Advanced Porous Materials Unit (APMU), IMDEA Energy Institute, 28935, Móstoles, Madrid, Spain.
Department of Inorganic Chemistry, University of Granada, 18071, Granada, Spain.
Sci Rep. 2024 Apr 3;14(1):7882. doi: 10.1038/s41598-024-58014-w.
Pharmaceutical active compounds (PhACs) are some of the most recalcitrant water pollutants causing undesired environmental and human effects. In absence of adapted decontamination technologies, there is an urgent need to develop efficient and sustainable alternatives for water remediation. Metal-organic frameworks (MOFs) have recently emerged as promising candidates for adsorbing contaminants as well as providing photoactive sites, as they possess exceptional porosity and chemical versatility. To date, the reported studies using MOFs in water remediation have been mainly focused on the removal of a single type of PhACs and rarely on the combined elimination of PhACs mixtures. Herein, the eco-friendly bismuth-based MOF, SU-101, has been originally proposed as an efficient adsorbent-photocatalyst for the elimination of a mixture of three challenging persistent PhACs, frequently detected in wastewater and surface water in ng L to mg·L concentrations: the antibiotic sulfamethazine (SMT), the anti-inflammatory diclofenac (DCF), and the antihypertensive atenolol (At). Adsorption experiments of the mixture revealed that SU-101 exhibited a great adsorption capacity towards At, resulting in an almost complete removal (94.1 ± 0.8% for combined adsorption) in only 5 h. Also, SU-101 demonstrated a remarkable photocatalytic activity under visible light to simultaneously degrade DCF and SMT (99.6 ± 0.4% and 89.2 ± 1.4%, respectively). In addition, MOF-contaminant interactions, the photocatalytic mechanism and degradation pathways were investigated, also assessing the toxicity of the resulting degradation products. Even further, recycling and regeneration studies were performed, demonstrating its efficient reuse for 4 consecutive cycles without further treatment, and its subsequent successful regeneration by simply washing the material with a NaCl solution.
药物活性化合物(PhACs)是最难降解的水污染物之一,会对环境和人体造成不良影响。在缺乏适应性的净化技术的情况下,迫切需要开发高效、可持续的水修复替代方案。金属有机框架(MOFs)作为吸附污染物和提供光活性位点的候选材料,最近因其具有卓越的多孔性和化学多样性而备受关注。迄今为止,使用 MOFs 进行水修复的报道研究主要集中在去除单一类型的 PhACs 上,很少涉及 PhACs 混合物的联合去除。在这里,我们最初提出了一种环保的铋基 MOF,SU-101,作为一种高效的吸附-光催化剂,用于消除三种具有挑战性的持久性 PhACs 的混合物,这些 PhACs 经常在废水中和地表水中以纳克每升到毫克每升的浓度检测到:抗生素磺胺甲噁唑(SMT)、消炎药双氯芬酸(DCF)和抗高血压药阿替洛尔(At)。混合物的吸附实验表明,SU-101 对 At 表现出很强的吸附能力,仅在 5 小时内就实现了几乎完全去除(组合吸附的 94.1±0.8%)。此外,SU-101 在可见光下表现出显著的光催化活性,可同时降解 DCF 和 SMT(分别为 99.6±0.4%和 89.2±1.4%)。此外,还研究了 MOF-污染物相互作用、光催化机制和降解途径,并评估了产生的降解产物的毒性。甚至进一步进行了回收和再生研究,证明其在不进行进一步处理的情况下可连续重复使用 4 次,并通过简单地用 NaCl 溶液清洗材料即可成功再生。