Short Gabriel N, Burentugs Enerelt, Proaño Laura, Moon Hyun June, Rim Guanhe, Nezam Iman, Korde Akshay, Nair Sankar, Jones Christopher W
School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States.
JACS Au. 2023 Jan 4;3(1):62-69. doi: 10.1021/jacsau.2c00553. eCollection 2023 Jan 23.
Previous research has demonstrated that amine polymers rich in primary and secondary amines supported on mesoporous substrates are effective, selective sorbent materials for removal of CO from simulated flue gas and air. Common substrates used include mesoporous alumina and silica (such as SBA-15 and MCM-41). Conventional microporous materials are generally less effective, since the pores are too small to support low volatility amines. Here, we deploy our newly discovered zeolite nanotubes, a first-of-their-kind quasi-1D hierarchical zeolite, as a substrate for poly(ethylenimine) (PEI) for CO capture from dilute feeds. PEI is impregnated into the zeolite at specific organic loadings. Thermogravimetric analysis and porosity measurements are obtained to determine organic loading, pore filling, and surface area of the supported PEI prior to CO capture studies. MCM-41 with comparable pore size and surface area is also impregnated with PEI to provide a benchmark material that allows for insight into the role of the zeolite nanotube intrawall micropores on CO uptake rates and capacities. Over a range of PEI loadings, from 20 to 70 w/w%, the zeolite allows for increased CO capture capacity over the mesoporous silica by ∼25%. Additionally, uptake kinetics for nanotube-supported PEI are roughly 4 times faster than that of a comparable PEI impregnated in SBA-15. It is anticipated that this new zeolite will offer numerous opportunities for engineering additional advantaged reaction and separation processes.
先前的研究表明,负载在介孔载体上的富含伯胺和仲胺的胺聚合物是从模拟烟道气和空气中去除一氧化碳的有效、选择性吸附材料。常用的载体包括介孔氧化铝和二氧化硅(如SBA-15和MCM-41)。传统的微孔材料通常效果较差,因为其孔径太小,无法负载低挥发性胺。在此,我们将新发现的沸石纳米管(一种首创的准一维分级沸石)用作聚(乙烯亚胺)(PEI)的载体,用于从稀进料中捕获一氧化碳。将PEI以特定的有机负载量浸渍到沸石中。在进行一氧化碳捕获研究之前,通过热重分析和孔隙率测量来确定负载PEI的有机负载量、孔填充情况和表面积。还将具有可比孔径和表面积的MCM-41用PEI浸渍,以提供一种基准材料,从而深入了解沸石纳米管内壁微孔对一氧化碳吸收速率和容量的作用。在20至70 w/w%的一系列PEI负载量范围内,与介孔二氧化硅相比,沸石的一氧化碳捕获容量提高了约25%。此外,纳米管负载PEI的吸收动力学比浸渍在SBA-15中的可比PEI快约4倍。预计这种新型沸石将为设计更多具有优势的反应和分离过程提供众多机会。