电子转移
零价铁
选择性
化学
反应性(心理学)
四溴双酚A
生物炭
溶剂
动力学同位素效应
粒子(生态学)
化学工程
光化学
吸附
有机化学
催化作用
病理
阻燃剂
热解
氘
量子力学
工程类
地质学
医学
物理
替代医学
海洋学
作者
Fan Gao,Mingyi Zhang,Shakeel Ahmad,Jiaming Guo,Yinghao Shi,Xinzuo Yang,Jingchun Tang
标识
DOI:10.1016/j.jhazmat.2023.132028
摘要
Post-sulfidated nanoscale zero-valent iron with a controlled FeSX shell thickness deposited on biochar (S-nZVI/BC) was synthesized to degrade tetrabromobisphenol A (TBBPA). Detailed characterizations revealed that the increasing sulfidation degree altered shell thickness/morphology, S content/speciation/distribution, hydrophobicity, and electron transfer capacity. Meanwhile, the BC improved electron transfer capacity and hydrophobicity and inhibited the surface oxidation of S-nZVI. These properties endowed S-nZVI/BC with highly reactive (∼8.9–13.2 times) and selective (∼58.4–228.9 times) over nZVI/BC in TBBPA transformation. BC modification improved the reactivity and selectivity of S-nZVI by 1.77 and 1.96 times, respectively. The difference of S-nZVI/BC in reactivity was related to hydrophobicity and electron transfer, particularly FeSX shell thickness and morphology. Optimal shell thickness of ∼32 nm allowed the maximum association between Fe0 core and exterior FeSX, resulting in superior reactivity. A thicker shell with abundant networks increased the roughness but decreased the surface area and electron transfer. The higher [S/Fe]surface and [S/Fe]particle were conducive to the selectivity, and [S/Fe]particle was more influential than [S/Fe]surface on selectivity upon similar hydrophobicity. The solvent kinetic isotope effects (SKIEs) exhibited that increasing [S/Fe]dose tuned the relative contributions of atomic H and electron in TBBPA debromination but failed to alter the dominant debromination pathway (i.e., direct electron transfer) in (S)-nZVI/BC systems. Mechanism of electron transfer rather than atomic H contributed to higher selectivity. This work demonstrated that S-nZVI/BC was a prospective material for the remediation of TBBPA-contaminated groundwater.
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