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槐糖脂修饰使纳米零价铁对六价铬具有高反应活性和电子选择性。

Sophorolipid modification enables high reactivity and electron selectivity of nanoscale zerovalent iron toward hexavalent chromium.

机构信息

School of Environment, South China Normal University, Guangzhou, 510006, China; Guangdong Province Environmental Remediation Industry Technology Innovation Alliance, Guangzhou 510006, China.

School of Environment, South China Normal University, Guangzhou, 510006, China; Guangdong Province Environmental Remediation Industry Technology Innovation Alliance, Guangzhou 510006, China.

出版信息

J Environ Manage. 2023 Jan 15;326(Pt B):116775. doi: 10.1016/j.jenvman.2022.116775. Epub 2022 Nov 16.

Abstract

Nanoscale zero-valent iron is considered to be a promising nanostructure for environmental remediation, while increasing the electron selectivity of nanoscale zerovalent iron (nZVI) during target contaminant removal is still a challenge (electron selectivity, defined as the percentage of electrons transferred to the target contaminants over the number of electrons donated by nZVI). In this study, the strategy for increasing the reactivity and electron selectivity of nZVI via sophorolipid (SL-nZVI) modification was proposed. The results showed that the removal efficiency and electron selectivity of SL-nZVI toward Cr(VI) was 99.99% and 56.30%, which was higher than that of nZVI (61.16%, 25.91%). Meanwhile, the particles were well characterized and the mechanism for enhanced reactivity and electron selectivity was investigated. Specially, both the morphology and BET specific surface area characterization suggested that stability against aggregation was higher in SL-nZVI nanoparticles than in nZVI. Besides, X-ray photoelectron spectroscopy (XPS), Tafel polarization curves, and Electrochemical impedance spectroscopy also indicated that the introduction of sophorolipid successfully prevent the nanoparticles from oxidation and benefit the electron transferring. In addition, a water contact angle test revealed that SL-nZVI nanoparticles were less hydrophilic (contact angle = 34.8°) than nZVI (contact angle = 23.9°). Therefore, in terms of reactivity, sophorolipid modification inhibited the aggregation of the nanoparticles and enhanced the electrical conductivity. For electron selectivity, the introduction of sophorolipid not only benefited Cr(VI) adsorption and the electron transfer from Fe to the surface-adsorbed Cr(VI) that followed but also reduced the possibility of side reactions between Fe and HO. This study demonstrates that the introduction of sophorolipid is an effective strategy for developing a highly efficient nZVI-based nanocomposite system and highlights the potential role of sophorolipid in improving the electron selectivity of nZVI.

摘要

纳米零价铁被认为是一种有前途的环境修复纳米结构,而在去除目标污染物的过程中提高纳米零价铁(nZVI)的电子选择性仍然是一个挑战(电子选择性定义为转移到目标污染物的电子数与 nZVI 提供的电子数之比)。在这项研究中,提出了通过神经酰胺(SL-nZVI)修饰来提高 nZVI 的反应性和电子选择性的策略。结果表明,SL-nZVI 对 Cr(VI) 的去除效率和电子选择性分别为 99.99%和 56.30%,高于 nZVI(61.16%和 25.91%)。同时,对颗粒进行了很好的表征,并研究了增强反应性和电子选择性的机制。特别地,形态和 BET 比表面积的特征表明,SL-nZVI 纳米颗粒的稳定性高于 nZVI,不易发生聚集。此外,X 射线光电子能谱(XPS)、塔菲尔极化曲线和电化学阻抗谱也表明,神经酰胺的引入成功地阻止了纳米颗粒的氧化,并有利于电子转移。此外,水接触角测试表明,SL-nZVI 纳米颗粒的亲水性(接触角=34.8°)低于 nZVI(接触角=23.9°)。因此,就反应性而言,神经酰胺修饰抑制了纳米颗粒的聚集并提高了导电性。对于电子选择性,神经酰胺的引入不仅有利于 Cr(VI)的吸附以及随后从 Fe 到表面吸附的 Cr(VI)的电子转移,而且还减少了 Fe 和 HO 之间的副反应的可能性。本研究表明,引入神经酰胺是开发高效 nZVI 基纳米复合材料系统的有效策略,并强调了神经酰胺在提高 nZVI 电子选择性方面的潜在作用。

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