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用于高效捕获 CO 及 CO/ N 吸附选择性的先进 Ad-UiO-66@NGO 复合材料的合成与表征

Synthesis and characterization of advanced Ad-UiO-66@NGO composite for efficient CO capture and CO/N adsorption selectivity.

作者信息

Azizi Keywan, Shahhosseini Shahrokh, Esfahani Heidar Javdani

机构信息

School of Chemical, Petroleum and Gas Engineering, Iran University of Science and Technology, Tehran, Iran.

School of Chemical, Petroleum and Gas Engineering, Iran University of Science and Technology, Tehran, Iran.

出版信息

Environ Res. 2025 Mar 1;268:120819. doi: 10.1016/j.envres.2025.120819. Epub 2025 Jan 10.

Abstract

Highly effective adsorbents, with their impressive adsorption capacity and outstanding selectivity, play a pivotal role in technologies such as carbon capture and utilization in industrial flue gas applications, leading to significant reductions in greenhouse gas emissions. This study aims to synthesize advanced composites via solvothermal methods, incorporating a defective Zirconium-based MOF and amine-functionalized graphene oxide. The main objective is to enhance the CO adsorption capacity of the composite and improve its CO/N separation selectivity. The samples were characterized using XRD, FT-IR, TGA, FE-SEM, and nitrogen adsorption and desorption analysis. The composites' gas uptake capacity toward pure CO and N adsorption were tested at various temperatures and pressure ranges of 1-9 bar. The resulting amino-defective UiO-66/NGO composite containing 15 wt% of amine-modified GO, displayed the highest CO uptake capacity of 15.13 mmol/g at 298 K and 9 bar, representing a remarkable 48% increase compared to the pristine MOF. Furthermore, isotherm and kinetic modeling showed a high level of agreement between the experimental data and the Freundlich and Elovich models, as indicated by their R values of 0.998 and 0.973, respectively. Moreover, the thermodynamic evaluation confirmed the exothermic and the spontaneity of the reaction. Furthermore, the adsorbent's CO/N selectivity was evaluated using the ideal adsorbed solution theory, revealing a remarkable selectivity value of 148. The regenerability evaluation through cyclic adsorption experiments showed that the optimized composite maintained CO adsorption reversibility at over 81.50% after 55 adsorption-desorption cycles.

摘要

高效吸附剂凭借其令人印象深刻的吸附容量和出色的选择性,在工业烟气应用中的碳捕获与利用等技术中发挥着关键作用,从而显著减少温室气体排放。本研究旨在通过溶剂热法合成先进复合材料,将有缺陷的锆基金属有机框架(MOF)与胺功能化氧化石墨烯结合。主要目标是提高复合材料对CO的吸附容量并改善其CO/N2分离选择性。使用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、热重分析(TGA)、场发射扫描电子显微镜(FE-SEM)以及氮气吸附和解吸分析对样品进行了表征。在1-9巴的不同温度和压力范围内测试了复合材料对纯CO和N2的气体吸附容量。所得含15 wt%胺改性GO的氨基缺陷UiO-66/NGO复合材料在298 K和9巴下显示出最高的CO吸附容量为15.13 mmol/g,与原始MOF相比显著增加了48%。此外,等温线和动力学模型表明实验数据与Freundlich和Elovich模型高度吻合,其R值分别为0.998和0.973。此外,热力学评估证实了反应的放热性和自发性。此外,使用理想吸附溶液理论评估了吸附剂的CO/N2选择性,显示出显著的选择性值为148。通过循环吸附实验进行的再生性评估表明,优化后的复合材料在55次吸附-解吸循环后保持了超过81.50%的CO吸附可逆性。

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