Highly efficient reduction of 4-nitrophenol by heterostructured gold-magnetite nanocatalysts

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL
Fang-hsin Lin, Ruey-an Doong
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引用次数: 115

Abstract

In this study, the catalytic reduction of 4-nitrophenol by heterostructured Au–Fe3O4 nanocatalysts using NaBH4 as the reducing agent was investigated under various environmental conditions. The electron behaviors at the interface of Au and Fe3O4 nanoparticles were examined to elucidate the reaction mechanisms for 4-nitrophenol reduction. The transmission electron microscopic images show that the average particle size of Au–Fe3O4 heterostructures increases slightly from 14 to 18 nm after phase transfer from oil phase to aqueous solution. The X-ray photoelectron and X-ray absorption near edge spectroscopic results show the electron flow from Au seeds to Fe3O4, resulting in the formation of positively charged Au surface to accelerate the catalytic reduction efficiency and rate of 4-nitrophenol. In addition, the reduction of 4-nitrophenol is a surface-mediated reaction and the catalytic efficiency and rate of 4-nitrophenol is highly dependent on the initial 4-nitrophenol concentration, pH, and reaction temperature. The increase in pH lowers the reduction efficiency and rate of 4-nitrophenol and a 2.4-fold decrease in the pseudo-first-order rate constant is observed when pH increases from 5 to 9. In addition, the Au–Fe3O4 nanocatalysts show a good separation ability and reusability which can be repeatedly applied for complete reduction of 4-nitrophenol for at least six successive cycles without the loss of morphology and saturation magnetization. Results obtained in this study clearly demonstrate that the Au–Fe3O4 heterostructures are excellent nanocatalysts which can be applied in heterogeneous catalysis, water treatment, and green chemistry.

Abstract Image

异质结构金磁铁矿纳米催化剂高效还原4-硝基苯酚
本研究以NaBH4为还原剂,研究了异质结构Au-Fe3O4纳米催化剂在不同环境条件下对4-硝基苯酚的催化还原。研究了Au和Fe3O4纳米颗粒界面上的电子行为,以阐明4-硝基苯酚还原的反应机理。透射电镜图像显示,Au-Fe3O4异质结构从油相转移到水溶液后,平均粒径从14 nm略微增大到18 nm。x射线光电子和x射线吸收近边光谱结果表明,电子从Au种子流向Fe3O4,导致带正电的Au表面形成,加速了4-硝基苯酚的催化还原效率和速率。此外,4-硝基苯酚的还原是一个表面介导的反应,4-硝基苯酚的催化效率和速率高度依赖于4-硝基苯酚的初始浓度、pH和反应温度。pH值的增加降低了4-硝基苯酚的还原效率和还原速率,当pH值从5增加到9时,伪一级速率常数降低了2.4倍。此外,Au-Fe3O4纳米催化剂表现出良好的分离能力和可重复使用性,可以在不损失形貌和饱和磁化的情况下重复使用至少6个连续循环来完全还原4-硝基苯酚。本研究结果清楚地表明,Au-Fe3O4异质结构是一种优异的纳米催化剂,可应用于多相催化、水处理和绿色化学等领域。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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