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A Critical Revisit of Zeolites for CO2 Desorption in Primary Amine Solution Argues Its Genuine Catalytic Function
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-09-06 , DOI: 10.1021/acscatal.2c02368
Cheng Zhou 1 , Ibrahim Khalil 1 , Fatima Rammal 1 , Michiel Dusselier 1 , Parveen Kumar 2 , Maxime Lacroix 3 , Ekaterina Makshina 1 , Yuhe Liao 4 , Bert F. Sels 1
Affiliation  

Zeolites are the most widely reported solid materials that are used in primary amine-containing postcombustion CO2 capture processes for quicker solvent regeneration at a lower energy consumption. Catalytic solvolysis of the carbamate intermediate, assisted by the Brönsted acid sites (BAS), is commonly accepted as an explanation. However, there is little, if any, attention given to the regeneration of BAS in such basic amine-rich solution. Herein, we revisit the role of zeolite for CO2 desorption in primary amine solution at room to moderately elevated temperature ranges. We noticed indeed an accelerating effect on the CO2 desorption rate in the presence of BAS. Both their numbers as well as their accessibility for the amine-CO2 adduct (i.e., carbamate) (direct) or amine (indirect pathway) are important. However, we also noticed, using spectroscopic techniques and by zeolite reuse, a very strong chemical interaction between BAS and the regenerated amine. This suggests that BAS recovery to close the catalytic cycle is difficult and that zeolites can hardly be considered as genuine catalysts, but rather, this study concludes a merely stoichiometric effect of the zeolites for the overall desorption process, and this is in contrast to reference oxides such as TiO(OH)2.

中文翻译:

对沸石在伯胺溶液中解吸 CO2 的批判性回顾论证了其真正的催化功能

沸石是最广泛报道的固体材料,可用于含伯胺的燃烧后 CO 2捕集工艺,以更低的能耗实现更快的溶剂再生。在布朗斯台德酸位 (BAS) 的辅助下,氨基甲酸酯中间体的催化溶剂分解被普遍接受为一种解释。然而,对于在这种富含碱性胺的溶液中的 BAS 再生,几乎没有给予任何关注(如果有的话)。在此,我们重新审视了沸石在室温至适度升高的温度范围内对伯胺溶液中CO 2解吸的作用。我们确实注意到在 BAS 存在下对 CO 2解吸速率的加速作用。它们的数量以及它们对胺-CO 2的可及性加合物(即氨基甲酸酯)(直接)或胺(间接途径)很重要。然而,我们也注意到,使用光谱技术和沸石再利用,BAS 和再生胺之间存在非常强的化学相互作用。这表明 BAS 回收以关闭催化循环是困难的,沸石很难被认为是真正的催化剂,相反,本研究得出结论,沸石对整个解吸过程仅具有化学计量效应,这与参考氧化物形成对比如 TiO(OH) 2
更新日期:2022-09-06
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