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氧化石墨烯和 Ni(II)在氧化铁上的吸附和共吸附:光谱和微观研究。

Adsorption and co-adsorption of graphene oxide and Ni(II) on iron oxides: A spectroscopic and microscopic investigation.

机构信息

School of Environment and Chemical Engineering, North China Electric Power University, Beijing 102206, PR China; College of Chemistry and Chemical Engineering, College of Life Science, Shaoxing University, Zhejiang 312000, PR China.

College of Chemistry and Chemical Engineering, College of Life Science, Shaoxing University, Zhejiang 312000, PR China.

出版信息

Environ Pollut. 2018 Feb;233:125-131. doi: 10.1016/j.envpol.2017.10.047. Epub 2017 Oct 20.

Abstract

Graphene oxide (GO) may strongly interact with toxic metal ions and mineral particles upon release into the soil environment. We evaluated the mutual effects between GO and Ni (Ni(II)) with regard to their adsorption and co-adsorption on two minerals (goethite and hematite) in aqueous phase. Results indicated that GO and Ni could mutually facilitate the adsorption of each other on both goethite and hematite over a wide pH range. Addition of Ni promoted GO co-adsorption mainly due to the increased positive charge of minerals and cation-π interactions, while the presence of GO enhanced Ni co-adsorption predominantly due to neutralization of positive charge and strong interaction with oxygen-containing functional groups on adsorbed GO. Increasing adsorption of GO and Ni on minerals as they coexist may thus reduce their mobility in soil. Extended X-ray absorption fine structure (EXAFS) spectroscopy data revealed that GO altered the microstructure of Ni on minerals, i.e., Ni formed edge-sharing surface species (at R∼3.2 Å) without GO, while a GO-bridging ternary surface complexes (at R∼2.49 Å and R∼4.23 Å) was formed with GO. These findings improved the understanding of potential fate and toxicity of GO as well as the partitioning processes of Ni ions in aquatic and soil environments.

摘要

氧化石墨烯(GO)在释放到土壤环境中后可能会与有毒金属离子和矿物质颗粒发生强烈相互作用。我们评估了 GO 和 Ni(Ni(II))之间在水相中的两种矿物质(针铁矿和赤铁矿)上的吸附和共吸附方面的相互影响。结果表明,在很宽的 pH 范围内,GO 和 Ni 都可以促进彼此在针铁矿和赤铁矿上的吸附。Ni 的添加主要促进了 GO 的共吸附,这主要是由于矿物质的正电荷增加和阳离子-π 相互作用所致,而 GO 的存在则主要由于正电荷的中和以及与吸附的 GO 上含氧官能团的强烈相互作用而促进了 Ni 的共吸附。因此,当 GO 和 Ni 共存时,它们在矿物质上的吸附增加可能会降低它们在土壤中的迁移性。扩展 X 射线吸收精细结构(EXAFS)光谱数据表明,GO 改变了 Ni 在矿物质上的微观结构,即 Ni 在没有 GO 的情况下形成了边缘共享的表面物种(在 R∼3.2Å 处),而在有 GO 的情况下形成了 GO 桥接的三元表面络合物(在 R∼2.49Å 和 R∼4.23Å 处)。这些发现提高了对 GO 的潜在命运和毒性以及 Ni 离子在水相和土壤环境中分配过程的理解。

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