Removal of GenX and Perfluorinated Alkyl Substances from Water by Amine-Functionalized Covalent Organic Frameworks

被引:325
作者
Ji, Woojung [1 ]
Xiao, Leilei [1 ,2 ]
Ling, Yuhan [3 ]
Ching, Casey [3 ]
Matsumoto, Michio [1 ]
Bisbey, Ryan P. [1 ,2 ]
Helbling, Damian E. [3 ]
Dichtel, William R. [1 ]
机构
[1] Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA
[2] Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14853 USA
[3] Cornell Univ, Sch Civil & Environm Engn, Ithaca, NY 14853 USA
关键词
FILM-FORMING FOAMS; PERFLUOROALKYL ACIDS; DRINKING-WATER; FLUORINATED ALTERNATIVES; POLYFLUOROALKYL SUBSTANCES; CRYSTALLINE; DISCOVERY; HYDROGEN; PLATFORM; STORAGE;
D O I
10.1021/jacs.8b06958
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Per- and polyfluorinated alkyl substances (PFAS), such as perfluorooctanoic acid (PFOA), perfluorooctanesulfonate (PFOS), and ammonium perfluoro-2-propoxypropionate (GenX), contaminate ground and surface waters throughout the world. The cost and performance limitations of current PFAS removal technologies motivate efforts to develop selective and high-affinity adsorbents. Covalent organic frameworks (COFs) are unexplored yet promising adsorbents because of their high surface area and tunable pore sizes. Here we show that imine-linked two-dimensional (2D) COFs bearing primary amines adsorb GenX rapidly at environmentally relevant concentrations. COFs with partial amine incorporation showed the highest capacity and fastest removal, suggesting that the synergistic combination of the polar group and hydrophobic surfaces are responsible for GenX binding. A COF with 28% amine loading also removed more than 90% of 12 out of 13 PFAS. These results demonstrate the promise of COFs for PFAS removal and suggest design criteria for maximizing adsorbent performance.
引用
收藏
页码:12677 / 12681
页数:5
相关论文
共 34 条
[1]  
[Anonymous], 2016, Drinking Water Health Advisories for PFOA and PFOS
[2]   Discovery of 40 Classes of Per- and Polyfluoroalkyl Substances in Historical Aqueous Film-Forming Foams (AFFFs) and AFFF-Impacted Groundwater [J].
Barzen-Hanson, Krista A. ;
Roberts, Simon C. ;
Choyke, Sarah ;
Oetjen, Karl ;
McAlees, Alan ;
Riddell, Nicole ;
McCrindle, Robert ;
Ferguson, P. Lee ;
Higgins, Christopher P. ;
Field, Jennifer A. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2017, 51 (04) :2047-2057
[3]   Discovery and Implications of C2 and C3 Perfluoroalkyl Sulfonates in Aqueous Film-Forming Foams and Groundwater [J].
Barzen-Hanson, Krista A. ;
Field, Jennifer A. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY LETTERS, 2015, 2 (04) :95-99
[4]   Covalent Organic Frameworks as a Platform for Multidimensional Polymerization [J].
Bisbey, Ryan P. ;
Dichtel, William R. .
ACS CENTRAL SCIENCE, 2017, 3 (06) :533-543
[5]   Porous, crystalline, covalent organic frameworks [J].
Côté, AP ;
Benin, AI ;
Ockwig, NW ;
O'Keeffe, M ;
Matzger, AJ ;
Yaghi, OM .
SCIENCE, 2005, 310 (5751) :1166-1170
[6]   The precautionary principle and chemicals management: The example of perfluoroalkyl acids in groundwater [J].
Cousins, Ian T. ;
Vestergren, Robin ;
Wang, Zhanyun ;
Scheringer, Martin ;
McLachlan, Michael S. .
ENVIRONMENT INTERNATIONAL, 2016, 94 :331-340
[7]   Moving Beyond Boron: The Emergence of New Linkage Chemistries in Covalent Organic Frameworks [J].
DeBlase, Catherine R. ;
Dichtel, William R. .
MACROMOLECULES, 2016, 49 (15) :5297-5305
[8]   Thioether-Based Fluorescent Covalent Organic Framework for Selective Detection and Facile Removal of Mercury(II) [J].
Ding, San-Yuan ;
Dong, Ming ;
Wang, Ya-Wen ;
Chen, Yan-Tao ;
Wang, Huai-Zhen ;
Su, Cheng-Yong ;
Wang, Wei .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (09) :3031-3037
[9]  
Doonan CJ, 2010, NAT CHEM, V2, P235, DOI [10.1038/nchem.548, 10.1038/NCHEM.548]
[10]   Impact of Treatment Processes on the Removal of Perfluoroalkyl Acids from the Drinking Water Production Chain [J].
Eschauzier, Christian ;
Beerendonk, Erwin ;
Scholte-Veenendaal, Petra ;
De Voogt, Pim .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2012, 46 (03) :1708-1715