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氨基功能化MIL-53(Fe)对罗丹明B的吸附性能及机制研究

Adsorption performance and mechanism of amino-functionalized MIL-53(Fe)for rhodamine B
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摘要 通过一步溶剂法制备了含有氨基取代基的MIL-53(Fe)(NH_(2)-MIL-53(Fe)),并用于去除水溶液中的罗丹明B(RhB).利用SEM、XRD、XPS、FTIR等技术对MIL-53(Fe)和NH_(2)-MIL-53(Fe)的形貌和结构进行了表征.采用批量吸附实验研究了MIL-53(Fe)和NH_(2)-MIL-53(Fe)对RhB的吸附特性,考察了溶液pH值、共存离子、投加量等因素的影响,研究了NH_(2)-MIL-53(Fe)的再生性能,并通过实验和表征结果探讨了吸附机制.结果表明,NH_(2)-MIL-53(Fe)和MIL-53(Fe)对RhB吸附的控速步骤为化学吸附,吸附过程分为液膜扩散、颗粒内扩散和吸附平衡3个阶段.等温吸附实验表明,NH_(2)-MIL-53(Fe)和MIL-53(Fe)对RhB的吸附行为可被Langmuir和Temkin模型很好地描述,拟合所得最大吸附量分别为796.5 mg·g^(-1)和549.1 mg·g^(-1),NH_(2)-MIL-53(Fe)对RhB的吸附性能比MIL-53(Fe)提高了45%.当溶液pH值在5~8时,MIL-53(Fe)和NH_(2)-MIL-53(Fe)对RhB的吸附效果最佳;经过5次吸附-再生试验,NH_(2)-MIL-53(Fe)对RhB的吸附容量仍能保持初始吸附量的85%.NH_(2)-MIL-53(Fe)吸附RhB的机制包括氢键作用(普通氢键和电荷辅助氢键)、路易斯酸碱作用、静电引力、π-π相互作用和π-π相互作用.NH_(2)-MIL-53(Fe)作为一种吸附剂,在染料废水处理方面具有良好的潜力. Amino-functionalized MIL-53(Fe)(NH_(2)-MIL-53(Fe))was synthesized via a one-step solvent method and used for the removal of rhodamine B(RhB)from aqueous solutions.The morphology and structure of MIL-53(Fe)and NH_(2)-MIL-53(Fe)were characterized using SEM,XRD,XPS,FTIR,and other techniques.Batch adsorption experiments were conducted to investigate the adsorption characteristics of MIL-53(Fe)and NH_(2)-MIL-53(Fe)for RhB,examining the effects of solution pH,coexisting ions,and adsorbent dosage.The regeneration performance of NH_(2)-MIL-53(Fe)was evaluated,and the adsorption mechanism was elucidated through experimental and characterization results.Results indicated that the rate-limiting step of RhB adsorption by both NH_(2)-MIL-53(Fe)and MIL-53(Fe)was chemical adsorption,with process occurring in three stages:liquid film diffusion,particle diffusion,and adsorption equilibrium.Isotherm studies showed that the adsorption behavior of both NH_(2)-MIL-53(Fe)and MIL-53(Fe)for RhB followed the Langmuir and Temkin models,with maximum adsorption capacities of 796.5 mg·g^(-1)and 549.1 mg·g^(-1),respectively,approximately 45% increase for the amino-functionalized variant.Optimal adsorption was observed at pH 5~8.After five adsorption-regeneration cycles,NH_(2)-MIL-53(Fe)maintained 85%of its initial adsorption capacity.The adsorption mechanism involved hydrogen bonding(both ordinary and charge-assisted),Lewis acid-base interactions,electrostatic attraction,π-πinteractions,and n-πinteractions.As an adsorbent,NH_(2)-MIL-53(Fe)demonstrates great potential for dye wastewater treatment.
作者 马锋锋 焦雅仙 李庆 康宏兵 赵浩 张建 付嘉怡 MA Fengfeng;JIAO Yaxian;LI Qing;KANG Hongbing;ZHAO Hao;ZHANG Jian;FU Jiayi(School of Environmental and Municipal Engineering,Lanzhou Jiaotong University,Lanzhou 730070;Ministry of Education Engineering Research Center of Water Resource Comprehensive Utilization in Cold and Arid Regions,Lanzhou Jiaotong University,Lanzhou 730070)
出处 《环境科学学报》 北大核心 2025年第7期243-257,共15页 Acta Scientiae Circumstantiae
基金 兰州交通大学“天佑青年托举人才计划”基金 甘肃省自然科学基金资助项目(No.23JRRA874) 甘肃省教育厅高校科研创新平台重大培育项目(No.2024CXPT-14)。
关键词 铁基MOF 氨基功能化 罗丹明B 吸附 氢键作用 iron-based MOF amino functionalization rhodamine B adsorption hydrogen bonding
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