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基于聚偏二氟乙烯膜的黄铁矿嵌入多孔碳纳米催化剂用于有机污染物氧化。

Pyrite-embedded porous carbon nanocatalysts assembled in polyvinylidene difluoride membrane for organic pollutant oxidation.

机构信息

Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Tunxi Road 193, Hefei 230009, China.

Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Tunxi Road 193, Hefei 230009, China.

出版信息

J Colloid Interface Sci. 2022 Feb 15;608(Pt 3):2942-2954. doi: 10.1016/j.jcis.2021.11.021. Epub 2021 Nov 14.

Abstract

FeS-embedded in porous carbon (FeS/C) was prepared by simultaneous sulfidation and carbonization of an iron-based metal-organic framework precursor, and subsequently immobilized in polyvinylidene fluoride membranes (FeS/C@PVDF) for organics removal via peroxymonosulfate (PMS) activation. The composition, structure, and morphology of the FeS/C@PVDF membrane were extensively characterized. Scanning electron microscopy images manifest that the FeS/C nanoparticles with an average diameter of 40 nm are assembled on the external and internal membrane surface. The as-prepared FeS/C@PVDF membrane exhibits excellent performances over a wide pH range of 1.53-9.50, exceeding carbon-free syn-FeS@PVDF. The effective degradation could be improved by inner pyrite FeS cores and thus enhanced the electron transfer between carbon shell and PMS. Electron paramagnetic resonance and quenching experiments elucidated that radical (HO, SO) and nonradical (O) species were the predominant reactive oxidants. In addition, FeS/C@PVDF exhibited high stability with low Fe leaching (0.377 mg/L) owing to the effective protection of the outer carbon skeleton. Plentiful porosity of PVDF membranes not only affords a controlled size and confined uniform distribution of the immobilized FeS/C nanoparticles, but also enables a persistent exposure of active sites and enhanced mass transfer efficiency. Our findings demonstrate a promise for utilizing the novel FeS/C@PVDF membrane as an efficient catalyst for the environmental cleanup.

摘要

通过铁基金属有机骨架前体的同步硫化和碳化制备了嵌入多孔碳中的 FeS(FeS/C),随后将其固定在聚偏二氟乙烯膜(FeS/C@PVDF)中,通过过一硫酸盐(PMS)活化来去除有机物。对 FeS/C@PVDF 膜的组成、结构和形态进行了广泛的表征。扫描电子显微镜图像表明,平均直径为 40nm 的 FeS/C 纳米颗粒组装在膜的内外表面。所制备的 FeS/C@PVDF 膜在 1.53-9.50 的宽 pH 范围内表现出优异的性能,超过了无碳 syn-FeS@PVDF。内黄铁矿 FeS 核的有效降解可以提高电子转移效率,从而提高了电子转移效率,增强了碳壳与 PMS 之间的电子转移。电子顺磁共振和猝灭实验阐明了自由基(HO、SO)和非自由基(O)物种是主要的反应性氧化剂。此外,由于外碳骨架的有效保护,FeS/C@PVDF 表现出较高的稳定性,铁浸出率低(0.377mg/L)。PVDF 膜的丰富孔隙不仅提供了受控的尺寸和受限的固定化 FeS/C 纳米颗粒的均匀分布,而且还能持续暴露活性位点并提高传质效率。我们的研究结果表明,新型 FeS/C@PVDF 膜作为一种有效的环境净化催化剂具有广阔的应用前景。

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