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The adsorption kinetics of CO2 on copper hexacyanoferrate studied by thermogravimetric analysis
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0001-9304-8975
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0003-0598-4769
(English)Manuscript (preprint) (Other academic)
Abstract [en]

The CO2 adsorption and CO2 adsorption kinetics were evaluated by thermogravimetry on two Prussian blue analogues, K2x/3CuII[FeIIx FeIII1-x(CN)6]2/3, with nominally K-free x = 0.0 and K-rich x = 1.0. Differential isosteric heats of adsorption were determined from adsorption isotherms using the Clausius-Clapeyron equation and integral values by differential scanning calorimetry. The average differential heats of CO2 adsorption are 28 kJ/mol for x = 0.0 and 33 kJ/mol for x = 1.0.  Both compositions show small maxima in differential heat at ~1 mmol/g.  The integral adsorption heats were determined to be 26 kJ/mol for both x = 0.0 and x = 1.0. The kinetic CO2 adsorption/desorption curves can be modeled by a double exponential function describing two parallel processes with different rate constants. The activation energies for CO2 adsorption on x = 0.0 were 6(1) kJ/mol for the faster component and 16(1) kJ/mol for the slower one, while the corresponding values for x = 1.0 were 9(1) kJ/mol and 7(1) kJ/mol, respectively. The maximum CO2 uptake for both compositions was found to be ~4.5 mmol/g, 19.8 wt %, at 1 bar and 273 K. The materials exhibited fast adsorption kinetics and stable cyclic performance at room temperature. The kinetics were slower for the samples with x = 1.0 than for x = 0.0 which may be attributed to interactions between CO2 molecules and K+ ions.   

National Category
Chemical Sciences
Research subject
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:su:diva-146259OAI: oai:DiVA.org:su-146259DiVA: diva2:1136518
Available from: 2017-08-28 Created: 2017-08-28 Last updated: 2017-08-29Bibliographically approved
In thesis
1. Prussian blue analogue copper hexacyanoferrate: Synthesis, structure characterization and its applications as battery electrode and CO2 adsorbent
Open this publication in new window or tab >>Prussian blue analogue copper hexacyanoferrate: Synthesis, structure characterization and its applications as battery electrode and CO2 adsorbent
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Prussian blue (PB) and Prussian blue analogues (PBAs) are compounds with potential applications in a large variety of fields such as gas storage, poison antidotes, electrochromism, electrochemistry and molecular magnets. The compounds are easy to synthesize, cheap, environmentally friendly and have been pursued for both fundamental research and industrial purposes. Despite the multifunctionality of PB and PBAs, they have complicated compositions, which are largely dependent on the synthesis methods and storage conditions. Thus, performing investigations on such compounds with defined composition, stoichiometry and crystal structure is essential.

This thesis has focused on synthesis and detailed structure characterization of copper hexacyanoferrate (CuHCF) via X-ray powder diffraction (XRPD), neutron powder diffraction (NPD), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), inductively coupled plasma-optical emission spectroscopy (ICP-OES), scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS), Mössbauer spectroscopy, extended X-ray absorption fine structure (EXAFS), infrared (IR) and Raman techniques. In addition, kinetics of thermal dehydration process, CO2 adsorption and CO2 adsorption kinetics were investigated. Moreover, in operando synchrotron X-ray diffraction experiments were performed to gain insight into the structure-electrochemistry relationships in an aqueous CuHCF/Zn battery during operation.

Place, publisher, year, edition, pages
Stockholm: Materials and Environmental Chemistry, Stockholm University, 2017
Keyword
copper hexacyanoferrate, synthesis, structure refinement, thermal dehydration, CO2 adsorption, kinetic analysis, in operando synchrotron X-ray diffraction
National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
urn:nbn:se:su:diva-146335 (URN)978-91-7649-940-5 (ISBN)978-91-7649-941-2 (ISBN)
Public defence
2017-10-13, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius Väg 16 B, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Swedish Research Council, 2011:6512
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 4: Manuscript. Paper 5: Manuscript.

Available from: 2017-09-18 Created: 2017-08-29 Last updated: 2017-09-14Bibliographically approved

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