Organic-free, Ultrafast Synthesis of K-CHA Nano-aggregates with Various Morphologies and Their Adsorption Performances

doi:10.1007/s40242-024-4045-1

高等学校化学研究 ›› 2024, Vol. 40 ›› Issue (6): 1151-1159.doi: 10.1007/s40242-024-4045-1

Organic-free, Ultrafast Synthesis of K-CHA Nano-aggregates with Various Morphologies and Their Adsorption Performances

CHU Kailiang^1,2, WANG Yaquan^1,2, LIU Wenrong^1,2, BU Lingzhen^1,2, HUANG Yitong^1,2, GUO Niandong^1,2, QU Liping^1,2, SANG Juncai^1,2, LI Yaoning^1,2, SU Xuemei^1,2, ZHANG Xian^1,2

1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China;
2. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, P. R. China

收稿日期:2024-02-27 出版日期:2024-12-01 发布日期:2024-10-26
通讯作者: WANG Yaquan,yqwang@tju.edu.cn E-mail:yqwang@tju.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (No. 21276183).

Organic-free, Ultrafast Synthesis of K-CHA Nano-aggregates with Various Morphologies and Their Adsorption Performances

CHU Kailiang^1,2, WANG Yaquan^1,2, LIU Wenrong^1,2, BU Lingzhen^1,2, HUANG Yitong^1,2, GUO Niandong^1,2, QU Liping^1,2, SANG Juncai^1,2, LI Yaoning^1,2, SU Xuemei^1,2, ZHANG Xian^1,2

1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China;
2. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, P. R. China

Received:2024-02-27 Online:2024-12-01 Published:2024-10-26
Contact: WANG Yaquan,yqwang@tju.edu.cn E-mail:yqwang@tju.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (No. 21276183).

摘要/Abstract

摘要： K-Chabazite (K-CHA) zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective “one-pot” method. By solely employing colloidal silica and aluminum hydroxide in the K⁺/Sr²⁺ system without the assistance of seeds, fluorides or organic structure as directing agents, the K-CHA nano-aggregates were successfully synthesized in a few hours. The crystallization behavior of the gels with different SiO₂/Al₂O₃ molar ratios (SARs) was investigated using X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray fluorescence (XRF), ²⁷Al and ²⁹Si magic angle spinning nuclear magnetic resonance (MAS NMR), Fourier-transform infrared spectra (FTIR), UV-Raman characterizations. As the nucleation rates were changed with the SARs, three kinds of K-CHA nano-aggregates, namely, hamburger-, disk- and walnut-shaped, were obtained. A possible formation mechanism of the K-CHA nano-aggregates was proposed. Additionally, the walnut-shaped sample with an SAR of 7 possessed the largest pore volume and specific surface area, resulting in the highest methane adsorption capacity. Furthermore, it exhibited a CH₄/N₂ selectivity of more than 3 under relative pressures ranging from 0 to 0.6. This work offers guidance for modifying the stacking modes of other nano-sized zeolites.

关键词: Chabazite, Organic structure directing agent (OSDA)-free, Nano-aggregate, Methane, Adsorption separation

Abstract: K-Chabazite (K-CHA) zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective “one-pot” method. By solely employing colloidal silica and aluminum hydroxide in the K⁺/Sr²⁺ system without the assistance of seeds, fluorides or organic structure as directing agents, the K-CHA nano-aggregates were successfully synthesized in a few hours. The crystallization behavior of the gels with different SiO₂/Al₂O₃ molar ratios (SARs) was investigated using X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray fluorescence (XRF), ²⁷Al and ²⁹Si magic angle spinning nuclear magnetic resonance (MAS NMR), Fourier-transform infrared spectra (FTIR), UV-Raman characterizations. As the nucleation rates were changed with the SARs, three kinds of K-CHA nano-aggregates, namely, hamburger-, disk- and walnut-shaped, were obtained. A possible formation mechanism of the K-CHA nano-aggregates was proposed. Additionally, the walnut-shaped sample with an SAR of 7 possessed the largest pore volume and specific surface area, resulting in the highest methane adsorption capacity. Furthermore, it exhibited a CH₄/N₂ selectivity of more than 3 under relative pressures ranging from 0 to 0.6. This work offers guidance for modifying the stacking modes of other nano-sized zeolites.

Key words: Chabazite, Organic structure directing agent (OSDA)-free, Nano-aggregate, Methane, Adsorption separation

CHU Kailiang, WANG Yaquan, LIU Wenrong, BU Lingzhen, HUANG Yitong, GUO Niandong, QU Liping, SANG Juncai, LI Yaoning, SU Xuemei, ZHANG Xian. Organic-free, Ultrafast Synthesis of K-CHA Nano-aggregates with Various Morphologies and Their Adsorption Performances[J]. 高等学校化学研究, 2024, 40(6): 1151-1159.

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Organic-free, Ultrafast Synthesis of K-CHA Nano-aggregates with Various Morphologies and Their Adsorption Performances

Organic-free, Ultrafast Synthesis of K-CHA Nano-aggregates with Various Morphologies and Their Adsorption Performances

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