Leiduo Lai , Peng Zhou , Hongyu Zhou , Minglu Sun , Yue Yuan , Yang Liu , Gang Yao , Bo Lai
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引用次数: 39
摘要
二硫代石(DNT)与FeVO4偶联诱导PMS活化(FeVO4/PMS/DNT)可实现快速非均相Fe(III)还原,产生大量活性氧(ROS),在批处理模式下快速降解卡马西平(2.5 mg/L, 300 s内降解效率为90%)。DNT和还原态V推动的Fe(III)/Fe(II)循环经历了两个阶段。DNT诱导SO2−生成,是一种对Fe和V还原能力强的高活性物质。还原态V通过Fe- o -V键将电子给≡Fe(III),而不是直接与PMS反应,这意味着引入多价V来调节铁基材料增强了DNT的利用,减轻了ROS的猝灭效应。FeVO4/PMS/DNT体系具有良好的回用性和较强的耐自然水体性。我们的发现为加速非均相Fe(III)/Fe(II)循环促进fenton样氧化提供了新的思路,这可能是一种长期的水修复策略。
Heterogeneous Fe(III)/Fe(II) circulation in FeVO4 by coupling with dithionite towards long-lasting peroxymonosulfate activation: Pivotal role of vanadium as electron shuttles
Coupling dithionite (DNT) with FeVO4 induced PMS activation (FeVO4/PMS/DNT) effectuates fast heterogeneous Fe(III) reduction to generate multitudinous reactive oxygen species (ROS) for fast degradation of carbamazepine (2.5 mg/L, >90 % degradation efficiency within 300 s) in batch mode. The Fe(III)/Fe(II) circulation propelled by DNT and reduced V species experiences two stages. DNT induces SO2− generation, which is a highly active species with strong reducibility for Fe and V reduction. The reduced V species donate electrons to ≡Fe(III) via Fe-O-V bond rather than directly react with PMS, implying introducing polyvalent V to modulate Fe-based materials intensifies DNT utilization and alleviates ROS quenching effects. Moreover, FeVO4 crystalline form regains after reaction, and FeVO4/PMS/DNT system has an excellent reutilization and strong resistance to natural waters. Our discovery sheds new light on acceleration of heterogenous Fe(III)/Fe(II) circulation to promote Fenton-like oxidation, it may be a long-lasting strategy for water remediation.
期刊介绍:
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.