Surface structure regulation of sulfidated zero-valent iron by H2O2 for efficient pH self-regulation and proton cycle to boost heterogeneous Fenton-like reaction for pollutant control

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-12-27 DOI:10.1016/j.apcatb.2023.123667

Can Feng , Heng Zhang , Yang Liu , Yi Ren , Peng Zhou , Chuan-Shu He , Zhaokun Xiong , Weihua Liu , Xiaoqiang Dai , Bo Lai

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Abstract

Sulfidated zero-valent iron (SZVI) has been widely used in controlling organic pollutants. However, the significant decrease in catalytic activity of SZVI-based Fenton-like systems under neutral and alkaline conditions remains a large problem. Herein, it was found that surface structure regulation of SZVI with H₂O₂ (HT-SZVI) greatly enhanced its reactivity and efficiently activated H₂O₂ to oxidize various organics in a wide pH range. The HT-SZVI/H₂O₂ system exhibited a pH self-regulation capability that stabilized the eventual solution pH at ∼3.5 at the initial pH of 3.0–9.0. The excellent oxidation performance was primarily attributed to surface-bound ^•OH produced from H₂O₂ activation by surface Fe(II) sites on HT-SZVI. Additionally, dissolved Fe(II) converted from surface Fe(II) induced proton generation to self-regulate pH. Newly formed high proton-conductive FeS and Fe₃O₄ shells accelerated the transfer of accumulated protons in solution to iron core to produce Fe(II), enabling efficient proton consumption-regeneration cycle and enhancing ^•OH production.

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H2O2 对硫化零价铁表面结构的调控可实现高效的 pH 值自我调节和质子循环，从而促进异质 Fenton-like 反应，达到控制污染物的目的

硫化零价铁（SZVI）已被广泛用于控制有机污染物。然而，在中性和碱性条件下，基于 SZVI 的 Fenton-like 系统的催化活性明显降低，这仍然是一个很大的问题。研究发现，用 H2O2 调节 SZVI 的表面结构（HT-SZVI）可大大提高其反应活性，并在较宽的 pH 值范围内有效激活 H2O2 氧化各种有机物。HT-SZVI/H2O2 系统具有 pH 值自我调节能力，可在初始 pH 值为 3.0-9.0 时将最终溶液 pH 值稳定在 3.5 左右。优异的氧化性能主要归功于 HT-SZVI 表面铁（II）位点活化 H2O2 产生的表面结合 -OH。此外，溶解的 Fe（II）从表面 Fe（II）诱导的质子生成转化为自我调节 pH 值。新形成的高质子传导性 FeS 和 Fe3O4 外壳加速了溶液中积累的质子向铁核的转移，从而产生 Fe（II），实现了有效的质子消耗-再生循环，并增强了 -OH 的产生。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

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.