Postsynthetically Modified Covalent Organic Frameworks for Efficient and Effective Mercury Removal
文献类型：会议论文
| 作者 | Sun, Qi; Aguila, Briana; Perman, Jason; Earl, Lyndsey D.; Abney, Carter W.; Cheng, Yuchuan; Wei, Hao; Nguyen, Nicholas; Wojtas, Lukasz; Ma, Shengqian |
| 出版日期 | 2017 |
| 关键词 | HEAVY-METALS ENVIRONMENTAL REMEDIATION POROUS FRAMEWORKS MESOPOROUS SILICA AQUEOUS-SOLUTION AQUATIC SYSTEMS RAPID REMOVAL WATER CRYSTALLINE ADSORPTION |
| 卷号 | 139 |
| 期号 | 7 |
| DOI | 10.1021/jacs.6b12885 |
| 英文摘要 | A key challenge in environmental remediation is the design of adsorbents bearing an abundance of accessible chelating sites with high affinity, to achieve both rapid uptake and high capacity for the contaminants. Herein, we demonstrate how two-dimensional covalent organic frameworks (COFs) with well-defined mesopore structures display the right combination of properties to serve as a scaffold for decorating coordination sites to create ideal adsorbents. The proof-of-concept design is illustrated by modifying sulfur derivatives on a newly designed vinyl-functionalized mesoporous COF (COF-V) via thiol-ene click reaction. Representatively, the material (COF-S-SH) synthesized by treating COF-V with 1,2-ethanedithiol exhibits high efficiency in removing mercury from aqueous solutions and the air, affording He and H-g(0) capacities of 1350 and 863 mg g(-1), respectively, surpassing all those of thiol and thioether functionalized materials reported thus far. More significantly, COF-S-SH demonstrates an ultrahigh distribution coefficient value (K-d) of 2.3 X 10(9) mL g(-1), which allows it to rapidly reduce the Hg2+ concentration from 5 ppm to less than 0.1 ppb, well below the acceptable limit in drinking water (2 ppb). We attribute the impressive performance to the synergistic effects arising from densely populated chelating groups with a strong binding ability within ordered mesopores that allow rapid diffusion of mercury species throughout the material. X-ray absorption fine structure (XAFS) spectroscopic studies revealed that each Hg is bound exclusively by two S via intramolecular cooperativity in COF-S-SH, further interpreting its excellent affinity. The results presented here thus reveal the exceptional potential of COFs for high-performance environmental remediation. |
| 学科主题 | Chemistry |
| ISSN号 | 0002-7863 |
| 源URL | [http://ir.nimte.ac.cn/handle/174433/23435]  |
| 专题 | 会议专题 会议专题_会议论文 |
| 推荐引用方式 GB/T 7714 | Sun, Qi,Aguila, Briana,Perman, Jason,et al. Postsynthetically Modified Covalent Organic Frameworks for Efficient and Effective Mercury Removal[C]. 见:. |
入库方式： OAI收割
来源：宁波材料技术与工程研究所
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