Electrochemically mediated carbon capture utilizing redox-tunable organic sorbents has emerged as a promising strategy to mitigate anthropogenic carbon dioxide emissions. However, most reported systems are sensitive to molecular oxygen, severely limiting their application under ambient air conditions. Here we demonstrate an electrochemical carbon capture concept via non-aqueous proton-coupled electron transfer, where alkoxides are employed as the active sorbent while carbon dioxide absorption and desorption are modulated reversibly by the redox-tunable Brønsted basicity of certain organic molecules. Since all species involved in the process have outstanding oxygen stability and relatively low vapour pressure, our electrochemically mediated carbon capture mechanism intrinsically minimizes parasitic reactions and evaporative losses under aerobic conditions. Flow-based prototypes are demonstrated to operate efficiently in the presence of 20% oxygen under various practically relevant carbon dioxide feed concentrations, paving a way towards effective carbon capture driven by electrochemical stimuli.

利用氧化还原可调有机吸附剂进行电化学介导的碳捕获已成为减少人为二氧化碳排放的一种有前景的策略。然而，大多数报道的系统对分子氧敏感，严重限制了它们在环境空气条件下的应用。在这里，我们通过非水质子耦合电子转移演示了电化学碳捕获概念，其中醇盐用作活性吸附剂，而二氧化碳的吸收和解吸则通过某些有机分子的氧化还原可调的布朗斯特碱度可逆地调节。由于该过程中涉及的所有物质都具有出色的氧稳定性和相对较低的蒸气压，因此我们的电化学介导的碳捕获机制本质上最大限度地减少了有氧条件下的寄生反应和蒸发损失。基于流的原型被证明可以在 20% 氧气存在下、各种实际相关的二氧化碳进料浓度下有效运行，为电化学刺激驱动的有效碳捕获铺平了道路。