step thermal shrinkage method. Material characterisation confirmed the successful doping of phosphorus in graphite-phase carbon nitride (g-C3N4) by replacing the carbon atoms in its triazine ring structure to form Psingle bondN bonds. Phosphorus doping can regulate and re-organise the surface electronic structure of g-C3N4 without changing its structure. Moreover, phosphorus doping promotes varying degrees of optimisation of the g-C3N4 pore structure and electronic transport between the g-C3N4 sites. Batch experiments on tetracycline (TC) degradation revealed that 0.2 P-C3N4 showed the best physicochemical properties, the constructed P-C3N4/PMS system exhibited high TC removal efficiency and P-C3N4 exhibited good reusability and structural stability. Quenching experiments and electron paramagnetic resonance tests revealed that singlet oxygen was the primary active species in the P-C3N4/PMS system. The mechanism of PMS activation using P-C3N4 was then proposed. The analysis of TC and its intermediate products using liquid chromatography–mass spectroscopy demonstrated that TC was primarily degraded via ring-opening, hydroxylation, deamination and dealkylation reactions. Analysis using the toxicity estimation software tool demonstrated that most intermediate products were less toxic than TC. Thus, this study provides a feasible method for removing TC from aquatic environments.



中文翻译:

磷掺杂提高氮化碳降解四环素的过一硫酸盐活化效率

在此,采用一步热收缩法制备了一种新型过一硫酸盐(PMS)活化剂——磷掺杂氮化碳(PC 3 N 4 )。材料表征证实,通过取代三嗪环结构中的碳原子形成 P N 键,成功地将磷掺杂到石墨相氮化碳 (gC 3 N 4 ) 中。磷掺杂可以在不改变gC 3 N 4单键结构的情况下调节和重组其表面电子结构。此外,磷掺杂促进了gC 3 N 4孔结构和gC 3之间电子传输不同程度的优化。N 4 个站点。批量降解四环素(TC)实验表明,0.2 PC 3 N 4表现出最好的理化性质,构建的PC 3 N 4 /PMS系统表现出较高的TC去除效率,PC 3 N 4表现出良好的可重复使用性和结构稳定性。淬火实验和电子顺磁共振测试表明单线态氧是PC 3 N 4 /PMS体系中的主要活性物质。使用 PC 3 N 4激活 PMS 的机制然后被提议。使用液相色谱-质谱法对TC及其中间产物进行分析表明,TC主要通过开环、羟基化、脱氨和脱烷基反应进行降解。使用毒性估计软件工具进行的分析表明,大多数中间产品的毒性低于原药。因此,本研究为去除水生环境中的TC提供了一种可行的方法。

更新日期:2023-06-20
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