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用于二氧化碳捕集的ZSM-5沸石吸附剂的改性

Modification of the Zeolite ZSM‑5 Adsorbent for CO Capture.

作者信息

Al-Mamoori Ahmed, Saed Usama A, Saoud Ammar A, Abdul Jabbar Marwa F, Jasim Ahmed, Majdi Hasan Sh, Hanif Aamir, Iacomi Paul

机构信息

Department of Chemical Engineering, College of Engineering, Al-Nahrain University, Jadriya, Baghdad 10072, Iraq.

Linda and Bipin Doshi Department of Chemical and Biochemical Engineering, Missouri University of Science and Technology, 1101 N. State Street, Rolla, Missouri 65409, United States.

出版信息

ACS Omega. 2025 May 16;10(20):20129-20141. doi: 10.1021/acsomega.4c09747. eCollection 2025 May 27.

Abstract

The rise in greenhouse gas emissions has significantly raised the average global temperature, intensifying the global warming crisis. Addressing this challenge requires substantial efforts from both academia and industry to deliver impactful mitigation solutions. Thus, the development of efficient materials and processes for mitigating greenhouse gases, particularly carbon dioxide (CO), is of great interest. In this study, various zeolite adsorbents were synthesized, including pristine NH-ZSM-5, the calcined form H-ZSM-5, and its cation-exchanged variants (Ba-ZSM-5, Mn-ZSM-5, Ni-ZSM-5, and Zn-ZSM-5), and their effectiveness in CO capture was tested at different temperatures. All of the adsorbent materials demonstrated decent CO capacity, with NH-ZSM-5 achieving the highest capacity of 1.45 mmol/g at 25 °C and 1 atm under pure CO tests. Although the cation-exchange process slightly reduces the CO capture capacity under dry conditions, it enhanced the CO capacity under humid conditions as compared to the pristine NH-ZSM-5 material and also improved CO/N selectivity by limiting N uptake. The capacity for CO adsorption declined with increasing temperature, indicating a physisorption-driven interaction mechanism. Additionally, the materials exhibited rapid adsorption kinetics best described by a pseudo-first-order kinetic model. The adsorbents also showed stable capacity over five adsorption-desorption cycles, indicative of the robustness of the material. Furthermore, unary CO and HO adsorption isotherms, coadsorption uptake of CO in the presence of humidity, and CO breakthrough experiments under humid conditions relevant to postcombustion CO capture scenario were also carried out. X-ray diffraction, Brunauer-Emmett-Teller (BET) surface area analysis, and scanning electron microscopy-energy dispersive X-ray spectroscopy techniques were employed to examine the physicochemical characteristics of the materials. Thus, the development of an efficient CO adsorbent with high uptake, rapid kinetics, high selectivity, and excellent thermal stability applying the realistic condition is of paramount importance for future CO capture applications.

摘要

温室气体排放的增加显著提高了全球平均温度,加剧了全球变暖危机。应对这一挑战需要学术界和工业界做出巨大努力,以提供有效的缓解解决方案。因此,开发用于减少温室气体,特别是二氧化碳(CO)的高效材料和工艺备受关注。在本研究中,合成了各种沸石吸附剂,包括原始的NH-ZSM-5、煅烧形式的H-ZSM-5及其阳离子交换变体(Ba-ZSM-5、Mn-ZSM-5、Ni-ZSM-5和Zn-ZSM-5),并在不同温度下测试了它们对CO的捕集效果。所有吸附剂材料都表现出良好的CO吸附容量,在纯CO测试中,NH-ZSM-5在25°C和1个大气压下实现了最高吸附容量1.45 mmol/g。虽然阳离子交换过程在干燥条件下会略微降低CO捕集容量,但与原始的NH-ZSM-5材料相比,在潮湿条件下提高了CO吸附容量,并且通过限制N的吸附提高了CO/N选择性。CO吸附容量随温度升高而下降,表明是物理吸附驱动的相互作用机制。此外,材料表现出快速的吸附动力学,用准一级动力学模型能最好地描述。吸附剂在五个吸附-解吸循环中也表现出稳定的容量,表明材料的稳定性。此外,还进行了单一CO和H₂O吸附等温线、湿度存在下CO的共吸附吸收以及与燃烧后CO捕集场景相关的潮湿条件下的CO穿透实验。采用X射线衍射、布鲁诺尔-埃米特-泰勒(BET)表面积分析和扫描电子显微镜-能量色散X射线光谱技术来研究材料的物理化学特性。因此,开发一种在实际条件下具有高吸附量、快速动力学、高选择性和优异热稳定性的高效CO吸附剂对于未来的CO捕集应用至关重要。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1eee/12120639/6a3ccaa4cd33/ao4c09747_0001.jpg

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