Li Jingrui, Gong Aijun, Li Fukai, Qiu Lina, Zhang Weiwei, Gao Ge, Liu Yu, Li Jiandi
School of Chemistry and Biological Engineering, University of Science and Technology Beijing Beijing 100083 China
Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, University of Science and Technology Beijing Beijing 100083 China.
RSC Adv. 2018 Nov 22;8(68):39149-39161. doi: 10.1039/c8ra07762b. eCollection 2018 Nov 16.
In this study, novel magnetic mesoporous FeO@mSiO-DODGA nanoparticles were prepared for efficiently adsorbing and recycling REEs. FeO@mSiO-DODGA was characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), vibrating sample magnetometry (VSM), Fourier transform infrared spectroscopy (FT-IR) and thermogravimetric analysis (TGA). The adsorption behavior of FeO@mSiO-DODGA was investigated by ICP-OES. The results showed that the content of DODGA in the adsorbent was 367 μmol g. FeO@mSiO-DODGA exhibited the highest adsorption rates for 15 REEs, except Tm, in a 2 mol L nitric acid solution. Among these elements, the adsorption rates for Nd, Sm, Eu, Dy, Ho, Yb, Lu, Y and Sc ranged from 85.1% to 100.1%. The desorption rates for all 16 REE ions reached their maximum values when 0.01 mol L EDTA was used as the eluent. The desorption rates for Nd, Ce, Sm, Eu, Ho, Yb, Lu, Y, and Sc were 87.7-99.8%. FeO@mSiO-DODGA had high stability in 2 mol L HNO and could be used five times without significant loss of adsorption capacity. Moreover, these nanoparticles had high selectivity, and their adsorption rate was not affected even in a high-concentration solution of a coexisting ion. Therefore, 8 REE ions (Nd, Sm, Eu, Ho, Yb, Lu, Y, and Sc) were selected for the study of adsorption kinetics and adsorption isotherm experiments. It was demonstrated that the values of (equilibrium adsorption capacity) for Nd, Sm, Eu, Ho, Yb, Lu, Y, and Sc were 14.28-60.80 mg g. The adsorption of REEs on FeO@mSiO-DODGA followed the pseudo-second-order kinetic model, Elovich model and Langmuir isotherm model, which indicated that the adsorption process of FeO@mSiO-DODGA for REEs comprised single-layer adsorption on a non-uniform surface controlled by chemical adsorption. It was concluded that FeO@mSiO-DODGA represents a new material for the adsorption of REEs in strongly acidic solutions.
在本研究中,制备了新型磁性介孔FeO@mSiO-DODGA纳米颗粒,用于高效吸附和回收稀土元素。采用粉末X射线衍射(XRD)、透射电子显微镜(TEM)、振动样品磁强计(VSM)、傅里叶变换红外光谱(FT-IR)和热重分析(TGA)对FeO@mSiO-DODGA进行了表征。通过电感耦合等离子体发射光谱法(ICP-OES)研究了FeO@mSiO-DODGA的吸附行为。结果表明,吸附剂中DODGA的含量为367 μmol/g。在2 mol/L硝酸溶液中,FeO@mSiO-DODGA对15种稀土元素(除铥外)表现出最高的吸附率。在这些元素中,钕、钐、铕、镝、钬、镱、镥、钇和钪的吸附率在85.1%至100.1%之间。当使用0.01 mol/L乙二胺四乙酸(EDTA)作为洗脱剂时,所有16种稀土离子的解吸率均达到最大值。钕、铈、钐、铕、钬、镱、镥、钇和钪的解吸率为87.7-99.8%。FeO@mSiO-DODGA在2 mol/L硝酸中具有高稳定性,可重复使用5次而吸附容量无明显损失。此外,这些纳米颗粒具有高选择性,即使在共存离子的高浓度溶液中,其吸附率也不受影响。因此,选择8种稀土离子(钕、钐、铕、钬、镱、镥、钇和钪)进行吸附动力学和吸附等温线实验研究。结果表明,钕、钐、铕、钬、镱、镥、钇和钪的平衡吸附容量值为14.28-60.80 mg/g。稀土元素在FeO@mSiO-DODGA上的吸附遵循准二级动力学模型、埃洛维奇模型和朗缪尔等温线模型,这表明FeO@mSiO-DODGA对稀土元素的吸附过程包括在非均匀表面上由化学吸附控制的单层吸附。研究得出结论,FeO@mSiO-DODGA是一种用于在强酸性溶液中吸附稀土元素的新型材料。