Nature of the Active Sites for CO Reduction on Copper Nanoparticles; Suggestions for Optimizing Performance

Cheng, Tao; Xiao, Hai; Goddard, William A.

doi:10.1021/jacs.7b03300

Title: Nature of the Active Sites for CO Reduction on Copper Nanoparticles; Suggestions for Optimizing Performance

Journal Article · Wed Aug 16 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b03300· OSTI ID:1467599

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California Inst. of Technology (CalTech), Pasadena, CA (United States)

Recent experiments show that the grain boundaries (GBs) of copper nanoparticles (NPs) lead to an outstanding performance in reducing CO₂ and CO to alcohol products. We report here multiscale simulations that simulate experimental synthesis conditions to predict the structure of a 10 nm Cu NP (158 555 atoms). To identify active sites, we first predict the CO binding at a large number of sites and select four exhibiting CO binding stronger than the (211) step surface. Then, we predict the formation energy of the *OCCOH intermediate as a descriptor for C–C coupling, identifying two active sites, both of which have an under-coordinated surface square site adjacent to a subsurface stacking fault. As a result, 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.

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Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0004993

OSTI ID:: 1467599

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 34; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 122 works

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