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Incorporation of Catalytic Modalitie...

Perry, Albert, III.

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Incorporation of Catalytic Modalities for Forming of a Catalytic Cascade.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Incorporation of Catalytic Modalities for Forming of a Catalytic Cascade./
作者:	Perry, Albert, III.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2017,
面頁冊數:	137 p.
附註:	Source: Dissertation Abstracts International, Volume: 79-08(E), Section: B.
Contained By:	Dissertation Abstracts International79-08B(E).
標題:	Engineering. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10640361
ISBN:	9780355818383

Incorporation of Catalytic Modalities for Forming of a Catalytic Cascade.
Perry, Albert, III.

Incorporation of Catalytic Modalities for Forming of a Catalytic Cascade. - Ann Arbor : ProQuest Dissertations & Theses, 2017 - 137 p.

Source: Dissertation Abstracts International, Volume: 79-08(E), Section: B.

Thesis (Ph.D.)--The University of New Mexico, 2017.

As climate change progresses, the temperature on Earth is continuing to rise. According to the International Panel on Climate Change, the average temperature on Earth will increase by several degrees Celsius by the end of this century, which can lead to inhospitable temperature, decline in oceanic environments as well as increasingly severe weather. This increase is mainly anthropogenic due to our continual, exponential release of CO 2 by the utilization of traditional fuels. Thus, there is an ever-pressing need to develop alternative energy sources.

ISBN: 9780355818383Subjects--Topical Terms:

586835
Engineering.

Incorporation of Catalytic Modalities for Forming of a Catalytic Cascade.
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245 1 0 $a Incorporation of Catalytic Modalities for Forming of a Catalytic Cascade.
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300 $a 137 p.
500 $a Source: Dissertation Abstracts International, Volume: 79-08(E), Section: B.
500 $a Adviser: Plamen Atanassov.
502 $a Thesis (Ph.D.)--The University of New Mexico, 2017.
520 $a As climate change progresses, the temperature on Earth is continuing to rise. According to the International Panel on Climate Change, the average temperature on Earth will increase by several degrees Celsius by the end of this century, which can lead to inhospitable temperature, decline in oceanic environments as well as increasingly severe weather. This increase is mainly anthropogenic due to our continual, exponential release of CO 2 by the utilization of traditional fuels. Thus, there is an ever-pressing need to develop alternative energy sources.
520 $a While there is significant attention on large-scale energy production, small-scale energy sources also need to be considered. To address this, we need to further develop techniques that efficiently and completely extract energy through oxidation of given substrate by harvesting electrons at each step of the process. Efficient oxidation of a substrate has been demonstrated by nature through metabolons, such as those found in the TCA cycle. By observing these metabolons, it has been shown that intermediates are guided from one catalytic site to another in what has been termed substrate channeling. Building on this, there is an interest in replicating metabolons and substrate channeling utilizing different catalyst types, such as inorganic, enzymatic, and molecular catalysts. Each of these catalysts offers their own benefits, such as the ability to function in extreme conditions, selectively targeting a substrate, or having predictable redox mechanisms. To further research the incorporation of these modalities into a cascade reaction, this dissertation explores several inorganic catalysts for the sequential oxidation of organic substrates. Specifically, exploring how a biomimetic catalyst (Mn-aminoantipyrene), Pt and Pt alloys, as well as Pd combined with a Mn-N-C catalyst oxidize intermediates in the glycerol oxidation cascade.
520 $a The MnAAPyr catalyst, designed to mimic the reactive centers of oxalate decarboxylase (OxDC) and oxalate oxidase (OxOx) showed high activity towards the oxidation of oxalic acid with onset potentials of 0.714 +/- 0.002 V vs. SHE at pH = 4. OxOx and OxDC are Mn containing enzymes, in which Mn is surrounded by nitrogen atoms in the form of histidines. As such, MnAAPyr was synthesized utilizing the Sacrificial Support Method developed at the University of New Mexico and is shown to be a nano-structured material in which Mn is atomically dispersed on a nitrogendoped graphene matrix.
520 $a Pt, PtSn (1:1), PtSn (19:1), PtRu (1:4), PtRuSn (5:4:1), and PtRhSn (3:1:4), were also synthetized using the Sacrificial Support Method and tested for oxidation of oxalic acid at pH 4. PtSn (1:1) and PtRu (1:4) showed higher mass activity than Pt and the other alloys. These two, along with one of the worst performing catalysts, PtSn (19:1), were further analyzed for oxidation of oxalic acid at different pHs and concentrations. The results of these measurements showed the same increase in catalytic activity with decreased pH and a decrease in onset potential at more alkaline conditions. PtSn (19:1), PtSn (1:1), and PtRu (1:4) also showed a positive linear dependence of the generated current as a function of the concentration of oxalic acid.
520 $a Literature has shown that Pt is very susceptible to CO poisoning when oxidizing formic acid. As such, other more resistant, inorganic catalysts must be considered. A Pd and Mn-N-C hybrid catalyst (Pd/Mn-N-3D-GNS) were tested for the oxidation of glycerol intermediates: glyoxalic acid, mesoxalic acid, oxalic acid, and formic acid. The measurements show that when compared to Pd and Mn-N-C separately, Pd/Mn-N-3D-GNS showed a decreased onset potential towards the oxidation of mesoxalic acid. The hybrid catalyst also showed increased maximum currents from the oxidation of oxalic acid when compared to Pd and Mn-N-C. It is also shown that Pd and Mn-N-C oxidize formic acid differently. Pd oxidizes formic acid via dehydrogenation pathway, while Mn-N-C oxidizes via the less desired dehydration pathway.
520 $a Developing from the knowledge we have gained through the study of inorganic catalysts, Pd was selected to be incorporated with an enzymatic catalyst (OxDC) for a two-step cascade. Within this cascade, OxDC oxidizes oxalic acid to formic acid, which is then oxidized to carbon dioxide by Pd. To ensure co-localization, OxDC is immobilized onto a macro-porous graphene support by 1-pyrenebutanoic acid succinimidyl ester (PBSE). A novel deposition technique was developed to co-localize these catalysts and tested utilizing UV-VIS and electrochemical measurements.
590 $a School code: 0142.
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