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Published August 30, 2017 | Supplemental Material
Journal Article Open

Nature of the active sites for CO reduction on copper nanoparticles; suggestions for optimizing performance

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.

Additional Information

© 2017 American Chemical Society. Received: April 2, 2017; Published: August 16, 2017. This work was supported 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 No. DE-SC0004993. This computational work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation grant number ACI-1053575, and the Zwicky Astrophysics Supercomputer at Caltech. The authors declare no competing financial interest.

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