g-C3N4/Bi2MoO6/clinoptilolite 异质结在过硫酸盐存在下增强光催化降解水中抗生素的协同效应

IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC ACS Applied Electronic Materials Pub Date : 2024-08-31 DOI:10.1039/D4EW00549J
Phuong Thu Le, Thu Phuong Nguyen, Thi Hai Do, Hong Nam Nguyen, Thi Mai Thanh Dinh, Thi Thuy Phan, Toshiki Tsubota and Trung Dung Nguyen
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摘要

通过水热法合成了一种新型高效光催化剂 g-C3N4/Bi2MoO6/clinoptilolite 纳米复合材料(CNBC),并在可见光(vis)照射下作为 Z 型异质结有效激活过硫酸盐(PDS)降解土霉素(OTC)。通过 XRD、FT-IR、FE-SEM、EDX、BET、TGA、UV-vis DRS、PL 和 XPS 测定了光催化剂的形貌和结构。结果表明,在[OTC] = 20 mg L-1、[催化剂] = 500 mg L-1、[Na2S2O8] = 1.26 mM、室温下 pH = 4 的条件下,CNBC-30 的光催化性能最佳,120 min 内的 OTC 去除率超过 87%,远优于纯 g-C3N4、Bi2MoO6 和 CNB 复合材料。这种优越性得益于clinoptilolite 的出色吸附能力,它能有效地形成 g-C3N4/Bi2MoO6 异质结,从而提高分离电荷载流子的能力,同时降低电子-空穴对的重组率。此外,还全面研究了催化剂用量、氧化剂浓度、初始污染物浓度、溶液 pH 值和共存阴离子对 OTC 降解的影响。结果表明,CNBC-30/PDS 系统在不同 pH 值(3.0-11.0)下具有较高的重复使用性和适应性。淬灭试验表明,1O2、O2˙- 和 h+ 在 OTC 降解中起主要作用。此外,还根据 MS 分析结果确定了 OTC 的中间产物并提出了降解途径。DFT 计算成功预测了 OTC 分子上 Fukui 数较高且适合氧化剂攻击的位置。经过四个循环后,CNBC-30 能够稳定地降解 OTC,降解效率超过 78%,这证明了它的耐久性和实际应用潜力。这项研究深入探讨了在可见光区域通过基于clinoptilolite的Z-scheme异质结激活PDS以降解有机污染物的问题。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Synergistic effect of the heterojunction g-C3N4/Bi2MoO6/clinoptilolite to enhance the photocatalytic degradation of antibiotics in water in the presence of persulfate†

A novel and highly efficient photocatalyst, g-C3N4/Bi2MoO6/clinoptilolite nanocomposite (CNBC), was synthesized by a hydrothermal method and acted as a Z-scheme heterojunction for efficient activation of peroxydisulfate (PDS) to degrade oxytetracycline (OTC) under visible light (vis) irradiation. The morphology and structure of the photocatalyst were determined by XRD, FT-IR, FE-SEM, EDX, BET, TGA, UV-vis DRS, PL, and XPS. The results showed that CNBC-30 had the best photocatalytic performance with an OTC removal efficiency of more than 87% within 120 min under the conditions of [OTC] = 20 mg L−1, [catalyst] = 500 mg L−1, [Na2S2O8] = 1.26 mM, and pH = 4 at room temperature, which was much better than those of pure g-C3N4, Bi2MoO6, and CNB composites. This superiority is due to the excellent adsorption ability of clinoptilolite that effectively forms the g-C3N4/Bi2MoO6 heterojunctions, thus improving the ability to separate charge carriers while decreasing the recombination rate of electron–hole pairs. Furthermore, the effect of catalyst dosage, oxidant concentration, initial pollutant concentration, solution pH, and coexisting anions on the OTC degradation was comprehensively studied. The results showed that the CNBC-30/PDS system had high reusability and adaptability at different pH levels (3.0–11.0). Quenching tests showed that 1O2, O2˙, and h+ played the main roles in OTC degradation. In addition, OTC intermediates were identified and degradation pathways were proposed based on the results of MS analysis. DFT calculations successfully predicted the positions on the OTC molecule with high Fukui numbers that are suitable for attack by oxidants. CNBC-30 was stable for OTC degradation after four cycles with a degradation efficiency of above 78%, demonstrating its durability and potential for practical applications. This study provides insight into PDS activation in the visible light region by a clinoptilolite-based Z-scheme heterojunction for organic pollutant degradation.

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