Effects of synthesis temperature on ε-MnO2 microstructures and performance: Selective adsorption of heavy metals and the mechanism onto (100) facet compared with (001)
2022
Yang, Yuebei | Wang, Yaozhong | Li, Xiaofei | Xue, Chao | Dang, Zhi | Zhang, Lijuan | Yi, Xiaoyun
The heavy-metal adsorbent ε-MnO₂ was produced through a simple, one-step oxidation-reduction reaction at three different synthesis temperatures (25 °C, 50 °C and 75 °C) and their morphology and chemical-physical properties were compared. Of the three materials, MnO₂-25 had the largest specific surface area and the highest surface hydroxyl concentration. Its optimal performance was demonstrated by batch adsorption experiments with Pb²⁺, Cd²⁺ and Cu²⁺. Of the three metals, Pb²⁺ was adsorbed best (339.15 mg/g), followed by Cd²⁺ (107.50 mg/g) and Cu²⁺ (86.30 mg/g). When all three metals were present, Pb²⁺ was still absorbed best but now more Cu²⁺ was adsorbed than Cd²⁺. In order to explore the mechanism for the inconsistent adsorption order of Cd²⁺ and Cu²⁺ in single and competitive adsorption, we combined experimental data with density functional theory (DFT) calculations to elucidate the distinct adsorption nature of MnO₂-25 towards these three metals. This revealed that the adsorption affinity of the (100) facet was superior to (001), and since the surface complexes were also more stable on (100), this facet was most likely determining the adsorption order for the single metals. When the metals were present in combination, Pb²⁺ preferentially occupied the active adsorption sites of (100), forcing Cu²⁺ to be adsorbed on the (001) facet where Cd²⁺ was only poorly bound. Thus, the adsorption behavior was affected by MnO₂-25 surface chemistry at a molecular scale. This study provides an in-depth understanding of the adsorption mechanisms of the heavy metals on this adsorbent and offers theoretical guidance for production of adsorbent with improved removal efficiency.
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