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利用一种基于钛的金属有机框架进行选择性吸附和可见光驱动的水修复。

Harnessing a Ti-based MOF for selective adsorption and visible-light-driven water remediation.

作者信息

Myakala Stephen Nagaraju, Ladisich Magdalena, Ayala Pablo, Rabl Hannah, Batool Samar, Elsaesser Michael S, Cherevan Alexey, Eder Dominik

机构信息

Institute of Materials Chemistry, Division of Molecular Materials Chemistry, TU Wien Getreidemarkt 9/BC/02 1060 Vienna Austria

Department of Chemistry and Physics of Materials, Paris-Lodron-University of Salzburg 5020 Salzburg Austria.

出版信息

J Mater Chem A Mater. 2024 Jun 4;12(31):19924-19934. doi: 10.1039/d4ta01967a. eCollection 2024 Aug 6.

Abstract

In pursuit of universal access to clean water, photocatalytic water remediation using metal-organic frameworks (MOFs) emerges as a strong alternative to the current wastewater treatment methods. In this study, we explore a unique Ti-based MOF comprised of 2D secondary-building units (SBUs) connected biphenyl dicarboxylic acid (Hbpdc) ligands - denoted as COK-47 - as a visible-light-driven photocatalyst for organic dye degradation. Synthesized a recently developed microwave-assisted method, COK-47 exhibits high hydrolytic stability, demonstrates a strong dye uptake, and shows noteworthy dye-degradation performance under UV, visible, and solar light, outperforming benchmark TiO and MIL-125-Ti photocatalysts. Due to its nanocrystalline structure and surface termination with organic linkers, COK-47 exhibits selective degradation of cationic pollutants while remaining inert towards anionic dyes, thus highlighting its potential for selective oxidation reactions. Mechanistic studies reveal the involvement of superoxide radicals in the degradation process and emphasize the need to minimize the recombination of photogenerated electron-hole pairs to achieve optimal performance. Post-catalytic studies further confirm the high stability and reusability of COK-47, making it a promising photocatalyst for water purification, organic transformation, and water splitting reactions under visible light.

摘要

为了实现普遍获得清洁水的目标,使用金属有机框架(MOF)进行光催化水修复成为当前废水处理方法的有力替代方案。在本研究中,我们探索了一种独特的基于钛的MOF,它由二维二级建筑单元(SBU)与联苯二甲酸(Hbpdc)配体相连组成,记为COK-47,作为一种可见光驱动的光催化剂用于有机染料降解。采用最近开发的微波辅助方法合成的COK-47具有高水解稳定性,表现出很强的染料吸附能力,并且在紫外光、可见光和太阳光下均显示出显著的染料降解性能,优于基准TiO和MIL-125-Ti光催化剂。由于其纳米晶体结构和有机连接体的表面封端,COK-47对阳离子污染物表现出选择性降解,而对阴离子染料保持惰性,从而突出了其在选择性氧化反应中的潜力。机理研究揭示了超氧自由基参与降解过程,并强调需要尽量减少光生电子-空穴对的复合以实现最佳性能。催化后研究进一步证实了COK-47的高稳定性和可重复使用性,使其成为可见光下用于水净化、有机转化和水分解反应的有前途的光催化剂。

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