School of Resource & Environment and Safety Engineering, University of South China, Hengyang 421001, China.
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China.
Int J Biol Macromol. 2023 May 31;238:124074. doi: 10.1016/j.ijbiomac.2023.124074. Epub 2023 Mar 20.
A novel chitosan-based porous composite adsorbent with multifunctional groups, such as phosphoric acid, amidoxime, and quaternary ammonium groups, was prepared to improve the adsorption rate and competitive uranium‑vanadium adsorption of amidoxime group adsorbents. The maximum uranium adsorption capacity of PACNC was 962.226 mg g at 308 K and pH = 7. The maximum adsorption rate constant of PACNC for uranium was 2.83E-2 g mg min, which is 2.38 times that of ACNC (1.19E-2 g mg min). Moreover, the adsorption equilibrium time was shortened from 300 (ACNC) to 50 (PACNC) min. In simulated and real seawater, the K and adsorption capacity of PACNC for uranium were approximately 8 and 6.62 times those for vanadium, respectively. These results suggest that phosphorylation significantly improved the competitive adsorption of uranium‑vanadium and uranium adsorption rate. PACNC also exhibited good recycling performance and maintained stable adsorption capacity after five cycles. DFT calculations were used to analyze and calculate the possible co-complex structure of PACNC and uranium. The binding structure of phosphate and amidoxime is the most stable, and its synergistic effect effectively improves the competitive adsorption of uranium-vanadium of amidoxime. All the results demonstrated that PACNC has substantial application potential for uranium extraction from seawater.
一种新型的壳聚糖基多孔复合材料吸附剂,具有多功能基团,如磷酸基、偕胺肟基和季铵基,用于提高偕胺肟基吸附剂的吸附速率和竞争铀-钒吸附性能。在 308 K 和 pH = 7 时,PACNC 的最大铀吸附容量为 962.226mg/g。PACNC 对铀的最大吸附速率常数为 2.83E-2g/mg/min,是 ACNC(1.19E-2g/mg/min)的 2.38 倍。此外,吸附平衡时间从 300min(ACNC)缩短至 50min(PACNC)。在模拟海水和实际海水中,PACNC 对铀的 K 和吸附容量分别是对钒的 8 倍和 6.62 倍。这些结果表明,磷酸化显著提高了铀-钒的竞争吸附和铀的吸附速率。PACNC 还表现出良好的循环性能,经过五次循环后仍保持稳定的吸附容量。DFT 计算用于分析和计算 PACNC 和铀的可能共配合物结构。磷酸根和偕胺肟基的结合结构最稳定,其协同效应有效提高了偕胺肟基对铀-钒的竞争吸附性能。所有结果表明,PACNC 具有从海水中提取铀的巨大应用潜力。