Key Laboratory of Western China's Environmental Systems (Ministry of Education) and Key Laboratory for Environmental Pollution Prediction and Control, Gansu Province, College of Earth and Environmental Sciences, Lanzhou University, Lanzhou, 730000, People's Republic of China.
Environ Sci Pollut Res Int. 2022 Mar;29(15):21561-21575. doi: 10.1007/s11356-021-17258-z. Epub 2021 Nov 11.
Ferrihydrite often precipitates with humic acid in natural ways, affecting the fate of lead ions, the stabilization of humic acid, and the aging process of ferrihydrite. A series of 2-line ferrihydrite-humic (Fh-HA) acid with varying C loadings has been prepared, the morphology and surface properties of Fh-HA organo-minerals have been characterized, and the adsorption property of Pb ions onto Fh-HA has been studied. The results indicated that a strong interference of HA to ferrihydrite 2-line Fh dominated mineral phase in all samples, but with increasing C/Fe molar ratios, the crystallinity gradually weakened, particles became smaller, and SSA decreased significantly. The data of Mössbauer spectra confirmed C loadings changed the unit structure of ferrihydrite. Fh-HA performed good adsorption properties to Pb (II): high efficiency and big capacity, especially Fh-HA_2.0. pH had great effect on Pb (II) sorption, the pH change affects not only the amounts of competitive ions in solutions, but also the dissociation and protonation of functional groups on the surface of Fh-HA. Sorption kinetics can be well modeled by a pseudo-second-order model, and the process was controlled by film and intraparticle adsorption simultaneously. The adsorption isotherms can be well described by Freundlich isotherm model. The detailed determination results of Fe 2p, O 1 s, and Pb 4f spectra before and after lead adsorption showed mononuclear bidentate or binuclear bidentate ligands occurring on Fh-HA surface, forming stable inner-sphere complex. By comparison of Mössbauer spectra and TEM images, with aging time, a slower evolution of iron oxide/oxyhydroxide phases in Fh-HA-Pb system happened compared to pure ferrihydrite. Ferrihydrite has transformed to a combination of ferrihydrite, goethite, and hematite phases. In this study, the determination of C-Fe interaction, Pb fate influenced by Fh-HA, and transformation of ferrihydrite would have a great implication to application of Fh-HA precipitates in remediation for surface water or groundwater polluted by heavy metals.
天然条件下,针铁矿常常与腐殖酸共同沉淀,影响铅离子的命运、腐殖酸的稳定和针铁矿的老化过程。本研究制备了一系列不同 C 负载量的 2 线针铁矿-腐殖酸(Fh-HA)有机矿物,对 Fh-HA 有机矿物的形貌和表面性质进行了表征,并研究了 Pb 离子在 Fh-HA 上的吸附特性。结果表明,HA 对所有样品中 2 线 Fh 主导的针铁矿主矿物相具有很强的干扰作用,但随着 C/Fe 摩尔比的增加,结晶度逐渐减弱,颗粒变小,比表面积显著降低。穆斯堡尔谱数据证实 C 负载量改变了针铁矿的单元结构。Fh-HA 对 Pb(II)表现出良好的吸附性能:高效率和大容量,特别是 Fh-HA_2.0。pH 值对 Pb(II)的吸附有很大影响,pH 值的变化不仅影响溶液中竞争离子的数量,而且影响 Fh-HA 表面官能团的解离和质子化。吸附动力学可以很好地用拟二级模型来模拟,该过程同时受膜和颗粒内吸附的控制。吸附等温线可以很好地用 Freundlich 等温模型来描述。Pb 吸附前后 Fe 2p、O 1s 和 Pb 4f 谱的详细测定结果表明,Fh-HA 表面发生单核双齿或双核双齿配体,形成稳定的内圈络合物。通过比较穆斯堡尔谱和 TEM 图像,随着老化时间的增加,Fh-HA-Pb 体系中铁氧化物/氢氧化物相的演变比纯针铁矿要慢。针铁矿已转变为针铁矿、针铁矿和赤铁矿的组合相。在本研究中,确定 C-Fe 相互作用、Fh-HA 影响下的 Pb 命运以及针铁矿的转化,对于 Fh-HA 沉淀在修复受重金属污染的地表水或地下水方面的应用具有重要意义。