Department of Civil and Environmental Engineering, Northwestern University, Evanston, IL 60208, USA.
Department of Civil and Environmental Engineering, Northwestern University, Evanston, IL 60208, USA.
Water Res. 2024 Sep 1;261:121998. doi: 10.1016/j.watres.2024.121998. Epub 2024 Jun 26.
The presence of active pharmaceutical ingredients (APIs) in wastewater effluents and natural aquatic systems threatens ecological and human health. While activated carbon-based adsorbents, such as GAC and PAC, are widely used for API removal, they exhibit certain deficiencies, including reduced performance due to the presence of natural organic macromolecules (NOMs) and high regeneration costs. There is growing demand for a robust, stable, and self-regenerative adsorbent designed for API removal in various environments. In this study, we synthesized a self-generating metal oxide nano-composite (S-MGC) containing titanium dioxide (TiO) and silicon dioxide (SiO) combined with 3D graphene oxide (GO) to adsorb APIs and undergo regeneration via light illumination. We determined optimal TiO:SiO:GO compositions for the S-MGCs through experiments using a model contaminant, methylene blue. The physical and chemical properties of S-MGCs were characterized, and their adsorption and photodegradation capabilities were studied using five model APIs, including sulfamethoxazole, carbamazepine, ketoprofen, valsartan, and diclofenac, both in single-component and multi-component mixtures. In the absence of TiO/SiO, 3D graphene oxide (CGB) displayed better adsorption performance compared to GAC, and S-MGCs further improve CGB's adsorption capacity. This performance remained consistent in two complex water environments: aqueous solutions at varying NOM levels and artificial urine. TiO supported on the GO surface exhibits similar photocatalytic activity to suspended TiO. In a continuous fixed-bed column test, S-MGCs demonstrated robust API adsorption performance that is maintained in the presence of NOM or urine, and can be regenerated through multiple cycles of adsorption and light illumination.
废水中活性药物成分 (API) 的存在以及自然水生系统威胁着生态和人类健康。虽然基于活性炭的吸附剂(如 GAC 和 PAC)被广泛用于 API 的去除,但它们存在一些缺陷,例如由于天然有机大分子 (NOM) 的存在而导致性能降低和高再生成本。人们越来越需要一种用于各种环境中 API 去除的稳健、稳定和自再生吸附剂。在这项研究中,我们合成了一种自生成金属氧化物纳米复合材料 (S-MGC),其中包含二氧化钛 (TiO) 和二氧化硅 (SiO),并与 3D 氧化石墨烯 (GO) 结合,用于吸附 API,并通过光照进行再生。我们通过使用模型污染物亚甲蓝的实验确定了 S-MGC 中 TiO:SiO:GO 的最佳组成。通过实验确定了 S-MGC 的物理和化学性质,并研究了它们在五种模型 API(包括磺胺甲恶唑、卡马西平、酮洛芬、缬沙坦和双氯芬酸)中的吸附和光降解能力,包括单一组分和多组分混合物。在没有 TiO/SiO 的情况下,3D 氧化石墨烯 (CGB) 的吸附性能优于 GAC,而 S-MGC 进一步提高了 CGB 的吸附能力。这种性能在两种复杂的水环境中保持一致:不同 NOM 水平的水溶液和人工尿液。负载在 GO 表面上的 TiO 表现出与悬浮 TiO 相似的光催化活性。在连续固定床柱试验中,S-MGC 表现出强大的 API 吸附性能,在存在 NOM 或尿液的情况下仍能保持,并且可以通过多次吸附和光照再生循环进行再生。