共沉淀
化学
氢氧化物
吸附
选择性
傅里叶变换离子回旋共振
无机化学
纳米颗粒
核化学
腐植酸
质谱法
有机化学
化学工程
色谱法
催化作用
工程类
肥料
作者
Shishu Zhu,Wendan Luo,Yijun Mo,Kengbo Ding,Miaoyue Zhang,Chao Jin,Shizhong Wang,Yuanqing Chao,Yetao Tang,Rongliang Qiu
标识
DOI:10.1021/acs.est.3c03279
摘要
Coprecipitation of Fe/Cr hydroxides with natural organic matter (NOM) is an important pathway for Cr immobilization. However, the role of NOM in coprecipitation is still controversial due to its molecular heterogeneity and diversity. This study focused on the molecular selectivity of NOM toward Fe/Cr coprecipitates to uncover the fate of Cr via Fourier transform-ion cyclotron resonance-mass spectrometry (FT-ICR-MS). The results showed that the significant effects of Suwannee River NOM (SRNOM) on Cr immobilization and stability of the Fe/Cr coprecipitates did not merely depend on the adsorption of SRNOM on Fe/Cr hydroxides. FT-ICR-MS spectra suggested that two pathways of molecular selectivity of SRNOM in the coprecipitation affected Cr immobilization. Polycyclic aromatics and polyphenolic compounds in SRNOM preferentially adsorbed on the Fe/Cr hydroxide nanoparticles, which provided extra binding sites and promoted the aggregation. Notably, some specific compounds (i.e., polyphenolic compounds and highly unsaturated phenolic compounds), less unsaturated and more oxygenated than those adsorbed on Fe/Cr hydroxide nanoparticles, were preferentially incorporated into the insoluble Cr–organic complexes in the coprecipitates. Kendrick mass defect analysis revealed that the insoluble Cr–organic complexes contained fewer carbonylated homologous compounds. More importantly, the spatial distribution of insoluble Cr–organic complexes was strongly related to Cr immobilization and stability of the Fe/Cr-NOM coprecipitates. The molecular information of the Fe/Cr-NOM coprecipitates would be beneficial for a better understanding of the transport and fate of Cr and exploration of the related remediation strategy.
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