Co-grown novel S-scheme tubular P-UCN/S-TCN homojunction mediates photocatalysis-PMS activation synergistic system for efficient degradation of antibiotic.

Ting Wu, Zhifeng Liu, Binbin Shao, Yuan Pan, Qingyun He, Xiansheng Zhang, Lingfeng Zhou, Yunze Wang, Teng Li, Sheng Liu
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Abstract

The low photogenerated carrier separation and transport ability of the photocatalyst are the main factors inhibiting the photocatalytic activity. The construction of composite photocatalysts can effectively improve the efficiency of photogenerated carriers. However, the problem of reduced photocatalyst stability and catalytic activity due to easy separation of unstable composite interfaces has not been well solved for a long time. Therefore, in this work, a co-growth strategy was put forward to thermally co-polymerize sulfur-containing tubular supramolecular precursors with urea in order to achieve the growth of porous g-C3N4 nanoparticles (P-UCN) on the sulfur-doped tubular g-C3N4 (S-TCN), thus to successfully prepare P-UCN/S-TCN homojunction photocatalysts with chemically bonded stable composite interfaces. Furthermore, a coupled photocatalytic-peroxymonosulfate (PMS) activation system was constructed to further promote the photogenerated carrier separation of P-UCN/S-TCN as well as the catalytic activity of the reaction system through the electron donor-acceptor relationship between P-UCN/S-TCN and PMS. Experimental characterization and DFT theoretical calculations together revealed the band gap structural characteristics and the direction of electron flow of the P-UCN/S-TCN S-scheme homojunction, and confirmed the successful construction of a stable chemically bonded homojunction interface. Then the results of catalytic activity test of P-UCN1/S-TCN1 showed a high tetracycline hydrochloride (TCH) degradation efficiency (93.5%) within 30 min, and also demonstrated 100% degradation efficiency for Rhodamine B (RhB). This work made important progress in the design of a novel stable S-scheme homojunction interface and provided a reference for the application of photocatalysis-PMS coupling system in environmental remediation.

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共同生长的新型 S 型管状 P-UCN/S-TCN 同质结介导光催化-PMS 激活协同系统,实现抗生素的高效降解。
光催化剂的光生载流子分离和传输能力低是抑制光催化活性的主要因素。构建复合光催化剂可以有效提高光生载流子的效率。然而,长期以来,由于不稳定的复合界面易于分离而导致光催化剂稳定性和催化活性降低的问题一直没有得到很好的解决。因此,本研究提出了一种共生长策略,将含硫管状超分子前驱体与尿素进行热共聚合,以实现多孔 g-C3N4 纳米颗粒(P-UCN)在掺硫管状 g-C3N4 (S-TCN)上的生长,从而成功制备出具有化学键合稳定复合界面的 P-UCN/S-TCN 均相结光催化剂。此外,通过 P-UCN/S-TCN 与 PMS 之间的电子供体-受体关系,构建了一个耦合光催化-过氧单硫酸盐(PMS)活化体系,进一步促进了 P-UCN/S-TCN 的光生载流子分离以及反应体系的催化活性。实验表征和 DFT 理论计算共同揭示了 P-UCN/S-TCN S 型同质结的带隙结构特征和电子流动方向,并证实成功构建了稳定的化学键同质结界面。随后的催化活性测试结果表明,P-UCN1/S-TCN1在30分钟内对盐酸四环素(TCH)的降解效率高达93.5%,对罗丹明B(RhB)的降解效率也达到了100%。这项工作在设计新型稳定 S 型同质结界面方面取得了重要进展,为光催化-PMS 耦合系统在环境修复中的应用提供了参考。
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