The electrochemical reduction of carbon dioxide (CO₂) to value-added materials has received considerable attention. Both bulk transition-metal catalysts and molecular catalysts affixed to conductive noncatalytic solid supports represent a promising approach toward the electroreduction of CO₂. Here, we report a combined silver (Ag) and pyridine catalyst through a one-pot and irreversible electrografting process, which demonstrates the enhanced CO₂ conversion versus individual counterparts. We find that by tailoring the pyridine carbon chain length, a 200 mV shift in the onset potential is obtainable compared to the bare silver electrode. A 10-fold activity enhancement at −0.7 V vs reversible hydrogen electrode (RHE) is then observed with demonstratable higher partial current densities for CO, indicating that a cocatalytic effect is attainable through the integration of the two different catalytic structures. We extended the performance to a flow cell operating at 150 mA/cm², demonstrating the approach’s potential for substantial adaptation with various transition metals as supports and electrografted molecular cocatalysts.

中文翻译：

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通过表面工程电接枝吡啶在银催化剂上电解 CO2

将二氧化碳（CO ₂）电化学还原为增值材料已受到广泛关注。本体过渡金属催化剂和附着在导电非催化固体载体上的分子催化剂都代表了一种有前途的 CO ₂电还原方法。在这里，我们通过一锅法和不可逆的电接枝工艺报道了一种银 (Ag) 和吡啶的组合催化剂，证明了增强的 CO ₂转换与个别对应物。我们发现，通过调整吡啶碳链长度，与裸银电极相比，起始电位可发生 200 mV 的偏移。然后观察到在 -0.7 V 与可逆氢电极 (RHE) 相比，活性提高了 10 倍，CO 的分电流密度明显更高，这表明通过整合两种不同的催化结构可以获得助催化效果。我们将性能扩展到在 150 mA/cm ²下运行的流通池，证明了该方法在大量适应各种过渡金属作为载体和电接枝分子助催化剂的潜力。