Dramatic differences in carbon dioxide adsorption and initial steps of reduction between silver and copper
Yifan Ye, Hao Yang, Jin Qian, Hongyang Su, Kyung-Jae Lee, Tao Cheng, Hai Xiao, Junko Yano, William A. Goddard III, Ethan J. Crumlin
Abstract
Converting carbon dioxide (CO_2) into liquid fuels and synthesis gas is a world-wide priority. But there is no experimental information on the initial atomic level events for CO_2 electroreduction on the metal catalysts to provide the basis for developing improved catalysts. Here we combine ambient pressure X-ray photoelectron spectroscopy with quantum mechanics to examine the processes as Ag is exposed to CO_2 both alone and in the presence of H_2O at 298 K. We find that CO_2 reacts with surface O on Ag to form a chemisorbed species (O = CO_2^(δ−)). Adding H_2O and CO_2 then leads to up to four water attaching on O = CO_2^(δ−) and two water attaching on chemisorbed (b-)CO_2. On Ag we find a much more favorable mechanism involving the O = CO_2^(δ−) compared to that involving b-CO_2 on Cu. Each metal surface modifies the gas-catalyst interactions, providing a basis for tuning CO_2 adsorption behavior to facilitate selective product formations.
Group Members
Ye, Y., Yang, H., Qian, J., Su, H., Lee, K., Cheng, T., Xiao, H., Yano, J., III, W. A. G., & Crumlin, E. J. (2019). Dramatic differences in carbon dioxide adsorption and initial steps of reduction between silver and copper. *Nature Communications*, *10*(1), Art. No. 1875. https://doi.org/10.1038/s41467-019-09846-y