Nanoscale heterogeneity at the aqueous electrolyte–electrode interface
Using molecular dynamics simulations, we reveal emergent properties of hydrated electrode interfaces that while molecular in origin are integral to the behavior of the system across long times scales and large length scales. Specifically, we describe the impact of a disordered and slowly evolving ad...
| Main Authors: | , |
|---|---|
| Other Authors: | |
| Format: | Article |
| Language: | en_US |
| Published: |
Elsevier
2016
|
| Online Access: | http://hdl.handle.net/1721.1/106145 |
| _version_ | 1826207151450750976 |
|---|---|
| author | Limmer, David T. Willard, Adam P. |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Limmer, David T. Willard, Adam P. |
| author_sort | Limmer, David T. |
| collection | MIT |
| description | Using molecular dynamics simulations, we reveal emergent properties of hydrated electrode interfaces that while molecular in origin are integral to the behavior of the system across long times scales and large length scales. Specifically, we describe the impact of a disordered and slowly evolving adsorbed layer of water on the molecular structure and dynamics of the electrolyte solution adjacent to it. Generically, we find that densities and mobilities of both water and dissolved ions are spatially heterogeneous in the plane parallel to the electrode over nanosecond timescales. These and other recent results are analyzed in the context of available experimental literature from surface science and electrochemistry. We speculate on the implications of this emerging microscopic picture on the catalytic proficiency of hydrated electrodes, offering a new direction for study in heterogeneous catalysis at the nanoscale. |
| first_indexed | 2024-09-23T13:44:51Z |
| format | Article |
| id | mit-1721.1/106145 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T13:44:51Z |
| publishDate | 2016 |
| publisher | Elsevier |
| record_format | dspace |
| spelling | mit-1721.1/1061452022-09-28T15:53:48Z Nanoscale heterogeneity at the aqueous electrolyte–electrode interface Limmer, David T. Willard, Adam P. Massachusetts Institute of Technology. Department of Chemistry Willard, Adam P. Using molecular dynamics simulations, we reveal emergent properties of hydrated electrode interfaces that while molecular in origin are integral to the behavior of the system across long times scales and large length scales. Specifically, we describe the impact of a disordered and slowly evolving adsorbed layer of water on the molecular structure and dynamics of the electrolyte solution adjacent to it. Generically, we find that densities and mobilities of both water and dissolved ions are spatially heterogeneous in the plane parallel to the electrode over nanosecond timescales. These and other recent results are analyzed in the context of available experimental literature from surface science and electrochemistry. We speculate on the implications of this emerging microscopic picture on the catalytic proficiency of hydrated electrodes, offering a new direction for study in heterogeneous catalysis at the nanoscale. 2016-12-27T16:36:30Z 2016-12-27T16:36:30Z 2014-11 2014-10 Article http://purl.org/eprint/type/JournalArticle 00092614 http://hdl.handle.net/1721.1/106145 Limmer, David T., and Adam P. Willard. “Nanoscale Heterogeneity at the Aqueous Electrolyte–electrode Interface.” Chemical Physics Letters 620 (2015): 144–150. en_US http://dx.doi.org/10.1016/j.cplett.2014.11.013 Chemical Physics Letters Creative Commons Attribution-NonCommercial-NoDerivs License http://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf Elsevier arXiv |
| spellingShingle | Limmer, David T. Willard, Adam P. Nanoscale heterogeneity at the aqueous electrolyte–electrode interface |
| title | Nanoscale heterogeneity at the aqueous electrolyte–electrode interface |
| title_full | Nanoscale heterogeneity at the aqueous electrolyte–electrode interface |
| title_fullStr | Nanoscale heterogeneity at the aqueous electrolyte–electrode interface |
| title_full_unstemmed | Nanoscale heterogeneity at the aqueous electrolyte–electrode interface |
| title_short | Nanoscale heterogeneity at the aqueous electrolyte–electrode interface |
| title_sort | nanoscale heterogeneity at the aqueous electrolyte electrode interface |
| url | http://hdl.handle.net/1721.1/106145 |
| work_keys_str_mv | AT limmerdavidt nanoscaleheterogeneityattheaqueouselectrolyteelectrodeinterface AT willardadamp nanoscaleheterogeneityattheaqueouselectrolyteelectrodeinterface |