Hydrothermal reduction of CO2 captured by aqueous amine solutions into formate: Comparison between in situ generated H2 and gaseous H2 as reductant and evaluation of amine stability

Laura Quintana-Gómez , Luana Cristina Dos Santos , Fernando Cossio-Cid , Víctor Ciordia-Asenjo , Miguel Almarza , Alberto Goikoechea , Sergio Ferrero , Celedonio M․ Álvarez , José J․ Segovia , Ángel Martín , M․Dolores Bermejo
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Abstract

By CO2 Capture and Utilization technologies (CCU), organic compounds can be produced industrially in a sustainable manner, generating an economic benefit that offsets the cost of CO2 capture. In this context, the use of CO2 chemisorbed by amines to generate chemicals is an attractive alternative, given that large-scale facilities using absorption to capture CO2 are already operational. The aim of this work is to convert CO2 captured in aqueous amines, specifically 3-amino-1-propanol (AP) and 2-amino-2-methyl-1-propanol (AMP), to produce formate, using either Zn, Al or gaseous H2 as reductants and Pd/C as catalyst. The highest yield of formate (68 %) was achieved with AP (125 °C, 75 bar, 120 min) using gaseous hydrogen as reductant. Using metals as reductants, reaction yields were lower, with a 12 % yield at 200 °C as the best result. After reduction, NMR analyses show that the amines did not suffer degradation, raising the possibility of reusing them for CO2 capture in a continuous process. These results indicate that CO2-loaded amines reduction is a promising CCU technology that can be integrated with the current technologies for gas treatment.

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胺水溶液将捕获的 CO2 水热还原为甲酸盐:比较原位生成的 H2 与作为还原剂的气态 H2,评估胺的稳定性
通过二氧化碳捕获和利用技术(CCU),可以以可持续的方式在工业上生产有机化合物,产生的经济效益可以抵消二氧化碳捕获的成本。在这种情况下,利用胺对二氧化碳进行化学吸附来生产化学品是一种有吸引力的替代方法,因为利用吸收技术捕获二氧化碳的大型设施已经投入使用。这项工作的目的是利用 Zn、Al 或气态 H2 作为还原剂,Pd/C 作为催化剂,将捕集到水胺(特别是 3-氨基-1-丙醇 (AP) 和 2-氨基-2-甲基-1-丙醇 (AMP))中的二氧化碳转化为甲酸盐。使用气态氢作为还原剂,在 AP(125 °C,75 巴,120 分钟)条件下甲酸盐的产量最高(68%)。使用金属作为还原剂时,反应产率较低,200 ℃ 时的最佳产率为 12%。还原后的核磁共振分析表明,胺类物质没有发生降解,因此有可能在连续工艺中将其重新用于二氧化碳捕获。这些结果表明,二氧化碳负载胺还原是一种很有前景的 CCU 技术,可以与当前的气体处理技术相结合。
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