High cost of pure CO feed constitutes a significant economic obstacle in industrial-scale CO electrolysis. Direct CO electrochemical conversion from flue gas has emerged as a promising strategy to reduce feed cost, while the O in flue gas cannot be ignored due to its strong reactivity. Here, we achieved fast, selective CO electrosynthesis directly fed with simulated oxygen-containing flue gas (95% CO+5% O) over the amine-confined Ag catalysts in a flow cell, among which dimethylamine-modified Ag exhibited 80.6% CO Faradaic efficiency with partial current density of 333.7 mA cm. spectroscopy demonstrated that dimethylamine confinement endows a robust CO adsorption-conversion capacity. Theoretical calculations further elucidated that amine modification could not only mediate CO adsorption and ∗COOH intermediate formation but could also block the ∗OOH intermediate pathway in the side reaction of oxygen reduction. These findings pave a new avenue for rational design of amine-confined electrocatalysts for direct flue gas conversion and utilization.

中文翻译：

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流通池中胺限域银催化剂的直接含氧模拟烟气电解

纯二氧化碳进料的高成本构成了工业规模二氧化碳电解的重大经济障碍。烟气中的直接 CO 电化学转化已成为降低饲料成本的一种有前途的策略，而烟气中的 O 由于其强反应性而不容忽视。在这里，我们在流通池中的胺限域银催化剂上直接用模拟含氧烟气（95％CO + 5％O）实现了快速、选择性的CO电合成，其中二甲胺修饰的Ag表现出80.6％的CO法拉第效率与部分电流密度为 333.7 mA cm。光谱表明二甲胺限制赋予了强大的CO吸附转化能力。理论计算进一步阐明，胺修饰不仅可以介导CO吸附和*COOH中间体的形成，而且还可以阻断氧还原副反应中*OOH中间体的途径。这些发现为合理设计用于直接烟气转化和利用的胺限域电催化剂开辟了新途径。