Nan Wang, He Liang, Meng Zhang, Ruiping Liu*, Lina Li*, Li Zhao, Huijuan Liu and Jiuhui Qu,
{"title":"氟化物和碘化物在铁锰二元氧化物界面上的同步去除:竞争性吸附行为与机理","authors":"Nan Wang, He Liang, Meng Zhang, Ruiping Liu*, Lina Li*, Li Zhao, Huijuan Liu and Jiuhui Qu, ","doi":"10.1021/acsestengg.4c0017310.1021/acsestengg.4c00173","DOIUrl":null,"url":null,"abstract":"<p >The coexistence of high-concentration iodide (I<sup>–</sup>) and fluoride (F<sup>–</sup>) in high-iodine groundwater increases the occurrence of endemic diseases such as iodine-induced disorders and fluorosis, and their simultaneous removal has rarely been investigated. In this study, we developed cost-effective Fe/Mn binary oxides (FMBOs) with different Fe/Mn molar ratios (<i>R</i><sub>Fe:Mn</sub>) and investigated their performance and selective adsorption mechanisms for the synchronous removal of I<sup>–</sup> and F<sup>–</sup>. By optimizing the <i>R</i><sub>Fe:Mn</sub> ratios, an FMBO with <i>R</i><sub>Fe:Mn</sub> = 0.5:1 was developed to achieve synchronous removal of I<sup>–</sup> and F<sup>–</sup> with efficiencies of 67.7 and 80.7%, respectively, when the initial concentrations of I<sup>–</sup> and F<sup>–</sup> were 200 μg/L and 1.5 mg/L, and the FMBO dosage was 1.0 g/L. As the pH increases, the removal efficiency of I<sup>–</sup> and F<sup>–</sup> by FMBO decreases. According to the results of X-ray photoelectron spectroscopy (XPS), high-performance liquid chromatography–inductively coupled plasma mass spectrometry (HPLC-ICP/MS), and X-ray absorption spectroscopy results (XAS), FMBO is mainly composed of Fe(III), Mn(IV), and Mn(III). Mn oxide is mainly responsible for the heterogeneous oxidation of I<sup>–</sup>, whereas Fe oxide dominates in the adsorption of I<sup>–</sup> and F<sup>–</sup>. Based on density functional theory (DFT) calculations, the adsorption of SO<sub>4</sub><sup>2–</sup>, NO<sub>3</sub><sup>–</sup>, and HCO<sub>3</sub><sup>–</sup> was achieved via the formation of Fe–O bonds; moreover, the adsorption of I<sup>–</sup> and F<sup>–</sup> was attributed to the formation of Fe–I/F bonds. This study provides insight into the site-specific mechanism involved in I<sup>–</sup> and F<sup>–</sup> adsorption onto low-cost FMBO in realistic high-iodide groundwaters with complex coexisting anions.</p>","PeriodicalId":7008,"journal":{"name":"ACS ES&T engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synchronous Removal of Fluoride and Iodide on Fe–Mn Binary Oxides Interface: Competitive Adsorption Behaviors and Mechanism\",\"authors\":\"Nan Wang, He Liang, Meng Zhang, Ruiping Liu*, Lina Li*, Li Zhao, Huijuan Liu and Jiuhui Qu, \",\"doi\":\"10.1021/acsestengg.4c0017310.1021/acsestengg.4c00173\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The coexistence of high-concentration iodide (I<sup>–</sup>) and fluoride (F<sup>–</sup>) in high-iodine groundwater increases the occurrence of endemic diseases such as iodine-induced disorders and fluorosis, and their simultaneous removal has rarely been investigated. In this study, we developed cost-effective Fe/Mn binary oxides (FMBOs) with different Fe/Mn molar ratios (<i>R</i><sub>Fe:Mn</sub>) and investigated their performance and selective adsorption mechanisms for the synchronous removal of I<sup>–</sup> and F<sup>–</sup>. By optimizing the <i>R</i><sub>Fe:Mn</sub> ratios, an FMBO with <i>R</i><sub>Fe:Mn</sub> = 0.5:1 was developed to achieve synchronous removal of I<sup>–</sup> and F<sup>–</sup> with efficiencies of 67.7 and 80.7%, respectively, when the initial concentrations of I<sup>–</sup> and F<sup>–</sup> were 200 μg/L and 1.5 mg/L, and the FMBO dosage was 1.0 g/L. As the pH increases, the removal efficiency of I<sup>–</sup> and F<sup>–</sup> by FMBO decreases. According to the results of X-ray photoelectron spectroscopy (XPS), high-performance liquid chromatography–inductively coupled plasma mass spectrometry (HPLC-ICP/MS), and X-ray absorption spectroscopy results (XAS), FMBO is mainly composed of Fe(III), Mn(IV), and Mn(III). Mn oxide is mainly responsible for the heterogeneous oxidation of I<sup>–</sup>, whereas Fe oxide dominates in the adsorption of I<sup>–</sup> and F<sup>–</sup>. Based on density functional theory (DFT) calculations, the adsorption of SO<sub>4</sub><sup>2–</sup>, NO<sub>3</sub><sup>–</sup>, and HCO<sub>3</sub><sup>–</sup> was achieved via the formation of Fe–O bonds; moreover, the adsorption of I<sup>–</sup> and F<sup>–</sup> was attributed to the formation of Fe–I/F bonds. 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Synchronous Removal of Fluoride and Iodide on Fe–Mn Binary Oxides Interface: Competitive Adsorption Behaviors and Mechanism
The coexistence of high-concentration iodide (I–) and fluoride (F–) in high-iodine groundwater increases the occurrence of endemic diseases such as iodine-induced disorders and fluorosis, and their simultaneous removal has rarely been investigated. In this study, we developed cost-effective Fe/Mn binary oxides (FMBOs) with different Fe/Mn molar ratios (RFe:Mn) and investigated their performance and selective adsorption mechanisms for the synchronous removal of I– and F–. By optimizing the RFe:Mn ratios, an FMBO with RFe:Mn = 0.5:1 was developed to achieve synchronous removal of I– and F– with efficiencies of 67.7 and 80.7%, respectively, when the initial concentrations of I– and F– were 200 μg/L and 1.5 mg/L, and the FMBO dosage was 1.0 g/L. As the pH increases, the removal efficiency of I– and F– by FMBO decreases. According to the results of X-ray photoelectron spectroscopy (XPS), high-performance liquid chromatography–inductively coupled plasma mass spectrometry (HPLC-ICP/MS), and X-ray absorption spectroscopy results (XAS), FMBO is mainly composed of Fe(III), Mn(IV), and Mn(III). Mn oxide is mainly responsible for the heterogeneous oxidation of I–, whereas Fe oxide dominates in the adsorption of I– and F–. Based on density functional theory (DFT) calculations, the adsorption of SO42–, NO3–, and HCO3– was achieved via the formation of Fe–O bonds; moreover, the adsorption of I– and F– was attributed to the formation of Fe–I/F bonds. This study provides insight into the site-specific mechanism involved in I– and F– adsorption onto low-cost FMBO in realistic high-iodide groundwaters with complex coexisting anions.
期刊介绍:
ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources.
The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope.
Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.