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Article Abstract
Using atomically precise Ag(SPhF)(P(Ph--OMe)) nanoclusters as a well-defined platform, we systematically tune the number of Cu dopants to unravel Ag-Cu synergistic effects in electrocatalytic CO reduction. A catalyst containing, on average, two Cu atoms per cluster (AgCu) delivers a CH faradaic efficiency of 17.1% at -1.6 V RHE-dramatically higher than both the over-doped analogue AgCu (11.16%) and the undoped Ag parent (∼0%). Density-functional-theory calculations reveal that introducing one to two Cu atoms optimally raises the Cu valence state, strengthening *CO adsorption and thereby accelerating the *CO → *CHO step that governs CH formation. These results demonstrate that 'less is more': beyond a critical Cu loading, the cooperative electronic advantages are diminished and activity declines.
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