双金属 MIL-101(Fe,Cu)活化过硫酸盐体系增强气态苯降解:效率与机理

IF 4.9 2区 化学 Q2 CHEMISTRY, PHYSICAL
Tao Tian, Jie Zhang, Sijie Ge, Lijiang Tian
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引用次数: 0

摘要

过硫酸盐氧化技术是一种前景广阔的空气污染控制技术,但在温和条件下仍存在难以降解难降解挥发性有机化合物(VOCs)的问题。掺杂金属的金属有机框架(MOFs)为增强过硫酸盐活化和 VOCs 降解提供了一种新策略。本文制备了一种新型双金属 MIL-101(铁、铜),可通过过硫酸盐活化更有效地降解气态苯。在最佳条件下(铁/铜比例为 1:4,过硫酸盐浓度为 7 mM/L,pH 值为 5,反应温度为 70 °C),MIL-101(Fe1, Cu4)活化过硫酸盐体系的苯降解效率达到 79.1%,明显高于 MIL-101(Fe)(20.1%)。性能的提高可归因于 Fe²⁺/Fe³⁺ 和 Cu²⁺/Cu⁺ 氧化还原作用的协同效应,促进了过硫酸盐的活化和自由基物种的生成。密度泛函理论(DFT)计算表明,在掺入 Cu 的情况下,MIL-101(Fe)的吸附能从 -3.46 eV 上升到 -5.92 eV,费米能级从 0.5 eV 上升到 1.33 eV,从而提高了电子密度和迁移率。反应能图说明了苯降解过程中的反应途径和过渡状态。总之,在 MOFs 中加入 Cu 能显著提高基于过硫酸盐的氧化系统降解 VOCs 的效率。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Enhanced gaseous benzene degradation by bimetallic MIL-101(Fe, Cu) activated persulfate system: Efficiency and mechanism
Persulfate oxidation is a promising technology for air pollution control but still suffers from degrading refractory volatile organic compounds (VOCs) under mild conditions. Metal-doped metal-organic frameworks (MOFs) offer a novel strategy to enhance persulfate activation and VOCs degradation. Herein, a novel bimetallic MIL-101 (Fe, Cu) is prepared for more effective degradation of gaseous benzene via persulfate activation. Under optimal conditions (Fe/Cu ratio of 1:4, persulfate concentration of 7 mM/L, pH of 5, and reaction temperature of 70 °C), the MIL-101(Fe1, Cu4) activated persulfate system achieves a benzene degradation efficiency of 79.1 %, a value significantly higher than that of MIL-101(Fe) (20.1 %). The enhanced performance can be attributed to the synergistic effect of Fe²⁺/Fe³⁺ and Cu²⁺/Cu⁺ redox interactions facilitating the activation of persulfate and generation of radical species. Density functional theory (DFT) calculations indicate an increase in the adsorption energy of MIL-101(Fe) in the presence of Cu doping from −3.46 eV to −5.92 eV along with a rise in the Fermi energy level from 0.5 eV to 1.33 eV, enhancing the electron density and mobility. A reaction energy diagram is provided to illustrate the reaction pathways and transition states involved in the degradation of benzene. Overall, the incorporation of Cu in MOFs significantly enhances the efficiency of persulfate-based oxidation systems toward VOCs degradation.
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来源期刊
CiteScore
8.70
自引率
9.60%
发文量
2421
审稿时长
56 days
期刊介绍: Colloids and Surfaces A: Physicochemical and Engineering Aspects is an international journal devoted to the science underlying applications of colloids and interfacial phenomena. The journal aims at publishing high quality research papers featuring new materials or new insights into the role of colloid and interface science in (for example) food, energy, minerals processing, pharmaceuticals or the environment.
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