Predicted Structures of the Active Sites Responsible for the Improved Reduction of Carbon Dioxide by Gold Nanoparticles
Tao Cheng, Yufeng Huang, Hai Xiao, William A. Goddard III
Abstract
Gold (Au) nanoparticles (NPs) are known experimentally to reduce carbon dioxide (CO_2) to carbon monoxide (CO), with far superior performance to Au foils. To obtain guidance in designing improved CO_2 catalysts, we want to understand the nature of the active sites on Au NPs. Here, we employed multiscale atomistic simulations to computationally synthesize and characterize a 10 nm thick Au NP on a carbon nanotube (CNT) support, and then we located active sites from quantum mechanics (QM) calculations on 269 randomly selected sites. The standard scaling relation is that the formation energy of *COOH (ΔE_(*COOH)) is proportional to the binding energy of *CO (E^(binding)_(*CO)); therefore, decreasing ΔE_(*COOH) to boost the CO_2 reduction reaction (CO_2RR) causes an increase of E^(binding)_(*CO) that retards CO_2RR. We show that the NPs have superior CO_2RR because there are many sites at the twin boundaries that significantly break this scaling relation.
Group Members
Cheng, T., Huang, Y., Xiao, H., & III, W. A. G. (2017). Predicted Structures of the Active Sites Responsible for the Improved Reduction of Carbon Dioxide by Gold Nanoparticles. *J. Phys. Chem. Lett.*, *8*(14), 3317-3320. https://doi.org/10.1021/acs.jpclett.7b01335