Promoted CO2 Desorption in N-(2-Hydroxyethyl)ethylenediamine Solutions Catalyzed by Histidine

IF 4.5 3区 化学 Q2 CHEMISTRY, PHYSICAL
Catalysts Pub Date : 2025-12-29 DOI:10.3390/catal16010024
Siming Chen, Xinzhu Zhang, Guangfei Xing, Lei Zhang, Le Chang, Yubing Xu, Yongchun Zhang
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Abstract

This study systematically investigates the catalytic effect of histidine (HIS) on CO2 desorption in amine-based solvents, with a primary focus on 30 wt% N-(2-aminoethylamino)ethanol (AEEA) and its blends with N-methyldiethanolamine (MDEA). Experimental results show that the addition of 0.22 wt% HIS significantly enhances both the equilibrium desorption amount and the maximum desorption rate of CO2, particularly at elevated temperatures (e.g., 100 °C). Under optimal conditions, HIS increased the maximum desorption rate by 22.1% and reduced the heat duty to 71.7% compared to the non-catalytic benchmark. The catalytic performance was further confirmed in AEEA-MDEA mixed solvents, with the most pronounced effect observed in the 3:2 molar ratio system, where HIS enhanced both the equilibrium desorption amount and the maximum desorption rate by 15.3% and 20.8%, respectively. Through 13C NMR analysis and pH-dependent speciation monitoring, we revealed that HIS alters the reaction pathway by suppressing the formation of stable carbamate species (AEEA(a)COO−). The protonated (HIS+) and neutral (HIS±) forms were identified as the active species that promote more direct CO2 release from carbamate, while the deprotonated (HIS−) form facilitates proton transfer and amine regeneration. HIS also exhibited excellent catalytic stability over 10 absorption–desorption cycles. These findings highlight HIS as an efficient and stable organocatalyst for energy-efficient CO2 desorption processes.
组氨酸催化N-(2-羟乙基)乙二胺溶液促进CO2解吸
本研究系统地研究了组氨酸(HIS)在胺基溶剂中对CO2解吸的催化作用,主要研究了30 wt% N-(2-氨基乙胺)乙醇(AEEA)及其与N-甲基二乙醇胺(MDEA)的混合物。实验结果表明,添加0.22 wt%的HIS显著提高了CO2的平衡解吸量和最大解吸速率,特别是在高温下(例如100℃)。在最佳条件下,与非催化基准相比,HIS的最大解吸率提高了22.1%,热负荷降低到71.7%。在AEEA-MDEA混合溶剂中进一步证实了HIS的催化性能,其中在3:2摩尔比体系中效果最为明显,HIS的平衡解吸量和最大解吸速率分别提高了15.3%和20.8%。通过13C核磁共振分析和ph依赖性物种形成监测,我们发现HIS通过抑制稳定氨基甲酸酯物种(AEEA(a)COO−)的形成来改变反应途径。质子化(HIS+)和中性(HIS±)形式被认为是促进氨基甲酸酯更直接释放CO2的活性物质,而去质子化(HIS−)形式有助于质子转移和胺再生。HIS在10次吸附-解吸循环中也表现出优异的催化稳定性。这些发现突出了HIS作为一种高效稳定的有机催化剂用于节能CO2脱附过程。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Catalysts
Catalysts CHEMISTRY, PHYSICAL-
CiteScore
6.80
自引率
7.70%
发文量
1330
审稿时长
3 months
期刊介绍: Catalysts (ISSN 2073-4344) is an international open access journal of catalysts and catalyzed reactions. Catalysts publishes reviews, regular research papers (articles) and short communications. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced.
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