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<p>Graphitic carbon nitride, with its intrinsic nitrogen-rich framework and extended π-conjugated electronic structure, has emerged as a versatile support matrix for anchoring metal-based active sites. In this study, a series of monometallic and bimetallic copper-zinc catalysts with tunable copper/zinc molar ratios, supported on graphitic carbon nitride featuring a distinct wrinkled and porous structure, were synthesized. At a copper/zinc molar ratio of 1:1, the as-prepared catalyst, denoted as copper-zinc–graphitic carbon nitride (1:1), maximized the exposure of accessible active sites and accelerated mass transport of reactants and products, which were critical factors for boosting the kinetics of the carbon dioxide reduction reaction. Copper-zinc-graphitic carbon nitride (1:1) exhibited the highest current response, the smallest Tafel slope, and the largest electrochemical active surface area. At a potential of − 0.95&#xa0;V versus the reversible hydrogen electrode, this bimetallic catalyst achieved remarkable Faradaic efficiencies of 50.2% for carbon monoxide and 41.1% for methane, exhibiting negligible current decay over 12&#xa0;h of continuous electrolysis. Density functional theory calculations confirmed that introducing bimetallic sites onto the graphitic carbon support promoted internal charge transfer, which enhanced the adsorption of carbon dioxide molecules and lowered the energy barriers for the rate-determining steps in the carbon dioxide reduction reaction. Furthermore, the bimetallic synergy effectively suppressed the competing hydrogen evolution reaction, thereby improving the selectivity toward the carbon dioxide reduction reaction.</p> Graphical abstract <p></p>

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Internal charge transfer in copper-zinc-decorated graphitic carbon nitride tunes carbon dioxide reduction pathways

  • 期刊论文

  • 发表日期：

    2026年3月8日

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  • Daiming Song,
  • Xinmin Yang,
  • Liang Li,
  • Jing Yang,
  • Yufei Yan

摘要

Graphitic carbon nitride, with its intrinsic nitrogen-rich framework and extended π-conjugated electronic structure, has emerged as a versatile support matrix for anchoring metal-based active sites. In this study, a series of monometallic and bimetallic copper-zinc catalysts with tunable copper/zinc molar ratios, supported on graphitic carbon nitride featuring a distinct wrinkled and porous structure, were synthesized. At a copper/zinc molar ratio of 1:1, the as-prepared catalyst, denoted as copper-zinc–graphitic carbon nitride (1:1), maximized the exposure of accessible active sites and accelerated mass transport of reactants and products, which were critical factors for boosting the kinetics of the carbon dioxide reduction reaction. Copper-zinc-graphitic carbon nitride (1:1) exhibited the highest current response, the smallest Tafel slope, and the largest electrochemical active surface area. At a potential of − 0.95 V versus the reversible hydrogen electrode, this bimetallic catalyst achieved remarkable Faradaic efficiencies of 50.2% for carbon monoxide and 41.1% for methane, exhibiting negligible current decay over 12 h of continuous electrolysis. Density functional theory calculations confirmed that introducing bimetallic sites onto the graphitic carbon support promoted internal charge transfer, which enhanced the adsorption of carbon dioxide molecules and lowered the energy barriers for the rate-determining steps in the carbon dioxide reduction reaction. Furthermore, the bimetallic synergy effectively suppressed the competing hydrogen evolution reaction, thereby improving the selectivity toward the carbon dioxide reduction reaction.

Graphical abstract