Interphases are critical in electrochemical systems, influencing performance by controlling ion transport and stability. This study explores a metal-organic interphase in the electrocatalytic reduction of CO (CORR) on Cu, extending the concept of interphases to CO conversion. Investigating organic modifications on CuO, we discover metal-organic interphases over 10 nm thick in highly ethanol-selective systems, contrary to the expected monolayer adsorption. Using an automated platform, 1080 CORR experiments with 180 molecular modifiers identify functional groups affecting selectivity for ethanol and multi-carbon (C) products. We find that these modifiers consistently produce metal-organic interphases on the Cu or CuO surface. These interphases modulate Cu coordination, CORR intermediates, and interfacial water configuration, significantly improving electrocatalytic performance. Testing across 11 CuO-based catalysts validates this approach, culminating in the development of two electrocatalysts that achieve ~80% faradaic efficiency for C products with ethanol partial current densities up to 328 and 507 mA cm. This study highlights the pivotal role of interphases in CORR, advancing CO conversion technologies.
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| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC11871064 | PMC |
| http://dx.doi.org/10.1038/s41467-025-57221-x | DOI Listing |
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