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Analysis by synchrotron X-ray scattering of the kinetics of formation of an Fe-based metal-organic framework with high CO2 adsorption

DOI: 10.1063/1.5121644 DOI Help

Authors: Harry G. W. Godfrey (University of Manchester) , Lydia Briggs (University of Manchester) , Xue Han (University of Manchester) , William J. F. Trenholme (University of Manchester) , Christopher Morris (University of Manchester) , Mathew Savage (University of Manchester) , Louis Kimberley (University of Manchester) , Oxana Magdysyuk (Diamond Light Source) , Michael Drakopoulos (Diamond Light Source) , Claire A. Murray (Diamond Light Source) , Chiu C. Tang (Diamond Light Source) , Mark D. Frogley (Diamond Light Source) , Gianfelice Cinque (Diamond Light Source) , Sihai Yang (University of Manchester) , Martin Schroeder (University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Apl Materials , VOL 7

State: Published (Approved)
Published: November 2019
Diamond Proposal Number(s): 11278

Open Access Open Access

Abstract: Understanding the mechanism of assembly and function of metal-organic frameworks (MOFs) is important for the development of practical materials. Herein, we report a time-resolved diffraction analysis of the kinetics of formation of a robust MOF, MFM-300(Fe), which shows high adsorption capacity for CO2 (9.55 mmol g−1 at 293 K and 20 bar). Applying the Avrami-Erofe’ev and the two-step kinetic Finke-Watzky models to in situ high-energy synchrotron X-ray powder diffraction data obtained during the synthesis of MFM-300(Fe) enables determination of the overall activation energy of formation (50.9 kJ mol−1), the average energy of nucleation (56.7 kJ mol−1), and the average energy of autocatalytic growth (50.7 kJ mol−1). The synthesis of MFM-300(Fe) has been scaled up 1000-fold, enabling the successful breakthrough separations of the CO2/N2 mixture in a packed-bed with a selectivity for CO2/N2 of 21.6. This study gives an overall understanding for the intrinsic behaviors of this MOF system, and we have determined directly the binding domains and dynamics for adsorbed CO2 molecules within the pores of MFM-300(Fe).

Journal Keywords: Synchrotrons; Light scattering; Microspectroscopy; Image processing; X-ray diffraction; Arrhenius plot; Powder diffraction; Crystalline solids

Diamond Keywords: Carbon Capture and Storage (CCS); Gas Separation

Subject Areas: Materials, Chemistry, Environment

Instruments: B22-Multimode InfraRed imaging And Microspectroscopy , I11-High Resolution Powder Diffraction , I12-JEEP: Joint Engineering, Environmental and Processing

Added On: 08/11/2019 09:50


Discipline Tags:

Earth Sciences & Environment Climate Change Chemistry Materials Science Metal-Organic Frameworks Metallurgy Organometallic Chemistry

Technical Tags:

Diffraction Scattering Spectroscopy Energy Dispersive Diffraction (EDD) X-ray Powder Diffraction Wide Angle X-ray Scattering (WAXS) X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)