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一步合成及核壳结构 Fe@SiO2 纳米复合材料的表征用于六价铬(Cr(VI))的还原。

One-step synthesis and characterization of core-shell Fe@SiO2 nanocomposite for Cr (VI) reduction.

机构信息

Key Laboratory of Pollution Processes and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300071, PR China.

出版信息

Sci Total Environ. 2012 Apr 1;421-422:260-6. doi: 10.1016/j.scitotenv.2012.01.010. Epub 2012 Feb 29.

Abstract

A facile one-step method was developed to fabricate mono-dispersed Fe nanoparticles (Fe NPs) coated with SiO(2) shell by aqueous reduction method combined with modified Stöber method. Borohydride was acted not only as a reductant for iron salt but also as a catalyst for hydrolysis and polycondensation reaction of tetraethylorthosilicate (TEOS), and more importantly, there was no need to use surface primer for the generation of Fe NPs and catalyst NH(4)OH for SiO(2). Both the Fe NPs agglomeration and SiO(2) shell thickness can be controlled through the synthetic conditions. Lower potassium borohydride (KBH(4)) injection speed was preferable to assemble Fe NPs. The SiO(2) shell thickness increased gradually with the increase of TEOS amount. Under the condition of TEOS amount of 0.1mL and KBH(4) injection speed of 5mL/min, 25nm single Fe NP was coated with SiO(2) shell with thickness of about 9nm. The resulting nanoporous SiO(2) shell was proved to allow reactant to reach the Fe NPs while at the same time protect them from aggregation. The reactivity characterization of the SiO(2)-coated Fe nanoparticles (Fe@SiO(2)) showed that both TEOS concentration and KBH(4) injection speed had effect on Cr (VI) degradation ability. The highest removal capacity of Fe@SiO(2) can reach 467mgCr/gFe at an initial Cr (VI) concentration of 70mg/L under pH 6.0±0.1. XPS and TEM results showed that Cr (VI) was converted to nontoxic Cr (III) and the reaction product was completely adsorbed to SiO(2) shell.

摘要

一种简便的一步法,通过水相还原法结合改进的斯陶伯法制备单分散 Fe 纳米粒子(Fe NPs),并在其表面包覆 SiO(2)壳。硼氢化钠不仅作为铁盐的还原剂,而且作为正硅酸乙酯(TEOS)水解和缩聚反应的催化剂,更重要的是,生成 Fe NPs 时无需使用表面引发剂和催化剂 NH(4)OH。通过合成条件可以控制 Fe NPs 的团聚和 SiO(2)壳的厚度。较低的硼氢化钾(KBH(4))注入速度有利于组装 Fe NPs。随着 TEOS 用量的增加,SiO(2)壳的厚度逐渐增加。在 TEOS 用量为 0.1mL 和 KBH(4)注入速度为 5mL/min 的条件下,25nm 单 Fe NP 被约 9nm 厚的 SiO(2)壳包覆。所得的纳米多孔 SiO(2)壳被证明允许反应物到达 Fe NPs,同时保护它们不聚集。SiO(2)包覆 Fe 纳米颗粒(Fe@SiO(2))的反应性特征表明,TEOS 浓度和 KBH(4)注入速度均对 Cr(VI)降解能力有影响。在初始 Cr(VI)浓度为 70mg/L、pH 值为 6.0±0.1 的条件下,Fe@SiO(2)的最大去除容量可达 467mgCr/gFe。XPS 和 TEM 结果表明,Cr(VI)被转化为无毒的 Cr(III),反应产物完全被吸附到 SiO(2)壳上。

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