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用于增强可见光辅助过硫酸盐活化降解舒必利的超薄 S 掺杂石墨相氮化碳纳米片:性能与机制。

Ultrathin S-doped graphitic carbon nitride nanosheets for enhanced sulpiride degradation via visible-light-assisted peroxydisulfate activation: Performance and mechanism.

机构信息

School of Environment, Guangdong Key Laboratory of Environmental Pollution and Health, Jinan University, Guangzhou 510632, PR China.

School of Chemistry and Environmental Engineering, Hubei Key Lab of Novel Reactor and Green Chemical Technology, Wuhan Institute of Technology, Xiongchu Avenue, Wuhan 430073, PR China; Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou 450002, PR China.

出版信息

Chemosphere. 2021 Mar;266:128929. doi: 10.1016/j.chemosphere.2020.128929. Epub 2020 Nov 11.

Abstract

The wide use and distribution of sulpiride (SP) has caused potential threats to the water environment and human health. In this study, ultrathin S-doped graphitic carbon nitride nanosheets (US-CN) was successfully synthesized and characterized, and its SP removal efficiency was evaluated under various conditions via the visible-light-assisted peroxydisulfate (PDS) activation method. The degradation pathways and mechanism were also discussed through quenching experiments, density functional theory (DFT) calculations, and intermediate products detection. After sulfur doping and ultrasonic treatment, graphitic carbon nitride (CN) possessed an ultra-thin and porous structure, which facilitated the electronic distribution and more photocurrent, thus resulting in the excellent stability and removal efficiency for SP via PDS activation upon visible light irradiation. The singlet oxygen (O) generated by the US-CN/PDS/VL system played a significant role in SP degradation. Based on the bonds of electron-rich atoms fracturing and the SO extrusion, the SP degradation pathway was proposed. This work provides a useful information for the SP photocatalytic degradation via PDS activation.

摘要

舒必利(SP)的广泛使用和分布对水环境和人类健康造成了潜在威胁。在这项研究中,成功合成并表征了超薄 S 掺杂石墨相氮化碳纳米片(US-CN),并通过可见光辅助过二硫酸盐(PDS)活化法在各种条件下评价了其 SP 去除效率。通过猝灭实验、密度泛函理论(DFT)计算和中间产物检测讨论了降解途径和机制。经过硫掺杂和超声处理后,石墨相氮化碳(CN)具有超薄和多孔结构,有利于电子分布和更多光电流,从而在可见光照射下通过 PDS 活化实现了对 SP 的优异稳定性和去除效率。US-CN/PDS/VL 体系产生的单线态氧(O)在 SP 降解中发挥了重要作用。基于富电子原子键的断裂和 SO 的挤出,提出了 SP 的降解途径。这项工作为通过 PDS 活化进行 SP 的光催化降解提供了有用的信息。

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