Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids
Here we present a theory of ion aggregation and gelation of room temperature ionic liquids (RTILs). Based on it, we investigate the effect of ion aggregation on correlated ion transport-ionic conductivity and transference numbers-obtaining closed-form expressions for these quantities. The theory dep...
| Main Authors: | , , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
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American Chemical Society (ACS)
2021
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| Online Access: | https://hdl.handle.net/1721.1/133976 |
| _version_ | 1826204776634777600 |
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| author | McEldrew, Michael Goodwin, Zachary AH Zhao, Hongbo Bazant, Martin Z Kornyshev, Alexei A |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering McEldrew, Michael Goodwin, Zachary AH Zhao, Hongbo Bazant, Martin Z Kornyshev, Alexei A |
| author_sort | McEldrew, Michael |
| collection | MIT |
| description | Here we present a theory of ion aggregation and gelation of room temperature ionic liquids (RTILs). Based on it, we investigate the effect of ion aggregation on correlated ion transport-ionic conductivity and transference numbers-obtaining closed-form expressions for these quantities. The theory depends on the maximum number of associations a cation and anion can form and the strength of their association. To validate the presented theory, we perform molecular dynamics simulations on several RTILs and a range of temperatures for one RTIL. The simulations indicate the formation of large clusters, even percolating through the system under certain circumstances, thus forming a gel, with the theory accurately describing the obtained cluster distributions in all cases. However, based on the strength and lifetime of associations in the simulated RTILs, we expect free ions to dominate ionic conductivity despite the presence of clusters, and we do not expect the percolating cluster to trigger structural arrest in the RTIL. |
| first_indexed | 2024-09-23T13:01:13Z |
| format | Article |
| id | mit-1721.1/133976 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T13:01:13Z |
| publishDate | 2021 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1339762023-09-12T20:07:53Z Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids McEldrew, Michael Goodwin, Zachary AH Zhao, Hongbo Bazant, Martin Z Kornyshev, Alexei A Massachusetts Institute of Technology. Department of Chemical Engineering Here we present a theory of ion aggregation and gelation of room temperature ionic liquids (RTILs). Based on it, we investigate the effect of ion aggregation on correlated ion transport-ionic conductivity and transference numbers-obtaining closed-form expressions for these quantities. The theory depends on the maximum number of associations a cation and anion can form and the strength of their association. To validate the presented theory, we perform molecular dynamics simulations on several RTILs and a range of temperatures for one RTIL. The simulations indicate the formation of large clusters, even percolating through the system under certain circumstances, thus forming a gel, with the theory accurately describing the obtained cluster distributions in all cases. However, based on the strength and lifetime of associations in the simulated RTILs, we expect free ions to dominate ionic conductivity despite the presence of clusters, and we do not expect the percolating cluster to trigger structural arrest in the RTIL. 2021-10-27T19:57:27Z 2021-10-27T19:57:27Z 2021 2021-06-08T16:09:31Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/133976 en 10.1021/acs.jpcb.0c09050 Journal of Physical Chemistry B Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf American Chemical Society (ACS) arXiv |
| spellingShingle | McEldrew, Michael Goodwin, Zachary AH Zhao, Hongbo Bazant, Martin Z Kornyshev, Alexei A Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids |
| title | Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids |
| title_full | Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids |
| title_fullStr | Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids |
| title_full_unstemmed | Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids |
| title_short | Correlated Ion Transport and the Gel Phase in Room Temperature Ionic Liquids |
| title_sort | correlated ion transport and the gel phase in room temperature ionic liquids |
| url | https://hdl.handle.net/1721.1/133976 |
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