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用于从水溶液中去除过量氟化物的新型MOF(Zr)负载MOF(Ce)吸附剂。

Novel MOF(Zr)-on-MOF(Ce) adsorbent for elimination of excess fluoride from aqueous solution.

作者信息

Song Jiangyan, Yu Yongyi, Han Xiaoshuai, Yang Weisen, Pan Wenbin, Jian Shaoju, Duan Gaigai, Jiang Shaohua, Hu Jiapeng

机构信息

Key Laboratory of Green Chemical Technology of Fujian Province University, Fujian Provincial Key Laboratory of Eco-Industrial Green Technology, Wuyi University, Wuyishan 354300, China; College of Environment and Safety Engineering, Fuzhou University, Fuzhou 350001, China.

Key Laboratory of Green Chemical Technology of Fujian Province University, Fujian Provincial Key Laboratory of Eco-Industrial Green Technology, Wuyi University, Wuyishan 354300, China; Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, China.

出版信息

J Hazard Mater. 2023 Oct 24;463:132843. doi: 10.1016/j.jhazmat.2023.132843.

Abstract

Herein, we used a one-pot method to fabricate a novel MOF-on-MOF adsorbent, namely MOF(Zr)-on-MOF(Ce). The adsorbent demonstrated a high maximum fluoride-ions capture capacity of 164.47 mg g. The morphology, elemental distribution, pore size distribution, and thermal stability were studied using SEM-EDS, XRD, BET, and TGA. The influence of the temperature, solution pH, fluoride concentration, and coexisting ions was explored using intermittent experiments. The results suggested that MOF(Zr)-on-MOF(Ce) had a fast capture rate for fluoride. MOF(Zr)-on-MOF(Ce) maintained an excellent fluoride removal performance over a wide pH range with an initial fluoride concentration of 20 mg L. The optimal effect was obtained at a pH of 4, but a high removal efficiency of 94% was maintained even at a pH of 9. Interference experiments showed that only the PO had an adverse inhibition influence. The field experiments demonstrated that MOF(Zr)-on-MOF(Ce) can keep the safety threshold levels of fluoride in drinking water. The Langmuir and pseudo-second order kinetic models were well fitted for the defluoridation process, demonstrating that the adsorption of fluoride ions on MOF(Zr)-on-MOF(Ce) was dominated by monolayer chemisorption. With the further characterization and kinetic thermodynamic studies indicates that the removal mechanism involves ion exchange, electrostatic interactions and complexation effect.

摘要

在此,我们采用一锅法制备了一种新型的MOF-on-MOF吸附剂,即MOF(Zr)-on-MOF(Ce)。该吸附剂表现出高达164.47 mg g的最大氟离子捕获容量。利用扫描电子显微镜-能谱仪(SEM-EDS)、X射线衍射仪(XRD)、比表面积分析仪(BET)和热重分析仪(TGA)研究了其形态、元素分布、孔径分布和热稳定性。通过间歇实验探究了温度、溶液pH值、氟浓度和共存离子的影响。结果表明,MOF(Zr)-on-MOF(Ce)对氟具有快速的捕获速率。在初始氟浓度为20 mg L的情况下,MOF(Zr)-on-MOF(Ce)在较宽的pH范围内保持了优异的除氟性能。在pH为4时获得了最佳效果,但即使在pH为9时仍保持了94%的高去除效率。干扰实验表明,只有磷酸根有不利的抑制影响。现场实验表明,MOF(Zr)-on-MOF(Ce)可以将饮用水中的氟保持在安全阈值水平。朗缪尔和准二级动力学模型很好地拟合了脱氟过程,表明氟离子在MOF(Zr)-on-MOF(Ce)上的吸附以单层化学吸附为主。进一步的表征和动力学热力学研究表明,去除机制涉及离子交换、静电相互作用和络合作用。

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