Details
| Original language | English |
|---|---|
| Pages (from-to) | 4793-4799 |
| Number of pages | 7 |
| Journal | Nano letters |
| Volume | 23 |
| Issue number | 11 |
| Early online date | 17 May 2023 |
| Publication status | Published - 14 Jun 2023 |
Abstract
Solvents are increasingly known to influence chemical reactivity. However, the microscopic origin of solvent effects is scarcely understood, particularly at the individual molecule level. To shed light on this, we explored a well-defined model system of water (D2O) and carbon monoxide on a single-crystal copper surface with time-lapsed low-temperature scanning tunneling microscopy (STM) and ab initio calculations. Through detailed measurements on a time scale of minutes to hours at the limit of single-molecule solvation, we find that at cryogenic temperatures CO-D2O complexes are more mobile than individual CO or water molecules. We also obtain detailed mechanistic insights into the motion of the complex. In diffusion-limited surface reactions, such a solvent-triggered increase in mobility would substantially increase the reaction yield.
Keywords
- CO, complex formation, diffusivity, water
ASJC Scopus subject areas
- Chemical Engineering(all)
- Bioengineering
- Chemistry(all)
- Materials Science(all)
- Physics and Astronomy(all)
- Condensed Matter Physics
- Engineering(all)
- Mechanical Engineering
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In: Nano letters, Vol. 23, No. 11, 14.06.2023, p. 4793-4799.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Considerably Increased Dynamics of CO-Water Complexes over CO and Water Alone
AU - Bertram, Cord
AU - Zaum, Christopher
AU - Fang, Wei
AU - Michaelides, Angelos
AU - Morgenstern, Karina
N1 - Publisher Copyright: © 2023 American Chemical Society.
PY - 2023/6/14
Y1 - 2023/6/14
N2 - Solvents are increasingly known to influence chemical reactivity. However, the microscopic origin of solvent effects is scarcely understood, particularly at the individual molecule level. To shed light on this, we explored a well-defined model system of water (D2O) and carbon monoxide on a single-crystal copper surface with time-lapsed low-temperature scanning tunneling microscopy (STM) and ab initio calculations. Through detailed measurements on a time scale of minutes to hours at the limit of single-molecule solvation, we find that at cryogenic temperatures CO-D2O complexes are more mobile than individual CO or water molecules. We also obtain detailed mechanistic insights into the motion of the complex. In diffusion-limited surface reactions, such a solvent-triggered increase in mobility would substantially increase the reaction yield.
AB - Solvents are increasingly known to influence chemical reactivity. However, the microscopic origin of solvent effects is scarcely understood, particularly at the individual molecule level. To shed light on this, we explored a well-defined model system of water (D2O) and carbon monoxide on a single-crystal copper surface with time-lapsed low-temperature scanning tunneling microscopy (STM) and ab initio calculations. Through detailed measurements on a time scale of minutes to hours at the limit of single-molecule solvation, we find that at cryogenic temperatures CO-D2O complexes are more mobile than individual CO or water molecules. We also obtain detailed mechanistic insights into the motion of the complex. In diffusion-limited surface reactions, such a solvent-triggered increase in mobility would substantially increase the reaction yield.
KW - CO
KW - complex formation
KW - diffusivity
KW - water
UR - http://www.scopus.com/inward/record.url?scp=85160803344&partnerID=8YFLogxK
U2 - 10.17863/CAM.97184
DO - 10.17863/CAM.97184
M3 - Article
AN - SCOPUS:85160803344
VL - 23
SP - 4793
EP - 4799
JO - Nano letters
JF - Nano letters
SN - 1530-6984
IS - 11
ER -