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Studies of Colloidal Iron Carbide Nanoparticle Fischer-Tropsch Catalysts : = Characterizing Adsorption Sites and Reactivity Towards Hydrogen Atom Transfers.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Studies of Colloidal Iron Carbide Nanoparticle Fischer-Tropsch Catalysts :/
其他題名:	Characterizing Adsorption Sites and Reactivity Towards Hydrogen Atom Transfers.
作者:	Dwarica, Nicolas S.
面頁冊數:	1 online resource (139 pages)
附註:	Source: Dissertations Abstracts International, Volume: 85-01, Section: B.
Contained By:	Dissertations Abstracts International85-01B.
標題:	Inorganic chemistry. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=29397325click for full text (PQDT)
ISBN:	9798379780876

Studies of Colloidal Iron Carbide Nanoparticle Fischer-Tropsch Catalysts : = Characterizing Adsorption Sites and Reactivity Towards Hydrogen Atom Transfers.
Dwarica, Nicolas S.

Studies of Colloidal Iron Carbide Nanoparticle Fischer-Tropsch Catalysts :Characterizing Adsorption Sites and Reactivity Towards Hydrogen Atom Transfers. - 1 online resource (139 pages)

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

Thesis (Ph.D.)--Yale University, 2023.

Includes bibliographical references

Iron carbide catalysts have been used for nearly 100 years in the Fischer-Tropsch process (FTP), yet the atomic nature of the active site(s) for H2 and CO have not been fully characterized. The FTP has recently gained interest as a method for the sustainable production of aviation fuels; however, this process suffers from limited product selectivity. A better understanding of the active site(s) could allow for more rational design of iron carbide catalysts, where changes in active site structure(s) could be correlated with catalyst activity. Here, we present the synthesis, characterization, and catalysis by a well-defined dodecylamine-capped colloidal iron carbide (DDA-FexC) nanoparticle (NP) system. This colloidal NP system is amenable to solution phase reactivity studies, spectroscopic measurements, and catalysis towards olefin hydrogenation and carbon monoxide hydrogenation at mild conditions. The tandem use of x-ray and FTIR spectroscopies along with density functional theory (DFT) calculations and molecular dynamic simulations enabled the identification of the structures of adsorbed hydrogen (Hads) and carbon monoxide (COads) over these DDA-FexC NPs. 57Fe Nuclear resonant vibrational spectroscopy revealed a Fe-C vibration for COads consistent with terminally bound CO, as supported by DFT calculations. FTIR revealed a distribution of *C-D vibrations for NPs treated with D2, consistent with adsorption over surface carbide sites supported by DFT calculations. Extended x-ray absorption fine structure (EXAFS) measurements of DDA-FexC NPs treated with H2 and CO showed measurable increases in Fe-Fe and Fe-C bond lengths that varied with coverage. The experimentally measured vibrational energies are used to validate the active site structures generated by DFT calculations and molecular dynamics. These results demonstrate the powerful combination of experiment and theory to better understand an elusive catalytic system and may aid in the rational development of future iron carbide catalysts.

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

Mode of access: World Wide Web

ISBN: 9798379780876Subjects--Topical Terms:

3173556
Inorganic chemistry.
Subjects--Index Terms:

ColloidalIndex Terms--Genre/Form:

542853
Electronic books.

Studies of Colloidal Iron Carbide Nanoparticle Fischer-Tropsch Catalysts : = Characterizing Adsorption Sites and Reactivity Towards Hydrogen Atom Transfers.
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