School of Life Science, Shaoxing University, Huancheng West Road 508, Shaoxing, 312000, PR China.
School of Life Science, Shaoxing University, Huancheng West Road 508, Shaoxing, 312000, PR China.
Chemosphere. 2021 Jul;274:129743. doi: 10.1016/j.chemosphere.2021.129743. Epub 2021 Jan 27.
The recovery of uranium from wastewater and safe treatment of U(VI)-containing wastewater are of great important to ensure the sustainable development of nuclear-related energy. Although abundant studies of U(VI) sorption on various adsorbents have been widely achieved, U(VI) sorption at extreme pH and trace concentration is challenging issues due to limited sorption activity of natural adsorbents. The development of novel materials with highly efficient and excellent selectivity for capturing U(VI) from nuclear-related wastewater and seawater is highly desirable. In this study, amidoxime/carbon nitride (AO/g-CN) was fabricated and captured U(VI) under a variety of water chemistry. We demonstrated that AO/g-CN exhibited the high adsorption capacities (312 mg/g at pH 6.8), fast removal equilibrium (>98% at 10 min) and superior selectivity for U(VI) compared with the other radionuclides (e.g., 19.76 mg/g of Cs(I)). In addition, AO/g-CN exhibited the high uranium extraction capacity from natural seawater (9.55 mg/g at saturation time of 5.5 days) compared to vanadium (1.85 mg/g). U(VI) adsorption behavior at different pH can be excellently fitted by the surface complexation modeling with three inner sphere surface complexes (i.e., SOUO(CO), SO(UO)(OH) and SOUO species). According to XPS (X-ray Photoelectron Spectroscopy) analysis, the strong complexation of U(VI) with AO groups retained in CN nanosheet. The split of U-O subshell and the occurrence of U-C shell further demonstrated inner-sphere surface complexation by EXAFS (X-Ray Absorption Fine Structure) spectra analyses. These results revealed that the high potential of AO/g-CN materials for selective U(VI) capture from wastewater and seawater.
从废水中回收铀并安全处理含 U(VI)的废水对于确保与核能相关的能源的可持续发展非常重要。尽管已经广泛研究了各种吸附剂对 U(VI)的吸附,但由于天然吸附剂的吸附活性有限,在极端 pH 和痕量浓度下的 U(VI)吸附仍然是具有挑战性的问题。因此,开发具有高效和优异选择性的新型材料,用于从与核能相关的废水中和海水中捕获 U(VI)是非常可取的。在本研究中,制备了偕胺肟/氮化碳 (AO/g-CN),并在各种水化学条件下捕获 U(VI)。我们证明,与其他放射性核素(例如 Cs(I) 的 19.76mg/g)相比,AO/g-CN 对 U(VI)具有高吸附容量(pH 6.8 时为 312mg/g)、快速去除平衡(10min 内>98%)和优异的选择性。此外,与钒(1.85mg/g)相比,AO/g-CN 从天然海水中具有较高的铀提取能力(饱和时间为 5.5 天时为 9.55mg/g)。不同 pH 下的 U(VI)吸附行为可以通过三个内球表面络合物(即 SOUO(CO)、SO(UO)(OH)和 SOUO 物种)的表面络合模型得到很好的拟合。根据 XPS(X 射线光电子能谱)分析,保留在 CN 纳米片中的 AO 基团与 U(VI)的强络合作用。U-O 亚壳层的分裂和 U-C 壳层的出现进一步通过 EXAFS(X 射线吸收精细结构)谱分析证明了内球表面络合作用。这些结果表明,AO/g-CN 材料具有从废水中和海水中选择性捕获 U(VI)的高潜力。