Kiani Aida, Rosaria Acocella Maria, Auriemma Finizia, Guerra Gaetano
Department of Chemistry and Biology "A. Zambelli", University of Salerno, Via Giovanni Paolo II, 84084, Fisciano, Italy.
Department of Chemical Science, University of Napoli "Federico II", Via Cintia, Complesso Monte Sant'Amgelo 21, Napoli, 80126, Italy.
ChemSusChem. 2024 Dec 6;17(23):e202400264. doi: 10.1002/cssc.202400264. Epub 2024 Aug 8.
This paper explores possible procedures to accelerate CO capture from ambient air by a crystalline alkylamine surfactant (octadecylamine), leading to the corresponding crystalline ammonium-carbamate. Conversion of the amine to the carbamate, in different conditions, is studied by four different techniques: WAXD, FTIR, TGA, and DSC. The WAXD study also gives relevant information on the crystal structures of both amine and derived carbamate. Kinetics of reactions of the crystalline amine are mainly studied by DSC scans, by evaluating melting enthalpies of residual amine. The kinetics of conversion of the amine in ambient CO is strongly accelerated by ball milling with full conversion achieved after only 4 h, while the reaction kinetics of amine powder simply exposed to ambient CO is complete only after nearly 10 h. A substantial increase in kinetics of the solid-state amine reaction with ambient CO can be also achieved by increasing the temperature up to 50 °C, i. e. at a temperature slightly lower than amine melting. However, the time for full conversion remains much higher than for room-temperature ball-milled amine (roughly 10 h vs 4 h). Hence, suitable ball-milling procedures can lead to complete and relatively fast conversion of the crystalline amine to the crystalline ammonium-carbamate, even with ambient CO.
本文探讨了通过结晶烷基胺表面活性剂(十八烷基胺)加速从环境空气中捕获二氧化碳,生成相应结晶氨基甲酸盐的可能方法。采用四种不同技术研究了在不同条件下胺向氨基甲酸盐的转化:广角X射线衍射(WAXD)、傅里叶变换红外光谱(FTIR)、热重分析(TGA)和差示扫描量热法(DSC)。WAXD研究还提供了有关胺及其衍生氨基甲酸盐晶体结构的相关信息。通过评估残余胺的熔化焓,主要利用DSC扫描研究了结晶胺的反应动力学。通过球磨,胺在环境二氧化碳中的转化动力学得到显著加速,仅4小时后即可实现完全转化,而单纯暴露于环境二氧化碳中的胺粉末反应动力学在近10小时后才完成。将温度提高到50°C(即略低于胺熔点的温度),也可以显著提高固态胺与环境二氧化碳反应的动力学。然而,完全转化所需的时间仍远高于室温球磨胺(约10小时对4小时)。因此,即使在环境二氧化碳条件下,合适的球磨方法也能使结晶胺完全且相对快速地转化为结晶氨基甲酸盐。