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杂原子掺杂金属铁-聚偏氟乙烯(PVDF)膜用于增强有机污染物的氧化。

Heteroatoms doped metal iron-polyvinylidene fluoride (PVDF) membrane for enhancing oxidation of organic contaminants.

机构信息

Anhui Key Lab of Controllable Chemical Reaction & Material Chemical Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Tunxi Road 193, Hefei 230009, China; School of Chemistry and Material Science, University of Science and Technology of China, Hefei 230026, PR China.

Anhui Key Lab of Controllable Chemical Reaction & Material Chemical Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Tunxi Road 193, Hefei 230009, China.

出版信息

J Hazard Mater. 2017 Sep 15;338:265-275. doi: 10.1016/j.jhazmat.2017.05.026. Epub 2017 May 15.

Abstract

Iron nanoparticles (NPs) embedded in S, N-codoped carbon were prepared by one-step pyrolysis of a homogeneous mixture consisting of Fe, S, N, C precursors, and then immobilized in poly (vinylidene fluoride) membranes as a multifunctional catalytic system (NSC-Fe@PVDF) to effectively activate peroxymonosulfate (PMS) and oxidize organic compounds in water. The NSC-Fe@PVDF membranes effectively decolorized organic pollutants at a wide pH range (2.05-10.85), due to the synergistic effects between the S, N-doped carbon and iron NPs. The efficiency depended on the doping types, amount of metal, PMS dosages, reaction temperatures, solution pHs, and organic substrates. In-situ electron spin resonance spectroscopy and sacrificial-reagent incorporated catalysis indicate radical intermediates such as sulfate and hydroxyl radicals are mainly responsible for this persulfate-driven oxidation of organic compounds. Membrane's porous structure and high internal surface area not only minimize the NPs agglomeration, but also allow the facile transport of catalytic reactants to the active surface of metal catalysts. The results demonstrate the morphological and structural features of catalytic membranes enhance the overall catalytic activity.

摘要

铁纳米粒子(NPs)嵌入 S、N 共掺杂碳中,通过将 Fe、S、N、C 前体的均相混合物一步热解制备而成,然后将其固定在聚偏二氟乙烯(PVDF)膜中作为多功能催化体系(NSC-Fe@PVDF),以有效地激活过一硫酸盐(PMS)并氧化水中的有机化合物。NSC-Fe@PVDF 膜在很宽的 pH 值范围(2.05-10.85)内有效地使有机污染物脱色,这是由于 S、N 共掺杂碳和铁 NPs 之间的协同作用。效率取决于掺杂类型、金属含量、PMS 剂量、反应温度、溶液 pH 值和有机底物。原位电子自旋共振光谱和加入牺牲剂的催化实验表明,硫酸盐和羟基自由基等自由基中间体是这种过硫酸盐驱动的有机化合物氧化的主要原因。膜的多孔结构和高内表面积不仅最小化了 NPs 的团聚,而且还允许催化反应物容易地输送到金属催化剂的活性表面。结果表明,催化膜的形态和结构特征提高了整体催化活性。

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