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

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

Journal Article · 19 November 2018 · ACS Energy Letters

DOI: https://doi.org/10.1021/acsenergylett.8b01736 · OSTI ID:1490965

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

^[1]; Wang, Lei ^[1];

^[1];

^[1]

Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)

Here, 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.

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

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

Grant/Contract Number:: AC02-76SF00515; P2ELP2_168600; SC0004993

OSTI ID:: 1490965

Alternate ID(s):: OSTI ID: 1490728

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 62 works

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

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