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用于高效协同光催化产生羟基自由基和降解四环素的新型羽毛状磷/硫共掺杂石墨相氮化碳

Novel feathery P/S Co-doped graphitic carbon nitride for highly efficient synergistic photocatalytic HO generation and tetracycline degradation.

作者信息

Qin Lian, Zhao Zhongli, Fu Ning, Li Xiangyu, Hu Lei, Li Xingang, Zhang Chun

机构信息

School of Chemistry and Chemical Engineering, Lanzhou Jiaotong University Lanzhou 730070 PR China

Chongqing Titanium Industry Co. Ltd of Pangang Group Chongqing 400055 PR China.

出版信息

RSC Adv. 2024 Dec 4;14(52):38391-38402. doi: 10.1039/d4ra05879h. eCollection 2024 Dec 3.

DOI:10.1039/d4ra05879h
PMID:39635363
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11615658/
Abstract

Graphitic carbon nitride (g-CN) has garnered significant attention in photocatalytic pollutant degradation for its non-toxicity and cost-effectiveness. However, its limited photocatalytic performance has hindered its applications. Addressing this, we successfully synthesized a novel feathery multifunctional catalyst, phosphorus and sulfur co-doped g-CN (PS-CN), with an enlarged pore network through a hydrothermal method. This catalyst exhibits remarkable photocatalytic performance under visible light, achieving a hydrogen peroxide (HO) production rate of 28.6 mg L h and an efficiency of 87.3% in degrading tetracycline (TC). Comparative studies demonstrate that PS-CN outperforms singly doped catalysts P-CN and S-CN by increasing HO yield by 28.67% and 53.28% and improving TC degradation by 15.2% and 11.5%, respectively. These improvements can be attributed to the synergetic effects of P and S co-doping and the high number of active sites provided by its peculiar morphology, which enhance charge transfer and photocatalytic activity, and a more pronounced conjugation effect, resulting in a high electrostatic potential surface conducive to adsorption and activation, as confirmed by density-functional theory calculations. Our findings propose a mechanism for the synergistic photocatalytic-Fenton degradation (PSF) of TC using PS-CN. This present research contributes to the advancement of g-CN-based photocatalysts and promotes the exploration of more efficient carbon-based catalysts for environmental remediation.

摘要

石墨相氮化碳(g-CN)因其无毒且成本效益高,在光催化降解污染物方面受到了广泛关注。然而,其有限的光催化性能阻碍了它的应用。针对这一问题,我们通过水热法成功合成了一种新型的羽毛状多功能催化剂——磷硫共掺杂g-CN(PS-CN),其具有扩大的孔网络。该催化剂在可见光下表现出卓越的光催化性能,过氧化氢(HO)产率达到28.6 mg L h,降解四环素(TC)的效率为87.3%。对比研究表明,PS-CN分别比单掺杂催化剂P-CN和S-CN的HO产率提高了28.67%和53.28%,TC降解率提高了15.2%和11.5%。这些改进可归因于磷和硫共掺杂的协同效应以及其特殊形态提供的大量活性位点,这增强了电荷转移和光催化活性,以及更显著的共轭效应,从而形成有利于吸附和活化的高静电势表面,密度泛函理论计算证实了这一点。我们的研究结果提出了一种使用PS-CN对TC进行光催化-芬顿协同降解(PSF)的机制。本研究有助于推进基于g-CN的光催化剂的发展,并促进探索更高效的用于环境修复的碳基催化剂。

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