Enhancing CO2 adsorption performance of cold oxygen plasma-treated almond shell-derived activated carbons through ionic liquid incorporation

IF 7.2 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of CO2 Utilization Pub Date : 2024-09-11 DOI:10.1016/j.jcou.2024.102927
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Abstract

To enhance the CO2 adsorption of almond shell-derived activated carbon (AC) samples treated with cold oxygen plasma, the samples were impregnated with cholinium-amino acid ionic liquids ([Cho][AA] ILs) using the vacuum-assisted impregnation method. The physicochemical and textural properties of the resulting composites (ILs@AC) were characterized using various techniques, including Fourier-transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), scanning electron microscopy (SEM) coupled with energy-dispersive X-ray (EDX) spectroscopy, and Brunauer-Emmett-Teller (BET) surface area measurement. The CO2 adsorption performance of the samples was evaluated using a quartz crystal microbalance (QCM) over a temperature range of 288.15–308.15 K and gas pressures up to 1 bar. The IL@AC composite materials exhibited notably improved CO2 adsorption capacities compared to pristine AC. The CO2 adsorption isotherms onto the IL@AC composite samples closely conformed to the Langmuir isotherm model, indicating the dominant involvement of strong intermolecular interactions, particularly driven by amine functionalities. Meanwhile, the results revealed that [Cho][His]@AC showed lowered CO2 adsorption capacity compared to [Cho][Pro]@AC and [Cho][Gln]@AC. Among the studied ionic liquids, [Cho][Pro]@AC showed the highest absorption capacity (2.332 mmol·g−1 at 288 K and 1 bar). This was due to the obstruction of internal pores within the AC structure caused by excessive amine incorporation into its porous framework. In the meantime, for a deeper insight into the impregnation process of ILs onto the AC surfaces and their potential interactions with CO2 molecules, we conducted density-functional theory (DFT) calculations using the ωB97XD/6-31 + G(d,p) method. The calculated interaction energies, ranging from − 1.19 to − 1.44 eV, along with calculated quantum chemical descriptors, indicated a notable stabilization of IL species on the AC surfaces, with high affinity toward CO2 molecules.

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通过加入离子液体提高经冷氧等离子体处理的杏仁壳活性炭的二氧化碳吸附性能
为了提高经冷氧等离子体处理的杏仁壳活性炭(AC)样品对二氧化碳的吸附能力,采用真空辅助浸渍法对样品进行了胆碱-氨基酸离子液体([Cho][AA] ILs)浸渍。利用傅立叶变换红外光谱(FTIR)、热重分析(TGA)、扫描电子显微镜(SEM)和能量色散 X 射线(EDX)光谱以及布鲁纳-埃美特-泰勒(BET)比表面积测量等多种技术对所制备复合材料(ILs@AC)的物理化学和质构特性进行了表征。使用石英晶体微天平(QCM)在 288.15-308.15 K 的温度范围和高达 1 bar 的气体压力下评估了样品的二氧化碳吸附性能。与原始 AC 相比,IL@AC 复合材料的二氧化碳吸附能力明显提高。IL@AC复合材料样品上的二氧化碳吸附等温线与Langmuir等温线模型非常吻合,这表明强分子间相互作用,特别是胺官能团的驱动在其中起了主导作用。同时,研究结果表明,与[Cho][Pro]@AC和[Cho][Gln]@AC相比,[Cho][His]@AC对二氧化碳的吸附能力较低。在所研究的离子液体中,[Cho][Pro]@AC 的吸收能力最高(288 K 和 1 bar 条件下为 2.332 mmol-g-1)。这是因为 AC 结构的多孔框架中加入了过量的胺,导致内部孔隙受阻。同时,为了更深入地了解 IL 在 AC 表面的浸渍过程及其与 CO2 分子的潜在相互作用,我们采用 ωB97XD/6-31 + G(d,p) 方法进行了密度泛函理论(DFT)计算。计算得出的相互作用能在 - 1.19 至 - 1.44 eV 之间,量子化学描述符的计算结果也表明,IL 物种在 AC 表面上具有显著的稳定性,对 CO2 分子具有很高的亲和力。
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
Journal of CO2 Utilization
Journal of CO2 Utilization CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.90
自引率
10.40%
发文量
406
审稿时长
2.8 months
期刊介绍: The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials. The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications. The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.
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