Guan Xun, Zhang Ge, Li Jinlei, Kim Sang Cheol, Feng Guangxia, Li Yuqi, Cui Tony, Brest Adam, Cui Yi
Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305.
Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA 94025.
Proc Natl Acad Sci U S A. 2024 Nov 5;121(45):e2410841121. doi: 10.1073/pnas.2410841121. Epub 2024 Oct 28.
Electrochemical pH-swing strategies offer a promising avenue for cost-effective and energy-efficient carbon dioxide (CO) capture, surpassing the traditional thermally activated processes and humidity-sensitive techniques. The concept of elevating seawater's alkalinity for scalable CO capture without introducing additional chemical as reactant is particularly intriguing due to its minimal environmental impact. However, current commercial plants like chlor-alkali process or water electrolysis demand high thermodynamic voltages of 2.2 V and 1.23 V, respectively, for the production of sodium hydroxide (NaOH) from seawater. These high voltages are attributed to the asymmetric electrochemical reactions, where two completely different reactions take place at the anode and cathode. Here, we developed a symmetric electrochemical system for seawater alkalization based on a highly reversible and identical reaction taking place at the anode and cathode. We utilize hydrogen evolution reaction at the cathode, where the generated hydrogen is looped to the anode for hydrogen oxidation reaction. Theoretical calculations indicate an impressively low energy requirement ranging from 0.07 to 0.53 kWh/kg NaOH for established pH differences of 1.7 to 13.4. Experimentally, we achieved the alkalization with an energy consumption of 0.63 kWh/kg NaOH, which is only 38% of the theoretical energy requirements of the chlor-alkali process (1.64 kWh/kg NaOH). Further tests demonstrated the system's potential of enduring high current densities (~20 mA/cm) and operating stability over an extended period (>110 h), showing its potential for future applications. Notably, the CO adsorption tests performed with alkalized seawater exhibited remarkably improved CO capture dictated by the production of hydroxide compared to the pristine seawater.
电化学pH摆动策略为经济高效的二氧化碳(CO₂)捕获提供了一条有前景的途径,超越了传统的热激活工艺和湿度敏感技术。通过提高海水碱度来实现可扩展的CO₂捕获且不引入额外化学物质作为反应物的概念,因其对环境影响极小而特别引人关注。然而,目前的商业工厂,如氯碱工艺或水电解,分别需要2.2 V和1.23 V的高热力学电压才能从海水中生产氢氧化钠(NaOH)。这些高电压归因于不对称的电化学反应,即在阳极和阴极发生两个完全不同的反应。在此,我们基于在阳极和阴极发生的高度可逆且相同的反应,开发了一种用于海水碱化的对称电化学系统。我们利用阴极的析氢反应,将产生的氢气循环到阳极进行氢氧化反应。理论计算表明,对于1.7至13.4的既定pH差值,能量需求低至0.07至0.53 kWh/kg NaOH,令人印象深刻。在实验中,我们实现了碱化,NaOH的能耗为0.63 kWh/kg,仅为氯碱工艺理论能量需求(1.64 kWh/kg NaOH)的38%。进一步测试表明该系统能够承受高电流密度(约20 mA/cm²)并在较长时间(>110 h)内保持运行稳定性,显示出其在未来应用中的潜力。值得注意的是,与原始海水相比,用碱化海水进行的CO₂吸附测试显示,由于氢氧化物的产生,CO₂捕获能力有显著提高。