MIL-88(Fe)负载ZIF-8制备的分级多孔Fe3O4/Fe@C复合材料通过协同吸附和还原高效去除Cr(VI)

IF 3 4区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES
Dongyu Xie, Chenyu Zhou, Yingxue Wang, Mengxin Zhao, Xin Wang, Mei Wang, Xiaobin Zhou
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引用次数: 0

摘要

合成了一种新型的Fe3O4/Fe@C@ZIF-8复合材料,该复合材料将ZIF-8优越的吸附能力与Fe3O4/Fe@C核芯的氧化还原活性协同结合,用于Cr(VI)的协同吸附-还原。在最佳条件(投加量0.6 g·L−1,pH 4.0, 30℃)下,该复合材料对Cr(VI)的去除率为94.27%,初始浓度为30 mg·L−1。动力学和热力学分析表明,吸附过程符合拟二级动力学和Langmuir等温线模型,表明其具有自发和吸热特性的单层化学吸附。机理研究揭示了一种协同修复机制:ZIF-8中的质子化氮部分使Cr(VI)氧离子静电捕获,随后通过ZIF-8的分层孔扩散到Fe3O4/Fe@C核心;吸附的Cr(VI)离子被Fe0、Fe2+和C通过组分间电子转移部分还原为Cr(III),并形成Fe(III)。因此,生成的Cr(III)离子与Fe(III)共沉淀,形成无定形氢氧化物配合物,并粘附在Fe3O4/Fe@C@ZIF-8表面,从而实现了水环境中Cr的消除。总的来说,吸附、氧化还原转化和磁可分离性的结合使Fe3O4/Fe@C@ZIF-8成为重金属修复的有前途的候选材料,为基于mof的复合材料设计提供了新的见解。图形抽象
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Hierarchical Porous Fe3O4/Fe@C Composites Derived from MIL-88(Fe) Loaded with ZIF-8 for Efficient Cr(VI) Removal via Synergistic Adsorption and Reduction

A novel hierarchical Fe3O4/Fe@C@ZIF-8 composite, which synergistically combined ZIF-8’s superior adsorption capacity with the redox reactivity of the Fe3O4/Fe@C core, was synthesized for Cr(VI) synergistic adsorption-reduction. The composite demonstrated remarkable Cr(VI) removal efficiency, achieving 94.27% elimination from aqueous solutions (initial concentration: 30 mg·L−1) under optimized conditions (dosage: 0.6 g·L−1, pH 4.0, 30 ℃). Kinetic and thermodynamic analyses revealed the adsorption process followed pseudo-second-order kinetics and Langmuir isotherm models, indicative of monolayer chemisorption with spontaneous and endothermic characteristics. Mechanistic investigations unveiled a synergistic remediation mechanism: the protonated nitrogen moieties within ZIF-8 enabled electrostatic capture of Cr(VI) oxyanions, which subsequently diffused through ZIF-8’s hierarchical pores to access the Fe3O4/Fe@C core; the adsorbed Cr(VI) ions were partially reduced to Cr(III) by Fe0, Fe2+, and C via intercomponent electron transfer, accompanied by the formation of Fe(III). Consequently, the resulting Cr(III) ions co-precipitated with Fe(III), forming amorphous hydroxide complexes that adhered to the surface of Fe3O4/Fe@C@ZIF-8, thereby effectuating the elimination of Cr species from the aqueous environment. Overall, the combination of adsorption, redox transformation, and magnetic separability positioned Fe3O4/Fe@C@ZIF-8 as a promising candidate for heavy metal remediation, providing new insights into MOF-based composite design for environmental applications.

Graphical Abstract

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来源期刊
Water, Air, & Soil Pollution
Water, Air, & Soil Pollution 环境科学-环境科学
CiteScore
4.50
自引率
6.90%
发文量
448
审稿时长
2.6 months
期刊介绍: Water, Air, & Soil Pollution is an international, interdisciplinary journal on all aspects of pollution and solutions to pollution in the biosphere. This includes chemical, physical and biological processes affecting flora, fauna, water, air and soil in relation to environmental pollution. Because of its scope, the subject areas are diverse and include all aspects of pollution sources, transport, deposition, accumulation, acid precipitation, atmospheric pollution, metals, aquatic pollution including marine pollution and ground water, waste water, pesticides, soil pollution, sewage, sediment pollution, forestry pollution, effects of pollutants on humans, vegetation, fish, aquatic species, micro-organisms, and animals, environmental and molecular toxicology applied to pollution research, biosensors, global and climate change, ecological implications of pollution and pollution models. Water, Air, & Soil Pollution also publishes manuscripts on novel methods used in the study of environmental pollutants, environmental toxicology, environmental biology, novel environmental engineering related to pollution, biodiversity as influenced by pollution, novel environmental biotechnology as applied to pollution (e.g. bioremediation), environmental modelling and biorestoration of polluted environments. Articles should not be submitted that are of local interest only and do not advance international knowledge in environmental pollution and solutions to pollution. Articles that simply replicate known knowledge or techniques while researching a local pollution problem will normally be rejected without review. Submitted articles must have up-to-date references, employ the correct experimental replication and statistical analysis, where needed and contain a significant contribution to new knowledge. The publishing and editorial team sincerely appreciate your cooperation. Water, Air, & Soil Pollution publishes research papers; review articles; mini-reviews; and book reviews.
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