Controlling Architecture and Composition of Nanostructured, Multicomponent Materials for Applications in Sorption, Energy Storage, and Sensing

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Controlling Architecture and Composition of Nanostructured, Multicomponent Materials for Applications in Sorption, Energy Storage, and Sensing

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2022-08

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In this dissertation, synthetic methods for the preparation of materials containing multiple components with different properties were developed. Nanostructured multicomponent materials were synthesized with controlled architecture and composition to achieve desirable properties for applications in adsorption, charge storage, and ion sensing.In Chapter 2, our goal was to develop a dye adsorptive material with nanostructured properties for higher capacity and easy handling. To achieve our goal, a three-dimensionally ordered macroporous (3DOM) structure was applied to an adsorptive material, ZIF-8, because the 3DOM structure can provide nanosized features along with bulk properties that allow for easy handling. An adsorptive ZIF-8 layer was grown on 3DOM ZnO-CeO2-Al2O3 via a vapor-phase pseudomorphic transformation. The developed 3DOM multicomponent adsorbent improved the adsorption capacity from 20 mg/g (unsupported ZIF-8 particles) to 47 mg/g and could be recycled after use. In Chapter 3, multicomponent charge storage materials were studied for application in lithium-ion batteries. The irreversible lithium loss during the first cycle reduces the battery capacity for the rest of its operating life. Li8ZrO6 was utilized as a pre-lithiation additive to compensate for the lithium loss in combination with the cathode material LiNi0.5Mn1.5O4 and assembled in coin cells with graphite as an anode. A loading of 5 wt % LZO in the multicomponent material released 5 Li+ per Li8ZrO6 and resulted in up to 18% improved reversible capacity and up to 30% improved capacity retention, compared to pristine LiNi0.5Mn1.5O4. Chapter 4 addresses the development of a nanostructured multicomponent material used for ion sensing. A method of functionalizing carbon surfaces with a Co(II/III) redox buffer as a solid contact was developed with the goal to ultimately prepare calibration-free solid-contact ion-selective electrode. The Co(II/III) redox buffer was covalently attached to the carbon substrate by grafting a terpyridine ligand (Tpy-ph), followed by attaching Co2+ ions and an additional Tpy ligand. The preliminary electrochemical characterization of this solid contact showed an improved E˚ reproducibility with 8.8 mV electrode-to-electrode potential variation (or 1.5 mV for the best three electrodes), compared to electrodes without any solid contact (21.4 mV) or electrodes without the Co(II/III) redox buffer (13.9 mV).

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University of Minnesota Ph.D. dissertation. August 2022. Major: Chemistry. Advisor: Andreas Stein. 1 computer file (PDF); xxix, 185 pages.

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Kim, Minog. (2022). Controlling Architecture and Composition of Nanostructured, Multicomponent Materials for Applications in Sorption, Energy Storage, and Sensing. Retrieved from the University Digital Conservancy, https://hdl.handle.net/11299/259743.

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