Atomic Origins of Roughness-Enhanced Multicarbon Selectivity in Copper-Catalyzed CO2 Electroreduction
Source abstract
Abstract
Surface roughness in copper catalysts has emerged as a critical factor for enhancing the C 2+ product selectivity in electrochemical CO 2 reduction (eCO2RR), but the underlying mechanistic origins remain unclear. Here, we employ simulated sputtering and annealing to generate copper surfaces with varying roughness factors. Atomic-scale site-analysis of our model surfaces reveals that roughness increases the density of 4-fold and mixed-coordination sites, promoting CO adsorption and subsequent C–C coupling pathways. Selectivity maps overlaid with site distributions demonstrate that increased surface roughness enhances the fraction of active sites favoring C 2+ products, aligning with the experimental trends. Our findings highlight how roughness-induced atomic structural modulation promotes nanoenvironments with mixed high and low coordination 4-fold sites able to sustain C–C coupling, explaining observed selectivity enhancements. This work provides new insights into roughness-dependent site reactivity and offers strategies for rational catalyst design to optimize multicarbon product formation in eCO2RR.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Machine Learning in Materials Science
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, 443 Via Ortega, 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
Department of Chemistry and Chemical Engineering, Chalmers University of Technology, Kemivägen 10, 412 96 Gothenburg, Sweden
Chemical Sciences Division
Lawrence Berkeley National Laboratory
Department of Chemical and Biomolecular Engineering
University of California
Department of Chemical Engineering
Texas Tech University
Kenneth S. Pitzer Center for Theoretical Chemistry, Department of Chemistry
Funding
Welch Foundation · Basic Energy Sciences · Knut och Alice Wallenbergs Stiftelse · Energy Area of Advance, Chalmers Tekniska H?gskola
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