Investigating the Effect of Trace Levels of Manganese Ions During Solvothermal Synthesis of Massey University Framework-16 on CO 2 Uptake Capacity.

Autor: Sarswat A; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0100, United States., Bacsa J; Crystallography Lab, Emory University, Atlanta, Georgia 30322, United States., Roy A; School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332-0100, United States., Marreiros J; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0100, United States., Finn MG; School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332-0100, United States., Sholl DS; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0100, United States.; Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States., Lively RP; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0100, United States.
Jazyk: angličtina
Zdroj: Chemistry of materials : a publication of the American Chemical Society [Chem Mater] 2024 May 17; Vol. 36 (11), pp. 5378-5387. Date of Electronic Publication: 2024 May 17 (Print Publication: 2024).
DOI: 10.1021/acs.chemmater.4c00137
Abstrakt: The effects of impurities on reaction precursors for metal-organic framework (MOF) synthesis have not been studied in extensive detail. The impact of these impurities can be an important factor while considering scale-up of these materials. In this work, we study the apparently positive impact of the presence of manganese ions for the synthesis of a Co-based MOF, Massey University Framework-16 (MUF-16). The presence of a trace amount of manganese in the reaction mixture led to consistently high CO 2 uptake across multiple batches. Characterization including X-ray diffraction, scanning electron microscopy, Fourier transform infrared-attenuated total reflectance, ultraviolet-visible spectroscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy, and extended X-ray absorption fine structure spectroscopy led us to hypothesize that the differences in CO 2 adsorption among materials with differing synthesis routes arise from variations in the local environment around the cobalt metal center. Aided by density functional theory calculations, we speculate that manganese ions get inserted into the structure during crystallization and act as catalysts for ligand substitution, improving the possibility for octahedral coordination of cobalt with the ligand, thus leading to Co-based pristine structures with higher CO 2 uptakes.
Competing Interests: The authors declare no competing financial interest.
(© 2024 The Authors. Published by American Chemical Society.)
Databáze: MEDLINE
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