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Rapid and selective adsorption of a typical aromatic organophosphorus flame retardant on MIL-101-based metal-organic frameworks

机译：在MIL-101的金属有机框架上快速和选择性地吸附典型的芳香有机磷阻燃剂

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摘要

The pollution of aromatic organophosphorus flame retardants (aromatic OPFRs) in aquatic environments has drawn great attention over the last few years. Two MIL-101-based metal-organic frameworks (Cr-MIL-101 and Fe-MIL-101-NH2) which possess ordered mesoporous cavities (2.9 and 3.4 nm) and aromatic structures were chosen and prepared to selectively adsorb a typical aromatic OPFR [triphenyl phosphate (TPhP)] from aqueous solution. Pore distribution analysis showed that Cr-MIL-101 and Fe-MIL-101-NH2 had both a mesoporous structure (2-3.5 nm) and microporous structure (1-2 nm), conducive to diffusion and adsorption of TPhP molecules. Compared with Fe-MIL-101-NH2 as well as commercial activated carbon, Cr-MIL-101 showed rapid and efficient adsorption for TPhP, and its initial sorption velocity (v(0)) calculated from the pseudo-second-order model was up to 568.18 mu mol g(-1) h(-1). The adsorption equilibrium of TPhP on the Cr-MIL-101 was almost achieved within 12 h, while the equilibrium time of other adsorbents required more than 48 h. The study of selective adsorption found that Cr-MIL-101 had a higher sorption amount for aromatic OPFRs than alkyl-OPFRs and other aromatic compounds with different chemical structures. Cr-MIL-101 was able to keep a steady selective adsorption for TPhP in the presence of co-existing aromatic compounds. Based on the analysis of K-ow, molecular structure and further density functional theory calculations, hydrophobic interactions may play a dominant role in the selective adsorption process of TPhP, and pi-pi interactions may be also involved. Cr-MIL-101 exhibits reusability and promising potential to rapidly and selectively remove aromatic OPFR in environmental remediation.
机译：在过去几年中，水生环境中芳香有机磷阻燃剂（芳香OPFRS）的污染引起了很大的关注。选择具有有序介孔腔（2.9和3.4nm）和芳族结构的两个MIL-101的金属 - 有机框架（CR-MIL-101和Fe-MIL-101-NH2）并制备选择性地吸附典型的芳族OPFR从水溶液中[三苯基磷酸酯（TPHP）]。孔分布分析表明，Cr-MIL-101和Fe-MIL-101-NH2具有介孔结构（2-3.5nm）和微孔结构（1-2nm），有利于TPHP分子的扩散和吸附。与Fe-MIL-101-NH2以及商业活性炭相比，CR-MIL-101显示出对TPHP的快速有效的吸附，其初始二阶模型计算的初始吸附速度（V（0））是高达568.18 mm mol g（-1）h（-1）。在12小时内，CR-MIL-101上的TPHP的吸附平衡几乎达到，而其他吸附剂的平衡时间需要超过48小时。选择性吸附的研究发现，铬MIL-101具有比烷基OPFRs和具有不同化学结构的其他芳族化合物的芳族OPFRs更高的吸附量。 CR-MIL-101能够在共存芳族化合物存在下保持TPHP的稳定选择性吸附。基于K，超重，分子结构和进一步密度泛函理论计算的分析，疏水性相互作用可以在TPhP的选择性吸附过程中发挥主导作用，和π-π相互作用可以也参与其中。 CR-MIL-101表现出可重用性和有希望的潜力，以快速，选择性地除去环境修复中的芳香opfr。

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  • 来源
    《RSC Advances》 |2020年第4期|共11页
  • 作者

    Su Hui; Lv Jiaxin; Yang Liansheng; Feng Li; Liu Yongze; Du Ziwen; Zhang Liqiu;

  • 作者单位

    Beijing Forestry Univ Beijing Key Lab Source Control Technol Water Poll Engn Res Ctr Water Pollut Source Control &

    Ecorem Coll Environm Sci &

    Engn 35 Tsinghua East Rd Beijing 100083 Peoples R China;

    Beijing Forestry Univ Beijing Key Lab Source Control Technol Water Poll Engn Res Ctr Water Pollut Source Control &

    Ecorem Coll Environm Sci &

    Engn 35 Tsinghua East Rd Beijing 100083 Peoples R China;

    Beijing Forestry Univ Beijing Key Lab Source Control Technol Water Poll Engn Res Ctr Water Pollut Source Control &

    Ecorem Coll Environm Sci &

    Engn 35 Tsinghua East Rd Beijing 100083 Peoples R China;

    Beijing Forestry Univ Beijing Key Lab Source Control Technol Water Poll Engn Res Ctr Water Pollut Source Control &

    Ecorem Coll Environm Sci &

    Engn 35 Tsinghua East Rd Beijing 100083 Peoples R China;

    Beijing Forestry Univ Beijing Key Lab Source Control Technol Water Poll Engn Res Ctr Water Pollut Source Control &

    Ecorem Coll Environm Sci &

    Engn 35 Tsinghua East Rd Beijing 100083 Peoples R China;

    Beijing Forestry Univ Beijing Key Lab Source Control Technol Water Poll Engn Res Ctr Water Pollut Source Control &

    Ecorem Coll Environm Sci &

    Engn 35 Tsinghua East Rd Beijing 100083 Peoples R China;

    Beijing Forestry Univ Beijing Key Lab Source Control Technol Water Poll Engn Res Ctr Water Pollut Source Control &

    Ecorem Coll Environm Sci &

    Engn 35 Tsinghua East Rd Beijing 100083 Peoples R China;

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