Macroscopic and spectroscopic insights into the mutual interaction of graphene oxide, Cu(II), and Mg/Al layered double hydroxides

Macroscopic and spectroscopic insights into the mutual interaction of graphene oxide, Cu(II), and Mg/Al layered double hydroxides
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对氧化石墨烯、Cu(II) 和 Mg/Al 层状双氢氧化物相互作用的宏观和光谱见解

DOI:
10.1016/j.cej.2016.12.102
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发表时间:
2017-04
影响因子:
15.1
通讯作者:
Huang Yuying
Huang Yuying
中科院分区:
工程技术1区
文献类型:
--
作者:
Hu Baowei;Huang Chengcai;Li Xue;Sheng Guodong;Li Hui;Ren Xuemei;Ma Jingyuan;Wang Jin;Huang Yuying

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氧化石墨烯(GO)的环境行为和影响最近由于其快速生产和广泛应用而受到相当大的关注,因此其不可避免地释放到自然生态系统中,其中重金属和矿物颗粒通常共存。本工作首先旨在确定Cu(II)和GO与Mg/Al层状双氢氧化物(LDH)相互作用的相互影响。结果表明,Cu(II)和GO对LDH的共吸附具有交互增强作用。结果表明,GO与Cu(II)的共吸附主要是通过阳离子-π相互作用形成“LDH-Cu(II)-GO”三元表面络合物而增强的。同时,增加的Cu(II)与GO的共吸附主要源自通过Cu(II)与吸附的GO上的含O基团的相互作用形成“LDH-GO-Cu(II)”三元表面络合物(即,GO桥接)。EXAFS分析表明,GO可以显着抑制形成的外层配合物的Cu(II)在低pH值,而抑制形成的表面沉淀物在高pH值。增加吸收的GO和Cu(II)的矿物,因为它们共存可能会降低它们的流动性。这些新的见解提供了关于GO在真实的生态系统中的命运和风险以及生态环境中金属的自然净化的额外细节。
The environmental behavior and impact of graphene oxide (GO) has recently received considerable attention due to its rapid production and wide applications, and thus its inevitable release into the natural ecosystem, wherein heavy metals and mineral particles are generally co-existed. This work was firstly aimed to identify the mutual effect of Cu(II) and GO interaction with Mg/Al layered double hydroxides (LDH). The results demonstrate that Cu(II) and GO exhibited interactively enhancement roles in their co-adsorption on LDH. Namely, enhanced co-adsorption of GO with Cu(II) was mainly ascribed from formation of “LDH-Cu(II)-GO” ternary surface complexes via cation–π interaction. Meanwhile, increased co-adsorption of Cu(II) with GO was primarily derived from formation of “LDH-GO-Cu(II)” ternary surface complexes through interaction of Cu(II) with O-bearing groups on adsorbed GO (i.e., GO-bridging). EXAFS analysis indicates that GO could significantly inhibit formation of outer-sphere complexes for Cu(II) at low pH, while suppress formation of surface precipitates at high pH. Increased uptake of GO and Cu(II) on minerals as they co-exist may decrease their mobility. These new insights provide additional details to be considered concerning the fate and risk of GO in real ecosystem, as well as the natural purification of metals in ecological environments.
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