醌功能化碳作为电化学二氧化碳捕获的新材料,Journal of Materials Chemistry A

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醌功能化碳作为电化学二氧化碳捕获的新材料
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-06-30 , DOI: 10.1039/d3ta02213g
Niamh A. Hartley ₁ , Suzi M. Pugh ₁ , Zhen Xu ₁ , Daniel C. Y. Leong ₁ , Adam Jaffe ₂ , Alexander C. Forse ₁

Affiliation

对具有成本效益的二氧化碳捕获技术的需求正在迅速增加。为了在下个世纪内将全球气温升高限制在1.5°C以内，需要大幅提高CO ₂减排水平。电流捕获技术，即胺洗涤带来了限制广泛部署的几个挑战：高再生能量、高运营成本和降解问题。电化学驱动的二氧化碳捕获是一种新兴的节能技术，可以解决胺的一些局限性。例如，氧化还原活性醌分子能够在电化学还原后捕获二氧化碳，然后可以在电化学氧化时再生。_{尽管用于电化学CO 2}捕获的醌化学取得了巨大进步，然而，将醌集成到碳捕获装置中仍然是一个持续的挑战。_{在这里，我们提出了一种用于电化学 CO 2}的新型醌功能化电极捕获，利用重氮自由基反应将醌分子接枝到多孔碳表面。通过将氧化还原活性分子接枝到该导电表面，不仅当结合的醌物质被电化学还原时二氧化碳捕获显着增强，而且功能化过程还改善了碳材料的能量存储。_{通过CO 2}存在下的恒流实验，观察到可逆碳捕获，初始吸收容量为0.4 mmol g ^-1，经过100个循环稳定至0.2 mmol g ^-1，能耗为254 kJ mol ^-1每个周期。我们对醌官能化碳的简便低成本合成具有高度可调性，因为碳和氧化还原活性分子都可以被修饰，因此我们的工作为设计和发现用于电化学CO 2 捕获的改进电极材料铺平了_道路。

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Quinone-functionalised carbons as new materials for electrochemical carbon dioxide capture

The need for cost-effective carbon dioxide capture technology is rapidly increasing. To limit the global temperature increase to 1.5 °C within the next century, the level of CO₂ mitigation needs to increase drastically. Current capture technology, i.e., amine scrubbing, provides several challenges that limit widespread deployment: high regeneration energy, high operational costs and degradation issues. An emerging energy-efficient technology that can address some of the limitations of amines is electrochemically driven carbon dioxide capture. For example, redox-active quinone molecules are capable of capturing carbon dioxide following electrochemical reduction, and can then be regenerated upon electrochemical oxidation. Despite great advances in the chemistry of quinones for electrochemical CO₂ capture, however, the integration of quinones in carbon capture devices remains an ongoing challenge. Here we present a new class of quinone-functionalized electrodes for electrochemical CO₂ capture, using the diazonium radical reaction to graft quinone molecules to a porous carbon surface. By grafting redox-active molecules to this conductive surface, not only is carbon dioxide capture significantly enhanced when the bound quinone species are electrochemically reduced, but the functionalization process also improves the energy storage of the carbon material. Through constant current experiments in the presence of CO₂, reversible carbon capture was observed with initial uptake capacities at 0.4 mmol g⁻¹ which stabilizes to 0.2 mmol g⁻¹ over 100 cycles with an energy consumption of 254 kJ mol⁻¹ per cycle. Our facile low-cost synthesis of quinone-functionalised carbons is highly tunable since both the carbon and redox-active molecule can be modified, and our work therefore paves the way for the design and discovery of improved electrode materials for electrochemical CO₂ capture.

更新日期：2023-06-30

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