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Article Dans Une Revue Nature Communications Année : 2023

Solvent-derived defects suppress adsorption in MOF-74

Résumé

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 13 C 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 N 2 and CO 2 adsorption with respect to the defect concentration. In-situ NMR analysis and molecular simulations of CO 2 dynamics elaborate the adsorption mechanisms in defective MOF-74. Our study establishes comprehensive strategies to search, elucidate and manipulate defects in MOFs.

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Chimie

Dates et versions

hal-04500729 , version 1 (12-03-2024)

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Citer

Yao Fu, Yifeng Yao, Alexander Forse, Jianhua Li, Kenji Mochizuki, et al.. Solvent-derived defects suppress adsorption in MOF-74. Nature Communications, 2023, 14 (1), pp.2386. ⟨10.1038/s41467-023-38155-8⟩. ⟨hal-04500729⟩
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