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CO2-Induced Degradation of Amine-Containing Adsorbents: Reaction Products and Pathways
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2012-08-09 , DOI: 10.1021/ja304888a
Abdelhamid Sayari 1 , Aliakbar Heydari-Gorji 1 , Yong Yang 1
Affiliation  

A comprehensive study was conducted to investigate the stability of a wide variety of mesoporous silica-supported amine-containing adsorbents in the presence of carbon dioxide under dry conditions. CO(2)-induced degradation of grafted primary and secondary monoamines (pMono, sMono), diamines with one primary and one secondary amines (Diamine) and triamine with one primary and two secondary amines (TRI) as well as different impregnated polyamines such as branched and linear polyethylenimine (BPEI and LPEI) and polyallylamine (PALL) was investigated using extensive CO(2) adsorption-desorption cycling as well as diffuse reflectance infrared Fourier transform (DRIFT) and (13)C CP MAS NMR measurements. Except for sMono, all other supported amines underwent significant deactivation in the presence of dry CO(2) under mild conditions. In all cases, the decrease in CO(2) uptake was associated with the formation of urea linkages at the expense of amine groups. The urea-containing species were identified, and the deactivation pathways were delineated.

中文翻译:

含胺吸附剂的 CO2 诱导降解:反应产物和途径

进行了一项综合研究,以研究干燥条件下二氧化碳存在下各种介孔二氧化硅负载的含胺吸附剂的稳定性。CO(2) 诱导的接枝伯胺和仲单胺(pMono、sMono)、具有一种伯胺和一种仲胺的二胺 (Diamine) 和具有一种伯胺和两种仲胺 (TRI) 的三胺以及不同的浸渍多胺的降解,例如使用广泛的 CO(2) 吸附-解吸循环以及漫反射红外傅里叶变换 (DRIFT) 和 (13) C CP MAS NMR 测量对支链和线性聚乙烯亚胺 (BPEI 和 LPEI) 和聚烯丙胺 (PALL) 进行了调查。除了 sMono,所有其他受支持的胺在温和条件下干 CO(2) 的存在下经历了显着的失活。在所有情况下,CO(2) 吸收的减少与以胺基团为代价的尿素键的形成有关。确定了含尿素的物质,并描绘了失活途径。
更新日期:2012-08-09
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