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   Thin films of Ni 3 Al and Ni 3 Ga on carbon solid supports have been shown to generate multi-carbon products in electrochemical CO 2 reduction, an activity profile that, until recently, was ascribed exclusively to Cu-based catalysts. This catalytic behavior has introduced questions regarding the role of each metal, as well as other system components, during CO 2 reduction. Here, the significance of electrode structure and solid support choice in determining higher- versus lower-order reduction products is explored, and the commonly invoked Fischer–Tropsch-type mechanism of CO 2 reduction to multi-carbon products is indirectly probed. Electrochemical studies of both intermetallic and non-mixed Ni–Group 13 catalyst films suggest that intermetallic character is required to achieve C2 and C3 products irrespective of carbon support choice, negating the possibility of separate metal sites performing distinct yet complementary roles in CO 2 reduction. Furthermore, Ni 3 Al and Ni 3 Ga were shown to be incapable of generating higher-order reduction products in D 2 O, suggesting a departure from accepted mechanisms for CO 2 reduction on Cu. Additional routes to multi-carbon products may therefore be accessible when developing intermetallic catalysts for CO 2 electroreduction. 

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