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

revised on 28.10.2019, 21:27 and posted on 29.10.2019, 20:58 by Joseph Gauthier, Meredith Fields, Michal Bajdich, Leanne D. Chen, Robert B. Sandberg, Karen Chan, Jens Kehlet Nørskov
We estimate the rate of electron transfer to CO2 at the Au (211)|water interface during adsorption in an electrochemical environment under reducing potentials. Based on density functional theory calculations at the generalized gradient approximation and hybrid levels of theory, we find electron transfer to 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 are 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 timescale of the nuclear degrees of freedom, that is, the adsorption process.


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. Department of Energy under Contract No. DE-AC02-05CH11231.

M. F. also acknowledges NSF for a Graduate Fellowship. K. C. and J. K. N. also acknowledge support from Research Grant 9455 from VILLUM FONDEN.


Email Address of Submitting Author


SLAC National Accelerator Laboratory


United States

ORCID For Submitting Author


Declaration of Conflict of Interest


Version Notes

Revised submission before the second review


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in The Journal of Physical Chemistry C