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Highly efficient and selective pillararene-based organic materials for Hg2+ and CH3Hg+ extraction from aqueous solution
Chen, LX; Wang, Y; Wan, YS; Cai, YM; Xiong, YQ; Fan, ZW; Conradson, SD; Fu, HY; Yuan, LH; Feng, W
2020
Source PublicationCHEMICAL ENGINEERING JOURNAL
ISSN1385-8947
Volume387Pages:-
Subtype期刊论文
AbstractPillararenes, a rising star in macrocyclic chemistry, are recognized as promising organic materials for metal ion separation. Herein, three novel pillar[5]arenes (1a-c) appended with N,N-dimethyldithiocarbamoyl groups were designed for highly efficient extraction of aqueous mercury. This work represents the first case of using pillararene-based materials for organic mercury removal, and rather low Hg(II) residue (3.45 ppb) was found in the extraction raffinate of mercury spiked river water after being treated with the as-prepared extractants, which is a rare example of solvent extraction systems that meet the waste water discharge standard (< 5 ppb). The extraction performance of the extractant materials was evaluated under different acidities, equilibrium time and sodium nitrate concentrations. High extraction efficiency (> 99%) and selectivity (SFHg/M > 690) were achieved under the optimum condition, and the near quantitative stripping after two contacts enable regeneration of the ligands as well as mercury recovery. The stoichiometric ratio between ligands and Hg2+ was ascertained to be 1:1 from the slope analysis method and mass spectroscopy. Investigation of the extracted species by NMR, IR, EXAFS techniques and DFT simulation reveals that the C=S moieties of the ligands play a crucial role in metal complexation. It is noted that the as-prepared extractants show excellent recovery and removal ability towards mercury using simulated samples. After extraction by 1c, the total Hg(II) in spiked river samples was reduced to lower than 5 ppb, the maximum tolerable concentration set by China for industrial waste water. This study demonstrates the potential application of N,N-dimethyldithiocarbamoyl modified pillararenes as functional materials for aquatic mercury remediation.
KeywordIONIC LIQUIDS ABSORPTION-SPECTROSCOPY MERCURY REMOVAL METHYLMERCURY SEPARATION DIGLYCOLAMIDES PERFORMANCE LIGANDS HEAVY
DOI10.1016/j.cej.2020.124087
Indexed BySCI ; EI
Language英语
Citation statistics
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/32905
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.Sichuan Univ, Coll Chem, Inst Nucl Sci & Technol, Key Lab Radiat Phys & Technol,Minist Educ, Chengdu 610064, Peoples R China
2.Jozef Stefan Inst, Dept Complex Matter, Ljubljana, Slovenia
3.Washington State Univ, Dept Chem, Pullman, WA 99164 USA
4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China
Recommended Citation
GB/T 7714
Chen, LX,Wang, Y,Wan, YS,et al. Highly efficient and selective pillararene-based organic materials for Hg2+ and CH3Hg+ extraction from aqueous solution[J]. CHEMICAL ENGINEERING JOURNAL,2020,387:-.
APA Chen, LX.,Wang, Y.,Wan, YS.,Cai, YM.,Xiong, YQ.,...&Feng, W.(2020).Highly efficient and selective pillararene-based organic materials for Hg2+ and CH3Hg+ extraction from aqueous solution.CHEMICAL ENGINEERING JOURNAL,387,-.
MLA Chen, LX,et al."Highly efficient and selective pillararene-based organic materials for Hg2+ and CH3Hg+ extraction from aqueous solution".CHEMICAL ENGINEERING JOURNAL 387(2020):-.
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