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采用 MgO 和琥珀酸形貌控制合成 MgFe-LDH 以增强砷吸附:动力学、平衡和机理研究。

Morphologically controlled synthesis of MgFe-LDH using MgO and succinic acid for enhanced arsenic adsorption: Kinetics, equilibrium, and mechanism studies.

机构信息

Graduate school of Creative Science and Engineering, Waseda University, Okubo 3-4-1, Shinjuku, Tokyo, 169-8555, Japan.

Department of Marine Resources and Energy, Tokyo University of Marine Science and Technology, 4‑5‑7 Konan, Minato‑Ku, Tokyo 108‑8477, Japan.

出版信息

J Environ Sci (China). 2025 Feb;148:637-649. doi: 10.1016/j.jes.2024.01.049. Epub 2024 Feb 10.

Abstract

In this study, we investigated improving the performance of a layered double hydroxide (LDH) for the adsorption of As(III) and As(V) by controlling the morphology of LDH crystals. The LDH was synthesized via a simple coprecipitation method using barely soluble MgO as a precursor and succinic acid (SA) as a morphological control agent. Doping the LDH crystals with carboxylate ions (RCOO) derived from SA caused the crystals to develop in a radial direction. This changed the pore characteristics and increased the density of active surface sites. Subsequently, SA/MgFe-LDH showed excellent affinity for As(III) and As(V) with maximum sorption densities of 2.42 and 1.60 mmol/g, respectively. By comparison, the pristine MgFe-LDH had sorption capacities of 1.56 and 1.31 mmol/g for As(III) and As(V), respectively. The LDH was effective over a wide pH range for As(III) adsorption (pH 3-8.5) and As(V) adsorption (pH 3-6.5). Using a combination of spectroscopy and sorption modeling calculations, the main sorption mechanism of As(III) and As(V) on SA/MgFe-LDH was identified as inner-sphere complexation via ligand exchange with hydroxyl group (-OH) and RCOO. Specifically, bidentate As-Fe complexes were proposed for both As(III) and As(V) uptake, with the magnitude of formation varying with the initial As concentration. Importantly, the As-laden adsorbent had satisfactory stability in simulated real landfill leachate. These findings demonstrate that SA/MgFe-LDH exhibits considerable potential for remediation of As-contaminated water.

摘要

在这项研究中,我们通过控制层状双氢氧化物(LDH)晶体的形态,研究了如何提高其对 As(III)和 As(V)的吸附性能。该 LDH 是通过简单的共沉淀法合成的,使用难溶的 MgO 作为前体,琥珀酸(SA)作为形态控制剂。LDH 晶体中掺杂来自 SA 的羧酸盐离子(RCOO)会导致晶体沿径向生长。这改变了孔隙特征并增加了活性表面位点的密度。随后,SA/MgFe-LDH 对 As(III)和 As(V)表现出优异的亲和力,最大吸附密度分别为 2.42 和 1.60 mmol/g。相比之下,原始的 MgFe-LDH 对 As(III)和 As(V)的吸附容量分别为 1.56 和 1.31 mmol/g。该 LDH 在较宽的 pH 范围内(pH 3-8.5 用于 As(III)吸附,pH 3-6.5 用于 As(V)吸附)对 As(III)吸附有效。通过光谱和吸附模型计算的结合,确定了 As(III)和 As(V)在 SA/MgFe-LDH 上的主要吸附机制是通过与羟基(-OH)和 RCOO 的配体交换进行内球络合。具体来说,对于 As(III)和 As(V)的摄取,提出了双齿 As-Fe 配合物,其形成的大小随初始 As 浓度的变化而变化。重要的是,负载 As 的吸附剂在模拟真实垃圾渗滤液中具有令人满意的稳定性。这些发现表明,SA/MgFe-LDH 对受 As 污染的水的修复具有相当大的潜力。

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