Nature of the active sites for CO reduction on copper nanoparticles; suggestions for optimizing performance
Tao Cheng, Hai Xiao, William A. Goddard III
Abstract
Recent experiments show that the grain boundaries (GBs) of copper nanoparticles (NP) lead to outstanding performance in reducing CO_2 and CO to alcohol products. We report here multiscale simulations that mimic experimental synthesis conditions to predict the structure of a 10nm Cu NP (158,555 atoms). To identify active sites, we first predict the CO binding at a large number of sites and select 4 exhibiting CO binding stronger than the (211) step surface. Then, we predict the formation energy of *OCCOH intermediate as a descriptor for C-C coupling, identifying two active sites, both of which have an undercoordinated surface square site adjacent to a subsurface stacking fault. We then propose a periodic Cu surface (4 by 4 supercell) with a similar site that substantially decreases the formation energy of *OCCOH, by 0.14 eV.
Group Members
Cheng, T., Xiao, H., & III, W. A. G. (2017). Nature of the active sites for CO reduction on copper nanoparticles; suggestions for optimizing performance. *J. Am. Chem. Soc.*, *139*(34), 11642-11645. https://doi.org/10.1021/jacs.7b03300