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一种新型杂化MIL-53(Al)@稻壳用于水中草甘膦吸附的研究:过程特性与机理

Application of a novel hybrid MIL-53(Al)@rice husk for the adsorption of glyphosate in water: Characteristics and mechanism of the process.

作者信息

Zambrano-Intriago Luis Angel, Daza-López Erlinjka Valentina, Fernández-Andrade Alex, Luque Rafael, Amorim Célia G, Araújo Alberto N, Rodríguez-Díaz Joan Manuel, Montenegro Maria C B S M

机构信息

LAQV-REQUIMTE/Departamento de Ciências Químicas, Faculdade de Farmácia - Universidade Do Porto, R. Jorge Viterbo Ferreira, 228, 4050-313, Porto, Portugal; Laboratorio de Análisis Químicos y Biotecnológicos, Instituto de Investigación, Universidad Técnica de Manabí, Portoviejo, 130105, Ecuador.

Programa de Posgrado en Ingeniería Química, Instituto de Posgrado, Universidad Técnica de Manabí, S/N, Avenida Urbina y Che Guevara, Portoviejo, 130104, Ecuador.

出版信息

Chemosphere. 2023 Jun;327:138457. doi: 10.1016/j.chemosphere.2023.138457. Epub 2023 Mar 20.

DOI:10.1016/j.chemosphere.2023.138457
PMID:36948257
Abstract

The development of new materials that have a high capacity to remove pollutants in water-based media is becoming increasingly important because of the serious contamination of water and the negative impact on biodiversity and public health. The presence of glyphosate in water, the most widely used herbicide worldwide, has triggered alerts owing to the collateral effects it may cause on human health. The main objective of the present study was to investigate the potential of the hybrid material MIL-53(Al)@RH for the adsorption of glyphosate in aqueous solution. The material was obtained following the methodology of MIL-53(Al) synthesis in the presence of hydrolyzed rice husk assisted by microwave. Batch adsorption experiments were carried out to evaluate the adsorbent dosage, pH solution effect, contact time, adsorbate concentration, and temperature effect. The results demonstrated that a maximum adsorption capacity of 296.95 mg g, at pH 4 with a ratio of 0.04 g MIL-53(Al)@RH/50 mL of solution, was achieved in 30 min. The Avrami and pseudo-second order models appropriately described the adsorption kinetics and the equilibrium by Langmuir and Sips models. The enthalpy changes (ΔH°) determined propose an endothermic reaction governed by chemisorption, corroborating the kinetic and equilibrium settings. Hydrogen bonds, π*-π interactions, and complexation between the metal centers of MIL-53(Al) and the anionic groups of glyphosate were postulated to be involved as adsorption mechanisms. Finally, for practical application, MIL-53(Al)@RH was packed in a column for a fixed-bed test which revealed that the hybrid can remove glyphosate with an adsorption capacity of 76.304 mg L, utilizing 90% of the bed.

摘要

由于水体受到严重污染以及对生物多样性和公众健康产生负面影响,开发具有高容量去除水基介质中污染物能力的新材料变得越来越重要。全球使用最广泛的除草剂草甘膦在水中的存在,因其可能对人类健康造成的附带影响而引发了警报。本研究的主要目的是研究杂化材料MIL-53(Al)@RH对水溶液中草甘膦的吸附潜力。该材料是按照在微波辅助下于水解稻壳存在的情况下合成MIL-53(Al)的方法制备的。进行了批量吸附实验,以评估吸附剂用量、溶液pH值影响、接触时间、吸附质浓度和温度影响。结果表明,在pH值为4、MIL-53(Al)@RH与溶液比例为0.04 g/50 mL的条件下,30分钟内实现了最大吸附容量296.95 mg/g。Avrami模型和准二级模型适当地描述了吸附动力学,而Langmuir模型和Sips模型描述了吸附平衡。所确定的焓变(ΔH°)表明该反应为吸热反应,受化学吸附控制,这与动力学和平衡情况相符。推测吸附机制涉及氢键、π*-π相互作用以及MIL-53(Al)的金属中心与草甘膦阴离子基团之间的络合作用。最后,为了实际应用,将MIL-53(Al)@RH填充到柱中进行固定床测试,结果表明该杂化材料能够去除草甘膦,吸附容量为76.304 mg/L,床层利用率为90%。

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