biostudies-literatureZhu JPolish Innovation Economy Operational ProgramChinese Scholarship Councile2505306https://www.ebi.ac.uk/biostudies/studies/S-EPMC12332811biostudies-literatureUnknown21(31)Bimetallic catalysts are appealing for electrochemical CO<sub>2</sub> reduction reaction (ECO2RR), yet the introduction of bimetallic sites leads to an incomprehensive understanding of the metal atom interaction and catalytic mechanism. In this study, a series of bimetallic Ni<sub>x</sub>Cu<sub>y</sub>@NC catalysts with varied Ni to Cu weight ratios are prepared. The as-prepared Ni<sub>2</sub>Cu<sub>1</sub>@NC catalyst shows high carbon monoxide (CO) Faradaic efficiencies (FE<sub>CO</sub>) over 90% in a broad potential range of -0.7 to -1.1 V (vs reversible hydrogen electrode (RHE)) with an exceptional durability of CO selectivity over 80% and a high partial current density of -44 mA cm<sup>-2</sup> at an extremely high potential of -1.3 V (vs RHE). The distinguished CO selectivity and activity are primarily attributed to the integration of Ni and Cu, which lowers the d-band center position and reconstructs the electronic structure according to the valence band spectra. More specifically, the downshifted d-band center position weakens the interaction strength with the *CO intermediate on the Ni<sub>2</sub>Cu<sub>1</sub>@NC catalyst's surface during the ECO2RR process, resulting in fast *CO desorption and high CO selectivity. This study provides researchers with a new insight for designing and optimizing the electrocatalysts for ECO2RR.Small (Weinheim an der Bergstrasse, Germany)Strategic Modulation of CO Intermediate Desorption Dynamics on Bimetallic Ni<sub>x</sub>Cu<sub>y</sub>@NC Catalyst: Synergistic Electrocatalysis for Sustainable CO<sub>2</sub> Conversion.PMC12332811POIR.04.02.00-00-D001/20POIG.02.01.00-12-023/08202008440279Li GKustrowski PZhu JDas SLu ZWang ZCool PRokicinska AfalseStrategic Modulation of CO Intermediate Desorption Dynamics on Bimetallic Ni<sub>x</sub>Cu<sub>y</sub>@NC Catalyst: Synergistic Electrocatalysis for Sustainable CO<sub>2</sub> Conversion.Bimetallic catalysts are appealing for electrochemical CO<sub>2</sub> reduction reaction (ECO2RR), yet the introduction of bimetallic sites leads to an incomprehensive understanding of the metal atom interaction and catalytic mechanism. In this study, a series of bimetallic Ni<sub>x</sub>Cu<sub>y</sub>@NC catalysts with varied Ni to Cu weight ratios are prepared. The as-prepared Ni<sub>2</sub>Cu<sub>1</sub>@NC catalyst shows high carbon monoxide (CO) Faradaic efficiencies (FE<sub>CO</sub>) over 90% in a broad potential range of -0.7 to -1.1 V (vs reversible hydrogen electrode (RHE)) with an exceptional durability of CO selectivity over 80% and a high partial current density of -44 mA cm<sup>-2</sup> at an extremely high potential of -1.3 V (vs RHE). The distinguished CO selectivity and activity are primarily attributed to the integration of Ni and Cu, which lowers the d-band center position and reconstructs the electronic structure according to the valence band spectra. More specifically, the downshifted d-band center position weakens the interaction strength with the *CO intermediate on the Ni<sub>2</sub>Cu<sub>1</sub>@NC catalyst's surface during the ECO2RR process, resulting in fast *CO desorption and high CO selectivity. This study provides researchers with a new insight for designing and optimizing the electrocatalysts for ECO2RR.2025-01-01T00:00:00Z2025 Aug2026-04-15T19:17:08.471Z2026-04-07T14:01:14.668ZS-EPMC123328114047856810.1002/smll.202505306