TY - JOUR
T1 - Elucidation of the Molecular Determinants for Optimal Perfluorooctanesulfonate Adsorption Using a Combinatorial Nanoparticle Library Approach
AU - Liu, Yin
AU - Su, Gaoxing
AU - Wang, Fei
AU - Jia, Jianbo
AU - Li, Shuhuan
AU - Zhao, Linlin
AU - Shi, Yali
AU - Cai, Yaqi
AU - Zhu, Hao
AU - Zhao, Bin
AU - Jiang, Guibin
AU - Zhou, Hongyu
AU - Yan, Bing
N1 - Funding Information:
We thank Yan Mu for technical assistance. This work was supported by the National Key Research and Development Program of China (2016YFA0203103), the National Natural Science Foundation of China (91543204 and 91643204), and the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB14030401).
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/6/20
Y1 - 2017/6/20
N2 - Perfluorooctanesulfonate (PFOS) persistently accumulates in the environment and in humans, causing various toxicities. To determine the key molecular determinants for optimal PFOS specificity and efficiency, we designed and synthesized a combinatorial gold nanoparticle (GNP) library consisting of 18 members with rationally diversified hydrophobic, electrostatic, and fluorine-fluorine interaction components for PFOS bindings. According to our findings, the electrostatic and F-F interactions between PFOS and nanoparticles are complementary. When F-F attractions are relatively weak, the electrostatic interactions are dominant. As F-F interactions increase, the electrostatic contributions are reduced to as low as 20%, demonstrating that F-F binding may overpower even electrostatic interactions. Furthermore, F-F interactions (28-79% binding efficiency) are 2-fold stronger than regular hydrophobic interactions (15-39% binding efficiency) for PFOS adsorption, explaining why these novel PFOS-binding nanoparticles are superior to other conventional materials based on either hydrophobic or electrostatic binding. The PFOS adsorption by the optimized nanoparticles performs well in the presence of ionic interferences and in environmental wastewater. This library mapping approach can potentially be applied to recognition mechanism investigation of other pollutants and facilitate the discovery of effective monitoring probes and matrices for their removal.
AB - Perfluorooctanesulfonate (PFOS) persistently accumulates in the environment and in humans, causing various toxicities. To determine the key molecular determinants for optimal PFOS specificity and efficiency, we designed and synthesized a combinatorial gold nanoparticle (GNP) library consisting of 18 members with rationally diversified hydrophobic, electrostatic, and fluorine-fluorine interaction components for PFOS bindings. According to our findings, the electrostatic and F-F interactions between PFOS and nanoparticles are complementary. When F-F attractions are relatively weak, the electrostatic interactions are dominant. As F-F interactions increase, the electrostatic contributions are reduced to as low as 20%, demonstrating that F-F binding may overpower even electrostatic interactions. Furthermore, F-F interactions (28-79% binding efficiency) are 2-fold stronger than regular hydrophobic interactions (15-39% binding efficiency) for PFOS adsorption, explaining why these novel PFOS-binding nanoparticles are superior to other conventional materials based on either hydrophobic or electrostatic binding. The PFOS adsorption by the optimized nanoparticles performs well in the presence of ionic interferences and in environmental wastewater. This library mapping approach can potentially be applied to recognition mechanism investigation of other pollutants and facilitate the discovery of effective monitoring probes and matrices for their removal.
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U2 - 10.1021/acs.est.7b01635
DO - 10.1021/acs.est.7b01635
M3 - Article
C2 - 28537376
AN - SCOPUS:85021669456
SN - 0013-936X
VL - 51
SP - 7120
EP - 7127
JO - Environmental Science & Technology
JF - Environmental Science & Technology
IS - 12
ER -