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Research Article

Enhanced carbon capture with motif-rich amino acid loaded defective robust metal-organic frameworks

Qi-Ye Ju1,3,4, Jia-Jia Zheng 2, Li Xu1,3,4, Hai-Yan Jiang1,5, Zi-Qian Xue6, Lu Bai1,5, Yang-Yang Guo1,5( ), Ming-Shui Yao1,5( ), Ting-Yu Zhu1,5( )
State Key Laboratory of Multi-phase Complex Systems, CAS Key Laboratory of Green Process and Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
Laboratory of Theoretical and Computational Nanoscience, National Center for Nanoscience and Technology, Chinese Academy of Sciences, Beijing 100190, China
School of Rare Earths, University of Science and Technology of China, Hefei 230026, China
Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China
University of Chinese Academy of Sciences, Chinese Academy of Sciences, Beijing 100049, China
Institute for Integrated Cell-Material Sciences, Kyoto University, Institute for Advanced Study, Kyoto University, Yoshida, Ushinomiya-cho, Sakyo-ku, Kyoto 606-8501, Japan
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Graphical Abstract

We demonstrate a channel broadening facilitated loading of functional motif-rich amino acids (AAs) into the defective and robust porous frameworks via the combined defect-engineering and post-synthetic methods. The resulting abundant active sites in a confined nano space endow it with good carbon dioxide (CO2) adsorption capacity and selectivity of CO2/N2.

Abstract

The use of metal-organic frameworks (MOFs) as solid adsorption materials for carbon capture is promising, but achieving efficient and reversible adsorption with a balance of capacity and selectivity for carbon dioxide (CO2) over N2 remains a challenge. To take full advantage of the strong channel traffic and robustness of MOFs with relatively small pores, it is highly necessary to employ a defect-engineering strategy to construct a broader channel structure that can facilitate the loading of functional motif-rich amino acids (AAs). This strategy can greatly enhance the CO2 adsorption performance of MOF. In this study, motif-rich amino acids are loaded into the defective and robust porous frameworks via combined defect-engineering and post-synthetic methods. The defective Zr/Hf-MOF-808s modified with AAs, especially for the 18 mol% 4-nitroisophthalic acid, generated defective products allowing for the loading of L-serine (L-Ser). This modification resulted in a significant improvement in both the adsorption capacity (248% improvement at 298 K, 100 kPa) and the selectivity of CO2/N2 using the ideal adsorbed solution theory (IAST), with the selectivity increasing to 120.55 and 38.27 at 15 and 100 kPa, respectively, while maintaining good cycling performance. Density functional theory (DFT) simulation, CO2 temperature-programmed desorption (CO2-TPD), and in situ Fourier transform infrared spectroscopy (FTIR) were further employed to have a better understanding of the enhanced CO2 adsorption capacity. Interestingly, unlike the AAs loaded pristine MOF-808s that showed the best CO2 adsorption capacity with the loading of short and small glycine (Gly), the broadened channel size in our work enables the loading of functional motif-rich L-serine, which brings more active binding sites, improving CO2 adsorption.

Keywords

carbon capture and storagemetal-organic framework (MOF)amino acids (AAs)defect-engineeringmotif-rich

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Nano Research
Volume 17 Issue 3,
March 2024
Pages 2004-2010
DOI: 10.1007/s12274-023-5961-y
Cite this article:
Ju Q-Y, J-J-Z, Xu L, et al. Enhanced carbon capture with motif-rich amino acid loaded defective robust metal-organic frameworks. Nano Research, 2024, 17(3): 2004-2010. https://doi.org/10.1007/s12274-023-5961-y
Topics:
Microporosity Porous materialsStructural design

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Received: 03 May 2023
Revised: 22 June 2023
Accepted: 26 June 2023
Published: 10 August 2023
© Tsinghua University Press 2023
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