Probing the intermolecular interaction mechanisms between humic acid and different substrates with implications for its adsorption and removal in water treatment

化学 吸附 腐植酸 疏水效应 DLVO理论 相互作用能 单层 粘附 氢键 化学工程 水溶液 分子间力 静电学 静电相互作用 分子 有机化学 化学物理 物理化学 胶体 肥料 生物化学 工程类
作者
Lei Xie,Qiuyi Lu,Xiaohui Mao,Jingyi Wang,Linbo Han,Junqing Hu,Qingye Lu,Yixiang Wang,Hongbo Zeng
出处
期刊:Water Research [Elsevier BV]
卷期号:176: 115766-115766 被引量:60
标识
DOI:10.1016/j.watres.2020.115766
摘要

Humic substance is a ubiquitous class of natural organic matter (NOM) in soil and aquatic ecosystems, which severely affects the terrestrial and aquatic environments as well as water-based engineering systems by adsorption on solids (e.g., soil minerals, nanoparticles, membranes) via different interaction mechanisms. Herein, the chemical force microscopy (CFM) technique was employed to quantitatively probe the intermolecular forces of humic acid (HA, a representative humic substance) interacting with self-assembled monolayers (SAMs, i.e., OH-SAMs, CH3-SAMs, NH2-SAMs and COOH-SAMs) in various aqueous environments at the nanoscale. The interaction forces measured during approach could be well fitted by the extended Derjaguin-Landau-Verwey-Overbeek (DLVO) theory by incorporating the hydrophobic interaction. The average adhesion energy followed the trend as: NH2-SAMs (∼3.11 mJ/m2) > CH3-SAMs (∼2.03 mJ/m2) > OH-SAMs (∼1.38 mJ/m2) > COOH-SAMs (∼0.52 mJ/m2) in 100 mM NaCl at pH 5.8, indicating the significant role of electrostatic attraction in contributing to the HA adhesion, followed by hydrophobic interaction and hydrogen bonding. The adhesion energy was found to be dependent on NaCl concentration, Ca2+ addition and pH. For the interaction between NH2-SAMs and HA, their electrostatic attraction at pH 5.8 turned to repulsion under alkaline condition which led to the sudden drop of adhesion energy. Such results promised the adsorption and release of HA using the recyclable magnetic Fe3O4 nanoparticles coated with (3-aminopropyl)tiethoxysilane (APTES). This work provides quantitative information on the molecular interaction mechanism underlying the adsorption of HA on solids of varying surface chemistry at the nanoscale, with useful implications for developing effective chemical additives to remove HA in water treatment and many other engineering processes.
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