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Facile Electron Transfer to CO₂ during Adsorption at the Metal | Solution Interface

Gauthier, Joseph A. and Fields, Meredith and Bajdich, Michal and Chen, Leanne D. and Sandberg, Robert B. and Chan, Karen and Nørskov, Jens K. (2019) Facile Electron Transfer to CO₂ during Adsorption at the Metal | Solution Interface. Journal of Physical Chemistry C, 123 (48). pp. 29278-29283. ISSN 1932-7447. doi:10.1021/acs.jpcc.9b10205.

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We estimate the rate of electron transfer to CO₂ at the Au (211)|water interface during adsorption in an electrochemical environment under reducing potentials. On the basis of density functional theory calculations at the generalized gradient approximation and hybrid levels of theory, we find electron transfer to the adsorbed *CO₂ to be very facile. This high rate of transfer is estimated by the energy distribution of the adsorbate-induced density of states as well as from the interaction between diabatic states representing neutral and negatively charged CO₂. Up to 0.62 electrons is transferred to CO₂, and this charge adiabatically increases with the bending angle to a lower limit of 137°. We conclude that this rate of electron transfer is extremely fast compared to the time scale of the nuclear degrees of freedom, that is, the adsorption process.

Item Type:Article
Related URLs:
URLURL TypeDescription Paper
Gauthier, Joseph A.0000-0001-9542-0988
Bajdich, Michal0000-0003-1168-8616
Chen, Leanne D.0000-0001-9700-972X
Chan, Karen0000-0002-6897-1108
Nørskov, Jens K.0000-0002-4427-7728
Alternate Title:Facile Electron Transfer to CO2 during Adsorption at the Metal | Solution Interface, Electron Transfer to CO2 during Adsorption at the Metal | Solution Interface, Electron Transfer to CO₂ during Adsorption at the Metal | Solution Interface
Additional Information:© 2019 American Chemical Society. Received: October 30, 2019; Published: November 12, 2019. This material is based upon work performed 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 resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility, supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231. M.F. also acknowledges the NSF for their graduate fellowship. K.C. and J.K.N. also acknowledge support from Research Grant 9455 from VILLUM FONDEN. The authors declare no competing financial interest.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
NSF Graduate Research FellowshipUNSPECIFIED
Villum Foundation9455
Subject Keywords:Charge transfer, Electrical energy, Adsorption, Potential energy, Molecules
Issue or Number:48
Record Number:CaltechAUTHORS:20210707-212629894
Persistent URL:
Official Citation:Facile Electron Transfer to CO2 during Adsorption at the Metal|Solution Interface. Joseph A. Gauthier, Meredith Fields, Michal Bajdich, Leanne D. Chen, Robert B. Sandberg, Karen Chan, and Jens K. Nørskov. The Journal of Physical Chemistry C 2019 123 (48), 29278-29283; DOI: 10.1021/acs.jpcc.9b10205
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:109752
Deposited By: Tony Diaz
Deposited On:08 Jul 2021 17:04
Last Modified:24 Mar 2023 18:10

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