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Surface Chemistry Control of 2D Nanomaterial Morphologies, Optoelecronic Responses, and Physicochemical Properties.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Surface Chemistry Control of 2D Nanomaterial Morphologies, Optoelecronic Responses, and Physicochemical Properties./
作者:	Lee, Jacob Thomas.
面頁冊數:	1 online resource (155 pages)
附註:	Source: Dissertations Abstracts International, Volume: 85-01, Section: B.
Contained By:	Dissertations Abstracts International85-01B.
標題:	Mechanical properties. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30506020click for full text (PQDT)
ISBN:	9798379844622

Surface Chemistry Control of 2D Nanomaterial Morphologies, Optoelecronic Responses, and Physicochemical Properties.
Lee, Jacob Thomas.

Surface Chemistry Control of 2D Nanomaterial Morphologies, Optoelecronic Responses, and Physicochemical Properties. - 1 online resource (155 pages)

Source: Dissertations Abstracts International, Volume: 85-01, Section: B.

Thesis (Ph.D.)--Purdue University, 2022.

Includes bibliographical references

The field of two-dimensional (2D) nanomaterials first began in earnest with the discovery of graphene in 2004 due to their unique shape-dependent optical, electronic, and mechanical properties. These properties arise due to their one-dimensional confinement and are further influenced by the elemental composition of the inorganic crystal lattice. There has been an intense focus on developing new compositions of 2D nanomaterials to take advantage of their intrinsic beneficial properties in a variety of applications including catalysis, energy storage and harvesting, sensing, and polymer nanocomposites. However, compared to the field of bulk materials, the influence of surface chemistry on 2D nanomaterials is still underdeveloped.2D nanomaterials are considered an "all-surface" atomic structure with heights of a single to few layers of atoms. The synthetic methods used to produce 2D materials include bottom-up colloidal methods and top-down exfoliation related techniques. Both cases result in poorly controlled surface chemistry with many undercoordinated surface atoms and/or undesirable molecules bound to the surface. Considering the importance surfaces play in most applications (i.e., catalysis and polymer processing) it is imperative to better understand how to manipulate the surface of 2D nanomaterials to unlock their full technological potential. Through a focus of the ligand-surface atom bonding in addition to the overall ligand structure we highlight the ability to direct morphological outcomes in lead free halide perovskites, maximize optoelectronic responses in substoichiometric tungsten oxide, and alter physicochemical properties titanium carbide MXenes.The careful control of precursor materials including poly(ethylene glycol) (PEG) surface ligands during the synthesis of bismuth halide perovskites resulted in the formation of 2D quasi-Ruddlesden-Popper phase nanomaterials. Through small angle X-ray scattering (SAXS) and in conjunction with X-ray photoelectron spectroscopy (XPS) we were able to conclude that an in-situ formation of an amino functional group on our PEG-amine ligand was inserted into the perovskite crystal lattice enabling 2D morphology formation. Additionally, through UV-vis absorption and ultraviolet photoelectron spectroscopies we were able to develop a complete electronic band structure of materials containing varying halides (i.e., Cl, Br, and I). Furthermore, through the increased solubility profile of the PEG ligands we observed solvent controlled assemblies of varying mesostructures.We developed an ex-situ ligand treatment to manipulate the localized surface plasmon resonance (LSPR) response of anion vacancy doped tungsten oxide (WO3-x) nanoplatelets (NPLs). Upon ligand treatment to alter the surface passivating ligand from carboxylic acid containing myristic acid (MA) to tetradecylphosphonic acid (TDPA) we observed a >100 nm blue shift in the LSPR response. Using Fourier transform infrared (FTIR) and Raman spectroscopies in conjunction with DFT calculated Raman spectra we were able to conclude this shift was due to the formation of tridentate phosphonate bonds on the NPLs surface. Phosphonate bonding allows for an increase in surface passivation per ligand decreasing surface trapped electrons. These previously trapped electrons were then able to participate as free electrons in the LSPR response. Electron paramagnetic spectroscopy (EPR) further supported this decrease in surface traps through a decrease and shift of the EPR signal related to metal oxide surface trapped electrons.

Electronic reproduction.
Ann Arbor, Mich. :
ProQuest,
2023

Mode of access: World Wide Web

ISBN: 9798379844622Subjects--Topical Terms:

3549505
Mechanical properties.
Index Terms--Genre/Form:

542853
Electronic books.

Surface Chemistry Control of 2D Nanomaterial Morphologies, Optoelecronic Responses, and Physicochemical Properties.
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520 $a The field of two-dimensional (2D) nanomaterials first began in earnest with the discovery of graphene in 2004 due to their unique shape-dependent optical, electronic, and mechanical properties. These properties arise due to their one-dimensional confinement and are further influenced by the elemental composition of the inorganic crystal lattice. There has been an intense focus on developing new compositions of 2D nanomaterials to take advantage of their intrinsic beneficial properties in a variety of applications including catalysis, energy storage and harvesting, sensing, and polymer nanocomposites. However, compared to the field of bulk materials, the influence of surface chemistry on 2D nanomaterials is still underdeveloped.2D nanomaterials are considered an "all-surface" atomic structure with heights of a single to few layers of atoms. The synthetic methods used to produce 2D materials include bottom-up colloidal methods and top-down exfoliation related techniques. Both cases result in poorly controlled surface chemistry with many undercoordinated surface atoms and/or undesirable molecules bound to the surface. Considering the importance surfaces play in most applications (i.e., catalysis and polymer processing) it is imperative to better understand how to manipulate the surface of 2D nanomaterials to unlock their full technological potential. Through a focus of the ligand-surface atom bonding in addition to the overall ligand structure we highlight the ability to direct morphological outcomes in lead free halide perovskites, maximize optoelectronic responses in substoichiometric tungsten oxide, and alter physicochemical properties titanium carbide MXenes.The careful control of precursor materials including poly(ethylene glycol) (PEG) surface ligands during the synthesis of bismuth halide perovskites resulted in the formation of 2D quasi-Ruddlesden-Popper phase nanomaterials. Through small angle X-ray scattering (SAXS) and in conjunction with X-ray photoelectron spectroscopy (XPS) we were able to conclude that an in-situ formation of an amino functional group on our PEG-amine ligand was inserted into the perovskite crystal lattice enabling 2D morphology formation. Additionally, through UV-vis absorption and ultraviolet photoelectron spectroscopies we were able to develop a complete electronic band structure of materials containing varying halides (i.e., Cl, Br, and I). Furthermore, through the increased solubility profile of the PEG ligands we observed solvent controlled assemblies of varying mesostructures.We developed an ex-situ ligand treatment to manipulate the localized surface plasmon resonance (LSPR) response of anion vacancy doped tungsten oxide (WO3-x) nanoplatelets (NPLs). Upon ligand treatment to alter the surface passivating ligand from carboxylic acid containing myristic acid (MA) to tetradecylphosphonic acid (TDPA) we observed a >100 nm blue shift in the LSPR response. Using Fourier transform infrared (FTIR) and Raman spectroscopies in conjunction with DFT calculated Raman spectra we were able to conclude this shift was due to the formation of tridentate phosphonate bonds on the NPLs surface. Phosphonate bonding allows for an increase in surface passivation per ligand decreasing surface trapped electrons. These previously trapped electrons were then able to participate as free electrons in the LSPR response. Electron paramagnetic spectroscopy (EPR) further supported this decrease in surface traps through a decrease and shift of the EPR signal related to metal oxide surface trapped electrons.
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