Porphyrinic based hydrogen-bonded organic framework/TiO2 nanocomposites for efficient photocatalytic degradation of sulfadiazine

IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES
Chunying Li , Yu Zhang , Mengfei Tian , Naveed Ahmad , Kaitao Jia , Zidan Luo , Bin Qiao , Jiabo Cheng , Chunjian Zhao
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引用次数: 0

Abstract

Porphyrinic hydrogen-bonded organic frameworks (porph-HOFs) have emerged as highly promising materials in the realm of photocatalysis due to their remarkable attributes, including low density, high surface area, efficient visible light absorption, and notable chemical stability. However, the rapid recombination of photogenerated charges remains a significant concern. In this work, a novel HOF-based photocatalyst, PFC-72/TiO2 was successfully designed with visible light response and high electron transfer capability. This involved bonding TiO2 nanoparticles to the PFC-72 framework synthesized using cobalt porphyrin as organic ligand and introducing bridging molecules 4-mercaptopyridine (4-PySH). Moreover, sulfadiazine (SDZ), a highly prevalent antibiotic, was effectively degraded from wastewater using PFC-72/TiO2. The high specific surface area of PFC-72 significantly improved the dispersion of TiO2 in PFC-72/TiO2, providing more active sites and improving the ability to adsorb SDZ. Characterizations and density functional theory analysis further confirmed that the photosensitization effect of porph-HOF extended the response range of TiO2 in PFC-72/TiO2 and reduced the recombination efficiency of photogenerated charges, consequently enhancing photocatalytic performance. Additionally, due to significantly improved robustness of PFC-72 and its axial coordination interaction with 4-PySH, PFC-72/TiO2 displayed excellent stability and recyclability. Consequently, optimized PFC-72/TiO2 exhibited a remarkable SDZ removal efficiency of 93.73% within 120 min, maintaining consistent photoactivity even after undergoing four cycles. Furthermore, intermediate products and degradation pathways were proposed based on UPLC-MS/MS.

Abstract Image

基于卟啉的氢键有机框架/二氧化钛纳米复合材料用于高效光催化降解磺胺嘧啶
卟啉氢键有机框架(porph-HOFs)因其低密度、高比表面积、高效吸收可见光和显著的化学稳定性等显著特性,已成为光催化领域极具前景的材料。然而,光生电荷的快速重组仍然是一个重大问题。在这项工作中,我们成功设计了一种新型的基于 HOF 的光催化剂 PFC-72/TiO2,它具有可见光响应和高电子转移能力。这包括将 TiO2 纳米颗粒与以卟啉钴为有机配体合成的 PFC-72 框架结合,并引入桥接分子 4-巯基吡啶 (4-PySH)。此外,PFC-72/TiO2 还能有效降解废水中的磺胺嘧啶(SDZ),这是一种非常普遍的抗生素。PFC-72 的高比表面积显著改善了 TiO2 在 PFC-72/TiO2 中的分散性,提供了更多的活性位点,提高了吸附 SDZ 的能力。表征和密度泛函理论分析进一步证实,porph-HOF 的光敏效应扩大了 PFC-72/TiO2 中 TiO2 的响应范围,降低了光生电荷的重组效率,从而提高了光催化性能。此外,由于 PFC-72 的稳健性及其与 4-PySH 的轴向配位相互作用得到明显改善,PFC-72/TiO2 显示出卓越的稳定性和可回收性。因此,优化后的 PFC-72/TiO2 在 120 分钟内对 SDZ 的去除率高达 93.73%,即使经过四次循环也能保持稳定的光活性。此外,还根据 UPLC-MS/MS 提出了中间产物和降解途径。
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来源期刊
Journal of Environmental Sciences-china
Journal of Environmental Sciences-china 环境科学-环境科学
CiteScore
13.70
自引率
0.00%
发文量
6354
审稿时长
2.6 months
期刊介绍: The Journal of Environmental Sciences is an international journal started in 1989. The journal is devoted to publish original, peer-reviewed research papers on main aspects of environmental sciences, such as environmental chemistry, environmental biology, ecology, geosciences and environmental physics. Appropriate subjects include basic and applied research on atmospheric, terrestrial and aquatic environments, pollution control and abatement technology, conservation of natural resources, environmental health and toxicology. Announcements of international environmental science meetings and other recent information are also included.
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