Guiding Electrochemical Carbon Dioxide Reduction toward Carbonyls Using Copper Silver Thin Films with Interphase Miscibility

Higgins, Drew; Landers, Alan T.; Ji, Yongfei; Nitopi, Stephanie; Morales-Guio, Carlos G.; Wang, Lei; Chan, Karen; Hahn, Christopher; Jaramillo, Thomas F.

doi:10.1021/acsenergylett.8b01736

Guiding Electrochemical Carbon Dioxide Reduction toward Carbonyls Using Copper Silver Thin Films with Interphase Miscibility

Journal Article · Wed Nov 14 00:00:00 EST 2018 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.8b01736· OSTI ID:1490728

^[1]; Landers, Alan T. ^[2]; Ji, Yongfei ^[3]; Nitopi, Stephanie ^[3]; ^[3]; Wang, Lei ^[3]; ^[3]; ^[3]; ^[3]

Department of Chemical Engineering, Stanford University, 443 Via Ortega Way, Stanford, California 94305, United States; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States; SLAC National Accelerator Laboratory
SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States; Department of Chemistry, Stanford University, 333 Campus Drive, Stanford, California 94305, United States
Department of Chemical Engineering, Stanford University, 443 Via Ortega Way, Stanford, California 94305, United States; SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States

Steering the selectivity of Cu-based electrochemical CO2 reduction (CO2R) catalysts toward targeted products will serve to improve the technoeconomic outlook of technologies based on this process. Using physical vapor deposition as a tool to overcome thermodynamic miscibility limitations, CuAg thin films with nonequilibrium Cu/Ag alloying were prepared for CO2R performance evaluation. In comparison to pure Cu, the CuAg thin films showed significantly higher activity and selectivity toward liquid carbonyl products, including acetaldehyde and acetate. Suppressed activity and selectivity toward hydrocarbons and the competing hydrogen evolution were also demonstrated on CuAg thin films, with a greater degree of suppression observed at increasing nominal Ag compositions. Compositional-dependent CO2R trends coupled with physical characterization and density functional theory suggest that significant miscibility of Ag into the Cu-rich phase of the catalyst underpinned the observed CO2R trends through tuning of adsorbate and reaction intermediate binding energies on the surface.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-76SF00515; SC0004993

OSTI ID:: 1490728

Alternate ID(s):: OSTI ID: 1490965

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 12 Vol. 3; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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