Identifying Active Sites for CO₂ Reduction on Dealloyed Gold Surfaces by Combining Machine Learning with Multiscale Simulations
Abstract
Gold nanoparticles (AuNPs) and dealloyed Au_3Fe core–shell NP surfaces have been shown to have dramatically improved performance in reducing CO_2 to CO (CO2RR), but the surface features responsible for these improvements are not known. The active sites cannot be identified with surface science experiments, and quantum mechanics (QM) is not practical for the 10 000 surface sites of a 10 nm NP (200 000 bulk atoms). Here, we combine machine learning, multiscale simulations, and QM to predict the performance (a-value) of all 5000–10 000 surface sites on AuNPs and dealloyed Au surfaces. We then identify the optimal active sites for CO2RR on dealloyed gold surfaces with dramatically reduced computational effort. This approach provides a powerful tool to visualize the catalytic activity of the whole surface. Comparing the a-value with descriptors from experiment, computation, or theory should provide new ways to guide the design of high-performance electrocatalysts for applications in clean energy conversion.
Additional Information
© 2019 American Chemical Society. Received: May 8, 2019; Published: June 18, 2019. This work was supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. This work uses the computational resources of Caltech High Performance Computing Center (HPC). The authors declare no competing financial interest.Attached Files
Updated - ja9b04956_si_001.pdf
Files
Name | Size | Download all |
---|---|---|
md5:0f59be1699d93f90b3685f5afa3301f7
|
5.8 MB | Preview Download |
Additional details
- Alternative title
- Identifying Active Sites for CO2 Reduction on Dealloyed Gold Surfaces by Combining Machine Learning with Multiscale Simulations
- Eprint ID
- 96498
- Resolver ID
- CaltechAUTHORS:20190618-103437881
- Joint Center for Artificial Photosynthesis (JCAP)
- Department of Energy (DOE)
- DE-SC0004993
- Created
-
2019-06-18Created from EPrint's datestamp field
- Updated
-
2021-11-16Created from EPrint's last_modified field
- Caltech groups
- JCAP
- Other Numbering System Name
- WAG
- Other Numbering System Identifier
- 1341