Guan Huanqin, Kim Ju Ye, Wei Kecheng, Agrawal Mayank, Peterson Andrew A, Sun Shouheng
Department of Chemistry, Brown University, Providence, Rhode Island, 02912, USA.
School of Engineering, Brown University, Providence, Rhode Island 02912, USA.
Nanoscale. 2024 Oct 10;16(39):18620-18628. doi: 10.1039/d4nr02925a.
Integrating air capture and conversion of CO is key to realizing energy sustainability. However, current integration approaches require high temperature and pressure, making them energy intensive. Here, we demonstrate a nanoparticle (NP) catalysis approach for the hydrogenation of alkyl carbonate, an intermediate obtained from the CO capture process, to formate, achieving one-pot air capture and conversion of CO under ambient conditions. The capture is realized in an ethylene glycol (EG) solution of KOH (EG-KOH) at room temperature, where CO is selectively converted into HO-CHCH-O-COOK (∼100% conversion). This carbonate is then hydrogenated using ammonia borane (under ambient pressure and at 50 °C) to formate (HCOOK) (>90% yield) in the presence of a stable Pd NP catalyst with EG being regenerated. Atomistic simulations suggest that the CO absorption process in the EG-KOH solution is energetically stable, and the catalyst surface provides the reaction site to break the C-O bond in the -O-COOK structure, enabling the hydrogenation of the alkyl carbonate to formate and the regeneration of EG. Our study provides a promising NP-catalysis approach for air capture and conversion of CO into value-added chemicals/fuels under ambient conditions.
将空气捕获与一氧化碳转化相结合是实现能源可持续性的关键。然而,目前的整合方法需要高温高压,使其能源密集。在此,我们展示了一种纳米颗粒(NP)催化方法,用于将碳酸酯(从一氧化碳捕获过程中获得的中间体)氢化为甲酸盐,在环境条件下实现一锅法空气捕获和一氧化碳转化。捕获在室温下氢氧化钾的乙二醇(EG-KOH)溶液中实现,其中一氧化碳被选择性地转化为HO-CHCH-O-COOK(转化率约100%)。然后在稳定的钯纳米颗粒催化剂存在下,使用氨硼烷(在常压和50°C下)将该碳酸盐氢化为甲酸盐(HCOOK)(产率>90%),同时乙二醇得以再生。原子模拟表明,EG-KOH溶液中的一氧化碳吸收过程在能量上是稳定的,催化剂表面提供了反应位点以断裂-O-COOK结构中的C-O键,从而实现碳酸酯氢化为甲酸盐以及乙二醇的再生。我们的研究为在环境条件下空气捕获和将一氧化碳转化为增值化学品/燃料提供了一种有前景的NP催化方法。