State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control, School of Environmental Science & Engineering, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China.
Department of Ocean Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China.
J Colloid Interface Sci. 2022 Dec 15;628(Pt B):807-818. doi: 10.1016/j.jcis.2022.08.093. Epub 2022 Aug 18.
Phosphate-induced water eutrophication has attracted global attention. Fabricating adsorbents with both high phosphate adsorption affinity and accessible separation property is challenging. Herein, PG@NZL, a hierarchical nanocomposite fibrous membrane, was fabricated via in-situ growth of La-doped NiZn-LDH (NiZnLa) over electrospun graphene oxide-polymer composite fibers (PG). The porous surface of the PG fibers provided abundant anchor sites for the vertical self-supported growth of NiZnLa nanosheets, contributing to a high surface area. The La-doped NiZnLa trimetallic LDH achieved a much higher adsorption capacity than NiZn-LDH. The negative adsorption energy (-1.45 eV), calculated with DFT, confirmed its spontaneous adsorption potential for phosphate. Interestingly, the PG fibers contributed to oxygen vacancies and the metal center electronic structure evolution of NiZnLa, thus strengthening the coordination with phosphate. Mechanistic analysis revealed that the high adsorption capacity of PG@NZL is attributed to its superior anion exchange property, oxygen vacancies, and inner-sphere complexation. Therefore, the flexible and easily separated PG@NZL nanocomposite fibrous membrane is a promising adsorbent for effectively treating phosphate-bearing wastewater.
磷酸盐引起的水体富营养化引起了全球关注。制备同时具有高磷酸盐吸附亲和力和可及的分离性能的吸附剂具有挑战性。在此,通过在静电纺丝氧化石墨烯-聚合物复合纤维 (PG) 上原位生长掺镧的 NiZn-LDH (NiZnLa) ,制备了分级纳米复合纤维膜 PG@NZL。PG 纤维的多孔表面为 NiZnLa 纳米片的垂直自支撑生长提供了丰富的锚定位点,有助于提高比表面积。与 NiZn-LDH 相比,掺杂 La 的 NiZnLa 三元 LDH 具有更高的吸附容量。用 DFT 计算出的负吸附能 (-1.45 eV) 证实了其对磷酸盐的自发吸附潜力。有趣的是,PG 纤维有助于 NiZnLa 的氧空位和金属中心电子结构演化,从而增强了与磷酸盐的配位。机理分析表明,PG@NZL 具有高吸附容量归因于其优越的阴离子交换性能、氧空位和内球络合。因此,这种灵活且易于分离的 PG@NZL 纳米复合纤维膜是一种很有前途的吸附剂,可有效处理含磷废水。