Faculty of Chemistry, University of Warsaw , 02-093 Warsaw, Poland.
Institute of Physical Chemistry, University of Innsbruck , A-6020 Innsbruck, Austria.
ACS Appl Mater Interfaces. 2017 Apr 19;9(15):12919-12923. doi: 10.1021/acsami.7b01875. Epub 2017 Apr 6.
Developing efficient methods for capture and controlled release of carbon dioxide is crucial to any carbon capture and utilization technology. Herein we present an approach using an organic semiconductor electrode to electrochemically capture dissolved CO in aqueous electrolytes. The process relies on electrochemical reduction of a thin film of a naphthalene bisimide derivative, 2,7-bis(4-(2-(2-ethylhexyl)thiazol-4-yl)phenyl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (NBIT). This molecule is specifically tailored to afford one-electron reversible and one-electron quasi-reversible reduction in aqueous conditions while not dissolving or degrading. The reduced NBIT reacts with CO to form a stable semicarbonate salt, which can be subsequently oxidized electrochemically to release CO. The semicarbonate structure is confirmed by in situ IR spectroelectrochemistry. This process of capturing and releasing carbon dioxide can be realized in an oxygen-free environment under ambient pressure and temperature, with uptake efficiency for CO capture of ∼2.3 mmol g. This is on par with the best solution-phase amine chemical capture technologies available today.
开发高效的二氧化碳捕获和控制释放方法对于任何碳捕集和利用技术都至关重要。在此，我们提出了一种使用有机半导体电极电化学捕获水溶液中溶解的 CO 的方法。该过程依赖于萘二酰亚胺衍生物 2,7-双(4-(2-(2-乙基己基)噻唑-4-基)苯基)苯并[lmn][3,8]菲咯啉-1,3,6,8(2H,7H)-四酮 (NBIT) 的薄膜电化学还原。该分子经过专门设计，可在水溶液中提供单电子可逆和单电子准可逆还原，而不会溶解或降解。还原的 NBIT 与 CO 反应形成稳定的半碳酸盐盐，随后可通过电化学氧化释放 CO。半碳酸盐结构通过原位红外光谱电化学得到证实。在无氧环境、环境压力和温度下，可以实现二氧化碳的捕获和释放，CO 的捕获效率约为 2.3 mmol g。这与当今可用的最佳溶液相胺化学捕获技术相当。
