Lee Yun-Yang, Cagli Eda, Klemm Aidan, Park Yensil, Dikki Ruth, Kidder Michelle K, Gurkan Burcu
Department of Chemical and Biomolecular Engineering, Case Western Reserve University, 10900 Euclid Ave, Cleveland, OH, 44106, USA.
Energy Science and Technology Directorate, Oak Ridge National Laboratory, 1 Bethel Valley Rd., Bldg. 5800, Oak Ridge, TN, 37830, USA.
ChemSusChem. 2023 Jul 7;16(13):e202300118. doi: 10.1002/cssc.202300118. Epub 2023 May 5.
Understanding the oxidative and thermal degradation of CO sorbents is essential for assessing long-term sorbent stability in direct air capture (DAC). The potential degradation pathway of imidazolium cyanopyrrolide, an ionic liquid (IL) functionalized for superior CO capacity and selectivity, is evaluated under accelerated degradation conditions to elucidate the secondary reactions that can occur during repetitive absorption-desorption thermal-swing cycles. The combined analysis from various spectroscopic, chromatographic, and thermal gravimetric measurements indicated that radical and S 2 mechanisms in degradation are encouraged by the nucleophilicity of the anion. Thickening of the liquid and gas evolution are accompanied by 50 % reduction in CO capacity after a 7-day exposure to O under 80 °C. To prevent long exposure to conventional thermal heating, microwave (MW) regeneration of the CO -reactive IL is used, where dielectric heating at 80 and 100 °C rapidly desorbs CO and regenerates the IL without any measurable degradation.
了解CO吸附剂的氧化和热降解对于评估直接空气捕获(DAC)中吸附剂的长期稳定性至关重要。在加速降解条件下评估了一种功能化的离子液体(IL)——氰基吡咯鎓咪唑盐的潜在降解途径,该离子液体具有优异的CO容量和选择性,以阐明在重复的吸附-解吸热摆动循环过程中可能发生的二级反应。各种光谱、色谱和热重测量的综合分析表明,阴离子的亲核性促进了降解中的自由基和S 2机制。在80°C下暴露于O 7天后,液体变稠和气体逸出伴随着CO容量降低50%。为了避免长时间暴露于传统热加热,采用了CO反应性IL的微波(MW)再生,其中在80和100°C下的介电加热可快速解吸出CO并使IL再生,且没有任何可测量的降解。