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过渡金属和稀土金属钇改性MIL-101金属有机框架吸附剂制备及其吸附脱硫性能

蒋博龙,  姜楠,  谭伟强

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文章导航 > 环境工程  > 2024 >  42(12): 126-135
蒋博龙, 姜楠, 谭伟强. 过渡金属和稀土金属钇改性MIL-101金属有机框架吸附剂制备及其吸附脱硫性能[J]. 环境工程, 2024, 42(12): 126-135. doi: 10.13205/j.hjgc.202412016
引用本文: 蒋博龙, 姜楠, 谭伟强. 过渡金属和稀土金属钇改性MIL-101金属有机框架吸附剂制备及其吸附脱硫性能[J]. 环境工程, 2024, 42(12): 126-135. doi: 10.13205/j.hjgc.202412016
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JIANG Bolong, JIANG Nan, TAN Weiqiang. PREPARATION OF MIL-101 METAL-ORGANIC FRAME ADSORBENT MODIFIED BY TRANSITION METAL AND YTTRIUM AND ITS ADSORPTION DESULFURIZATION PERFORMANCE[J]. ENVIRONMENTAL ENGINEERING , 2024, 42(12): 126-135. doi: 10.13205/j.hjgc.202412016
Citation: JIANG Bolong, JIANG Nan, TAN Weiqiang. PREPARATION OF MIL-101 METAL-ORGANIC FRAME ADSORBENT MODIFIED BY TRANSITION METAL AND YTTRIUM AND ITS ADSORPTION DESULFURIZATION PERFORMANCE[J]. ENVIRONMENTAL ENGINEERING , 2024, 42(12): 126-135. doi: 10.13205/j.hjgc.202412016
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过渡金属和稀土金属钇改性MIL-101金属有机框架吸附剂制备及其吸附脱硫性能

doi: 10.13205/j.hjgc.202412016

  • 1. 东北石油大学 化学化工学院, 黑龙江 大庆 163318;

  • 2. 青岛理工大学 环境与市政工程学院, 山东 青岛 266000

基金项目: 

国家自然科学基金项目(22008134)

详细信息
    作者简介:

    蒋博龙(1988-),男,副教授,主要研究方向为金属有机框架材料(MOF)吸附处理污水、微生物燃料电池阴极氧还原(ORR)催化剂。jiangbolong@qut.edu.cn

    通讯作者:

    蒋博龙(1988-),男,副教授,主要研究方向为金属有机框架材料(MOF)吸附处理污水、微生物燃料电池阴极氧还原(ORR)催化剂。jiangbolong@qut.edu.cn

PREPARATION OF MIL-101 METAL-ORGANIC FRAME ADSORBENT MODIFIED BY TRANSITION METAL AND YTTRIUM AND ITS ADSORPTION DESULFURIZATION PERFORMANCE

  • 1. College of Chemistry and Chemical Engineering, Northeast Petroleum University, Daqing 163318, China;

  • 2. Institute of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266000, China

    摘要
  • 摘要: 燃料油燃烧释放出的含硫化合物造成了严重的环境污染和生态恶化。以过渡金属TM (Ni、Ag和Cu)和稀土金属钇(Y)为改性交换离子,制备了TM-Y/MIL-101吸附剂,并对吸附剂的结构、形貌和金属价态进行了表征。以噻吩为模型硫化物,比较了不同过渡金属对TM-Y/MIL-101吸附剂吸附性能的影响,并分析了不同吸附剂对噻吩的吸附平衡性质、吸附速率控制步骤和吸附机理。结果表明:不同金属改性得到的TM-Y/MIL-101均保持了MIL-101的晶格结构,且过渡金属Cu和Ag以+1价态存在,Ni以+2价态存在;而稀土金属Y以+3价态存在于TM-Y/MIL-101吸附剂中,Cu-Y/MIL-101吸附剂具有最高的吸附容量(28.2 mg/g)和抗芳烃吸附脱硫选择性,不同吸附剂吸附性能顺序为Cu-Y/MIL-101> Ag-Y/MIL-101> Ni-Y/MIL-101。Langmuir模型准一级和准二级速率模型均可用来描述TM-Y/MIL-101对噻吩的吸附过程。吸附控制步骤为传质过程,吸附速率受薄膜扩散和吸附质内扩散控制。噻吩在TM-Y/MIL-101上的吸附主要是Y3+与噻吩S之间的S-M吸附,过渡金属离子(Ni2+、Ag+和Cu+)与噻吩环之间π络合吸附,以及MIL-101上芳环结构与噻吩之间的π-π相互作用3种机制协同作用的结果。
    Abstract: Sulfur-containing compounds released from the combustion of fuel oil have led to serious environmental pollution and ecological deterioration. In this study, a transition metal TM-Y/MIL-101 (TM=Ni, Ag and Cu) adsorbent was prepared, where transition metal (Ni, Ag and Cu) and rare earth element yttrium were selected as exchange ions for modification. The structure, morphology and metal valence of as-prepared adsorbents were characterized. Thiophene was selected to investigate the desulfurization performance of the prepared adsorbents. Langmuir and Freundlich models were used to analyze the adsorption equilibrium properties of thiophene with different adsorbents, study the adsorption kinetics and mechanism, and investigate the control steps of the adsorption rate. Results showed that TM-Y/MIL-101 adsorbents modified by different TMs had maintained the lattice structure of MIL-101, and Cu and Ag existed with a valence of +1, while Ni existed with a valence of +2. Furthermore, the rare earth metal Y existed in the valence state of +3. The adsorption process of thiophene by TM-Y/MIL-101 complied with the Langmuir model and the Cu-Y/MIL-101 possessed the highest adsorption capacity (28.2 mg/g) and anti-aromatic adsorption desulfurization selectivity. Their adsorption performance decreased in the order of Cu-Y/MIL-101 > Ag-Y/MIL-101 > Ni-Y/MIL-101. Both pseudo-first and second-order could describe the adsorption of thiophene onto TM-Y/MIL-101. The mass transfer was found to be the control step of the adsorption process, which was controlled by the film diffusion and internal diffusion of adsorbate. The fast adsorption of thiophene molecule on TM-Y/MIL-101 could be ascribed to the S-M interaction between Y3+ and S in thiophene, π complexation between transition metal ions (Ni2+, Ag+ and Cu+) and thiophene ring, and π-π interaction between aromatic rings of MIL-101 and thiophene molecule.
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  • 收稿日期:  2023-07-17
  • 网络出版日期:  2025-01-18

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