Atomically dispersed Zn regulates Cu nanosheets for ampere-level CO₂ electroreduction to C₂₊ products

Maintaining efficient C–C coupling at ampere-level current density remains challenging because the rates of *CO generation and consumption become kinetically mismatched at Cu interfaces. Here, atomically dispersed Zn-regulated Cu nanosheets (Zn_SA-Cu NS) were generated via in situ electrochemical reconstruction of low-Zn-loaded Cu-based oxide nanosheet precursors. Zn nanoparticle-modified Cu nanosheets (Zn_NP-Cu NS), reconstructed from high-Zn-loaded precursors, were used as a control to evaluate the influence of the reconstructed Zn state. In a flow cell with a neutral electrolyte, Zn_SA-Cu NS delivers a Faradaic efficiency for multicarbon (C₂₊) products (FE_C2+) of 89.4% at 1.0 A cm^-2, outperforming most reported Cu-based catalysts at high current density. Quasi-in situ X–ray absorption spectroscopy, together with in situ Raman and infrared spectroscopy, reveals a structurally stable Cu framework, regulated *CO adsorption behavior, and enhanced formation of *CHO and *OCCHO intermediates. These results indicate that atomic Zn–Cu coordination facilitates *CO hydrogenation and subsequent C–C coupling, whereas Zn-rich particles dominated by Zn–Zn coordination are associated with preferential CO release. This work identifies the Zn dispersion state as a key structural parameter for sustaining C–C coupling during ampere-level CO₂ electroreduction.