Zanatta Marcileia, García-Verdugo Eduardo, Sans Victor
Institute of Advanced Materials (INAM), Univesitat Jaume I, Avda Sos Baynat s/n, Castellón 12071, Spain.
Departamento de Química Inorgánica y Orgánica, Grupo de Química Sostenible y Supramolecular Universidad Jaume I, E-12071 Castellón, Spain.
ACS Sustain Chem Eng. 2023 Jun 23;11(26):9613-9619. doi: 10.1021/acssuschemeng.3c00890. eCollection 2023 Jul 3.
Direct air capture and integrated conversion is a very attractive strategy to reduce CO concentration in the atmosphere. However, the existing capturing processes are technologically challenging due to the costs of the processes and the low concentration of CO. The efficient valorization of the CO captured could help overcome many techno-economic limitations. Here, we present a novel economical methodology for direct air capture and conversion that is able to efficiently convert CO from the air into cyclic carbonates. The new approach employs commercially available basic ionic liquids, works without the need for sophisticated and expensive co-catalysts or sorbents and under mild reaction conditions. The CO from atmospheric air was efficiently captured by IL solution (0.98 molCO/mol) and, subsequently, completely converted into cyclic carbonates using epoxides or halohydrins potentially derived from biomass as substrates. A mechanism of conversion was evaluated, which helped to identify relevant reaction intermediates based on halohydrins, and consequently, a 100% selectivity was obtained using the new methodology.
直接空气捕获与集成转化是一种极具吸引力的降低大气中二氧化碳浓度的策略。然而,由于现有捕获过程的成本以及二氧化碳的低浓度,这些过程在技术上具有挑战性。捕获的二氧化碳的高效增值有助于克服许多技术经济限制。在此,我们提出了一种新颖的直接空气捕获与转化的经济方法,该方法能够将空气中的二氧化碳高效转化为环状碳酸酯。新方法采用市售的碱性离子液体,无需复杂且昂贵的助催化剂或吸附剂,并且在温和的反应条件下即可运行。大气中的二氧化碳被离子液体溶液高效捕获(0.98摩尔二氧化碳/摩尔),随后,使用可能源自生物质的环氧化物或卤代醇作为底物,将其完全转化为环状碳酸酯。评估了转化机理,这有助于基于卤代醇识别相关反应中间体,因此,使用新方法可获得100%的选择性。