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Solvent-derived defects suppress adsorption in MOF-74

Author

Listed:
  • Yao Fu

    (Zhejiang University
    Zhejiang University
    Univ. Grenoble Alpes, CEA, IRIG-MEM
    University of California)

  • Yifeng Yao

    (Zhejiang University)

  • Alexander C. Forse

    (University of California
    University of Cambridge
    University of California)

  • Jianhua Li

    (Zhejiang University)

  • Kenji Mochizuki

    (Zhejiang University)

  • Jeffrey R. Long

    (University of California
    University of California
    Lawrence Berkeley National Laboratory)

  • Jeffrey A. Reimer

    (University of California)

  • Gaël Paëpe

    (Univ. Grenoble Alpes, CEA, IRIG-MEM)

  • Xueqian Kong

    (Zhejiang University
    Zhejiang University
    Shanghai Jiao Tong University)

Abstract

Defects in metal-organic frameworks (MOFs) have great impact on their nano-scale structure and physiochemical properties. However, isolated defects are easily concealed when the frameworks are interrogated by typical characterization methods. In this work, we unveil the presence of solvent-derived formate defects in MOF-74, an important class of MOFs with open metal sites. With multi-dimensional solid-state nuclear magnetic resonance (NMR) investigations, we uncover the ligand substitution role of formate and its chemical origin from decomposed N,N-dimethylformamide (DMF) solvent. The placement and coordination structure of formate defects are determined by 13C NMR and density functional theory (DFT) calculations. The extra metal-oxygen bonds with formates partially eliminate open metal sites and lead to a quantitative decrease of N2 and CO2 adsorption with respect to the defect concentration. In-situ NMR analysis and molecular simulations of CO2 dynamics elaborate the adsorption mechanisms in defective MOF-74. Our study establishes comprehensive strategies to search, elucidate and manipulate defects in MOFs.

Suggested Citation

  • Yao Fu & Yifeng Yao & Alexander C. Forse & Jianhua Li & Kenji Mochizuki & Jeffrey R. Long & Jeffrey A. Reimer & Gaël Paëpe & Xueqian Kong, 2023. "Solvent-derived defects suppress adsorption in MOF-74," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38155-8
    DOI: 10.1038/s41467-023-38155-8
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    References listed on IDEAS

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    1. Thomas M. McDonald & Jarad A. Mason & Xueqian Kong & Eric D. Bloch & David Gygi & Alessandro Dani & Valentina Crocellà & Filippo Giordanino & Samuel O. Odoh & Walter S. Drisdell & Bess Vlaisavljevich , 2015. "Cooperative insertion of CO2 in diamine-appended metal-organic frameworks," Nature, Nature, vol. 519(7543), pages 303-308, March.
    2. Xinchen Kang & Kai Lyu & Lili Li & Jiangnan Li & Louis Kimberley & Bin Wang & Lifei Liu & Yongqiang Cheng & Mark D. Frogley & Svemir Rudić & Anibal J. Ramirez-Cuesta & Robert A. W. Dryfe & Buxing Han , 2019. "Integration of mesopores and crystal defects in metal-organic frameworks via templated electrosynthesis," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    3. Wenlong Xu & Yuwei Zhang & Junjun Wang & Yixiu Xu & Li Bian & Qiang Ju & Yuemin Wang & Zhenlan Fang, 2022. "Defects engineering simultaneously enhances activity and recyclability of MOFs in selective hydrogenation of biomass," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    4. Zhenfeng Pang & Jun Zhang & Weicheng Cao & Xueqian Kong & Xiaogang Peng, 2019. "Partitioning surface ligands on nanocrystals for maximal solubility," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    5. Matthew J. Cliffe & Wei Wan & Xiaodong Zou & Philip A. Chater & Annette K. Kleppe & Matthew G. Tucker & Heribert Wilhelm & Nicholas P. Funnell & François-Xavier Coudert & Andrew L Goodwin, 2014. "Correlated defect nanoregions in a metal–organic framework," Nature Communications, Nature, vol. 5(1), pages 1-8, September.
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