School of Chemical Science and Engineering, Shanghai Key Lab of Chemical Assessment and Sustainability, Tongji University, Shanghai 200092, China.
Environ Sci Technol. 2021 Feb 16;55(4):2618-2627. doi: 10.1021/acs.est.0c07106. Epub 2021 Jan 6.
The development of a selective removal method for group-targets of pollutants under the inhibition of nontoxic organic interferents is of great importance in environmental science. A novel TiO photoelectrode functionalized with dummy templates (PS-PAE-TiO) is designed, exhibiting group-targeting selectivity for nine phthalate ester (PAE) analogs. In total, 90-99% of PAEs were removed from 30 μg L in actual wastewater (chemical oxygen demand, 14.5 mg O L). The selectivity for PAEs originated from preferential enrichment close to the PS-PAE-TiO surface result in a twofold improvement in the apparent kinetic constant. The specific sites can be attributed to phenyl rings and -ester carbonyl groups through the molecular recognition process. The intermediates were analyzed quantitatively, and a degradation pathway with lower toxicity was proposed, excluding ring-hydroxylated phthalates. Almost 100% of the estrogenic activity and acute aquatic toxicity were eliminated and the genotoxicity was reduced by 92.5%, which was about 40% higher than that at the nonselective photoanode. An enhanced removal at the PS-PAE-TiO photoanode with better economic benefits was confirmed, saving energy consumption by 2.5 kWh m per order than that at the nonselective anode. The advanced removal method with group-targeting selective capability can provide a propagable strategy for the removal of a class of homologues from complex aqueous systems.
开发一种在无毒有机干扰物抑制下针对污染物进行组目标选择性去除的方法,在环境科学中具有重要意义。设计了一种新型 TiO2 光电化学电极,功能化有虚拟模板(PS-PAE-TiO),对 9 种邻苯二甲酸酯(PAE)类似物具有组目标选择性。在实际废水中(化学需氧量为 14.5 mg O/L),从 30 μg/L 的废水中去除了 90-99%的 PAEs。对 PAEs 的选择性来源于优先富集在 PS-PAE-TiO 表面附近,从而使表观动力学常数提高了两倍。特定的吸附位可以归因于苯环和 -酯羰基,通过分子识别过程。对中间产物进行了定量分析,并提出了一种毒性较低的降解途径,排除了环状羟化邻苯二甲酸酯。几乎消除了 100%的雌激素活性和急性水生毒性,遗传毒性降低了 92.5%,比非选择性光电阳极高约 40%。在 PS-PAE-TiO 光电阳极上进行了增强去除,具有更好的经济效益,比非选择性阳极每阶节省 2.5 kWh m 的能耗。具有组目标选择性去除能力的先进去除方法可为从复杂水系统中去除一类同系物提供一种可推广的策略。