Dual‐Atom Dopants Activated Copper Dilute Alloy Boosts Electroreduction CO ₂ ‐to‐C ₂₊ Products at Ampere‐Level Current Density

ABSTRACT Electrochemical CO 2 reduction reaction (CO 2 RR) with H 2 O as the hydrogen donor provides a sustainable and green route to product energy‐dense multi‐carbon (C 2+ ) products, but guiding selectivity remains challenging due to competing pathways. Here, we construct atomic Al and Zn into nanoporous Cu to regulate the adsorption energies of *CO and *H intermediates. Efficient electrosynthesis of C 2+ products from CO 2 RR are achieved, delivering a Faradaic efficiency approaching 91.4%, a partial current density of −1.5 A cm −2 , and a C 2+ /C 1 ratio up to 26.9 in gas‐fed flow cells. Experimental and theoretical studies reveal that the Al 1 ─Cu sites preferentially promote CO 2 activation, while Zn 1 ─Cu sites facilitate H 2 O dissociation to ensure intermediate hydrogenation, thus synergistically driving the conversion of *CO to *CHO and promoting asymmetric *CHO─*CO coupling to form C 2+ products on Cu site. This work establishes a dual‐atom alloy that enhances proton supply to CO 2 and intermediates while regulating *CO coverage, providing a rational design concept for electrocatalysts toward the selective reduction of CO 2 to C 2+ products.