The electrochemical CO₂ reduction reaction (CO₂RR) offers an environmentally friendly method to transform sequestered CO₂. While gas-phase electrolysis systems provide high efficiency, gas-phase electrolysis systems face challenges related to carbonate precipitate formation and crossover. As an alternative, liquid-phase (bi)carbonate electrolysis systems based on the use of bipolar membrane (BPM) electrode assemblies have emerged. These systems not only streamline the carbon capture and conversion process but also present economic benefits. However, liquid-phase (bi)carbonate electrolysis cells suffer limited stability and selectivity at relevant operating currents. Here, utilizing a Ni-based single atom catalyst (Ni-SAC) and bicarbonate electrolyte, we demonstrate exceptional CO faradaic efficiency (93%) at a partial current density of −186 mA cm⁻² at −3.7 V for over 18 hours with an integrated carbon capture system. Furthermore, we conducted a comparative analysis of various performance metrics between bicarbonate electrolysis and CO₂ gas electrolysis. Our results highlight the superior advantages of BPM-based electrolysis in terms of CO₂ utilization efficiency, stability, and CO product concentration in the outlet stream. Despite a higher energy demand, BPM-based electrolysis presents a technologically promising alternative to conventional CO₂ gas-phase systems. This breakthrough paves the way for efficient direct carbon capture and conversion, offering a promising pathway toward a more sustainable and carbon-neutral future.

中文翻译：

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通过双极膜电解从碳酸氢盐中集成碳捕获和二氧化碳生产

电化学CO ₂还原反应(CO ₂ RR) 提供了一种环保的方法来转化封存的CO ₂。虽然气相电解系统提供高效率，但气相电解系统面临与碳酸盐沉淀形成和交叉相关的挑战。作为替代方案，基于使用双极膜 (BPM) 电极组件的液相碳酸（氢）盐电解系统已经出现。这些系统不仅简化了碳捕获和转化过程，而且还带来了经济效益。然而，液相碳酸（氢）盐电解池在相关工作电流下的稳定性和选择性有限。在这里，利用镍基单原子催化剂（Ni-SAC）和碳酸氢盐电解质，我们在-3.7 V、-186 mA cm ^-2的部分电流密度下展示了出色的CO法拉第效率（93％）超过18小时集成的碳捕获系统。此外，我们对碳酸氢盐电解和CO ₂气体电解之间的各种性能指标进行了比较分析。我们的结果凸显了基于 BPM 的电解在 CO ₂利用效率、稳定性和出口流中 CO 产品浓度方面的卓越优势。尽管能源需求较高，但基于 BPM 的电解为传统 CO ₂气相系统提供了一种技术上有前景的替代方案。这一突破为高效的直接碳捕获和转化铺平了道路，为实现更加可持续和碳中和的未来提供了一条充满希望的途径。