School of Environment, Tsinghua University, Beijing 100084, China.
Department of Civil Engineering, The University of Hong Kong, Pokfulam, Hong Kong SAR China.
Environ Sci Technol. 2024 Oct 15;58(41):18435-18445. doi: 10.1021/acs.est.4c06733. Epub 2024 Oct 1.
The detrimental environmental effects of surfactant-like contaminants (SLCs) with distinctive amphiphilic structures have garnered significant attention, particularly since perfluorooctanesulfonate was classified as a persistent organic pollutant. Despite the numerous absorbents developed for SLCs removal, the underlying interaction mechanisms remain speculative and lack experimental validation. To address this research gap, we elucidate the mechanistic insights into the selective removal of SLCs using mesoporous polydopamine nanospheres (MPDA) fabricated via a novel soft-template method. We employed low-field nuclear magnetic resonance to quantitatively characterize the hydrophilicity of the absorbents using water molecules as probes. The results demonstrated that MPDA with uniform mesopores exhibited a remarkable threefold enhancement in SLCs' adsorption capacity compared to conventional polydopamine particles via intraparticle diffusion. We further demonstrated the dominant effects of electrostatic and hydrophobic interactions on the selective removal of SLCs with MPDA by regulating the isoelectric pH value and performing a comparative analysis. The mechanism-inspired SLC-removal strategy achieved an average removal rate of 76.3% from highly contaminated wastewater. Our findings offer new avenues for applying MPDA as an efficient adsorbent and provide innovative and mechanistic insights for targeted SLC removal in complex wastewater matrices.
具有独特两亲结构的表面活性剂类污染物 (SLCs) 对环境的有害影响引起了人们的极大关注,尤其是全氟辛烷磺酸被归类为持久性有机污染物之后。尽管已经开发出许多用于去除 SLCs 的吸附剂,但潜在的相互作用机制仍存在推测,缺乏实验验证。为了解决这一研究空白,我们通过一种新的软模板法阐明了使用介孔聚多巴胺纳米球 (MPDA) 选择性去除 SLCs 的机制见解。我们使用低场核磁共振技术,通过水分子作为探针,定量表征了吸附剂的亲水性。结果表明,与传统的聚多巴胺颗粒相比,具有均匀介孔的 MPDA 通过颗粒内扩散表现出 SLCs 吸附容量显著提高了三倍。我们进一步通过调节等电 pH 值并进行比较分析,证明了 MPDA 对 SLCs 的选择性去除主要依赖于静电和疏水相互作用。受机制启发的 SLC 去除策略从高污染废水中实现了平均 76.3%的去除率。我们的研究结果为将 MPDA 用作高效吸附剂提供了新途径,并为复杂废水基质中目标 SLC 去除提供了创新和机制见解。