Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 17, Pages 4590-4593Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201800335
Keywords
Hofmeister series; ionic transport; polyelectrolyte brushes; rectification inversion; solid nanochannels
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Funding
- National Basic Research Program of China [2016YFA0200104]
- Key Research Program of Frontier Sciences of Chinese Academy of Sciences [QYZDJ-SSW-SLH030]
- NSF of China [21775151, 21475138, 21790390, 21790391, 21790053, 21621062, 21435007]
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A nonintuitive observation of monovalent anion-induced ion current rectification inversion at polyimidazolium brush (PimB)-modified nanopipettes is presented. The rectification inversion degree is strongly dependent on the concentration and species of monovalent anions. For chaotropic anions (for example, ClO4-), the rectification inversion is easily observed at a low concentration (5mm), while there is no rectification inversion observed for kosmotropic anions (Cl-) even at a high concentration (1m). Moreover, at the specific concentration (for example, 10mm), the variation of rectification ratio on the type of anions is ranged by Hofmeister series (Cl- >= NO3- > BF4- > ClO4- > PF6-> Tf2N-). Estimation of the electrokinetic charge density (sigma(ek)) demonstrates that rectification inversion originates from the charge inversion owing to the over-adsorption of chaotropic monovalent anion. To qualitatively understand this phenomenon, a concentration-dependent adsorption mechanism is proposed.
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