“…A strategy involving reactor cascades, encompassing two separate systems corresponding to sequential CO 2 -to-CO and CO-to-C 2+ steps, has been implemented. , Despite its potential to boost selectivity for carbon-intensive products, reactor cascade systems encounter challenges related to operability, stability, high cost, and energy consumption. An alternative approach, tandem catalysis, couples independent single-atom sites for CO generation with Cu sites for subsequent deep reduction reactions, which effectively decouples multiple steps and increases the accessible CO concentration around Cu surfaces. , Notably, Ni single-atom (Ni-SA) catalysts have been shown to achieve efficient CO 2 RR performance with over 90% selectivity for CO production. − Furthermore, the spatial arrangement of these two sites can greatly affect the local CO concentration and the utilization efficiency of CO intermediates. , However, previous tandem strategies usually adopt the coplanar design, which encounters challenges associated with slow mass transfer and short residence time of CO, ultimately reducing the CO coverage on the Cu surface. Therefore, optimizing the spatial distribution of the different catalytic sites along the direction of the gas channel is critical to effectively overcome mass transport of CO and increase local CO enrichment.…”