Breaking Scaling Relationships in CO₂ Reduction on Copper Alloys with Organic Additives
Abstract
Boundary conditions for catalyst performance in the conversion of common precursors such as N₂, O₂, H₂O, and CO₂ are governed by linear free energy and scaling relationships. Knowledge of these limits offers an impetus for designing strategies to alter reaction mechanisms to improve performance. Typically, experimental demonstrations of linear trends and deviations from them are composed of a small number of data points constrained by inherent experimental limitations. Herein, high-throughput experimentation on 14 bulk copper bimetallic alloys allowed for data-driven identification of a scaling relationship between the partial current densities of methane and C₂₊ products. This strict dependence represents an intrinsic limit to the Faradaic efficiency for C–C coupling. We have furthermore demonstrated that coating the electrodes with a molecular film breaks the scaling relationship to promote C₂₊ product formation.
Additional Information
© 2021 The Authors. Published by American Chemical Society. Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0) Received: July 16, 2021; Published: October 14, 2021. This material is based on work performed by the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under Award DE-SC0021266. A.T. acknowledges Marie Skłodowska-Curie Fellowship H2020-MSCA-IF-2017 (793471). The Resnick Sustainability Institute at Caltech is acknowledged for support of the laboratory facilities in which this research was conducted. Author Contributions: Y.L. and N.B.W. contributed equally to this work. The authors declare no competing financial interest.Attached Files
Published - acscentsci.1c00860.pdf
Submitted - Breaking_Scaling_Relationships_in_CO2_Reduction_on_Copper_Alloys_with_Organic_Additives_v1.pdf
Supplemental Material - oc1c00860_si_001.pdf
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Additional details
- Alternative title
- Breaking Scaling Relationships in CO2 Reduction on Copper Alloys with Organic Additives
- PMCID
- PMC8554824
- Eprint ID
- 109461
- Resolver ID
- CaltechAUTHORS:20210610-080047277
- Department of Energy (DOE)
- DE-SC0021266
- Marie Curie Fellowship
- 793471
- Resnick Sustainability Institute
- Created
-
2021-06-10Created from EPrint's datestamp field
- Updated
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2023-03-24Created from EPrint's last_modified field
- Caltech groups
- Resnick Sustainability Institute, Liquid Sunlight Alliance