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Proton-coupled electron transfer rea...

Fernandez, Laura E.

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Proton-coupled electron transfer reactions: Electrochemical method development and applications.

Record Type:	Language materials, printed : Monograph/item
Title/Author:	Proton-coupled electron transfer reactions: Electrochemical method development and applications./
Author:	Fernandez, Laura E.
Description:	266 p.
Notes:	Source: Dissertation Abstracts International, Volume: 74-12(E), Section: B.
Contained By:	Dissertation Abstracts International74-12B(E).
Subject:	Chemistry, General. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3573774
ISBN:	9781303451058

Proton-coupled electron transfer reactions: Electrochemical method development and applications.
Fernandez, Laura E.

Proton-coupled electron transfer reactions: Electrochemical method development and applications. - 266 p.

Source: Dissertation Abstracts International, Volume: 74-12(E), Section: B.

Thesis (Ph.D.)--The Pennsylvania State University, 2013.

Proton-coupled electron transfer (PCET) reactions involve the transfer of single or multiple electrons and protons in sequential or concerted fashion. PCET reactions are important in biological systems such as photosynthesis and respirations, and in chemical systems, such as electrochemistry and catalysis. The applications studied here are relevant to systems such as artificial photosynthesis and water-splitting devices. Of central importance to PCET reactions is the donor-acceptor distance and effective frequency. The first application, which models proton relays that occur in fuel cells, artificial photosynthesis and enzyme reactions, illustrates the importance of the donor-acceptor distance in the case of a single and a double proton transfer. In the second application, we investigate electrocatalysts inspired by hydrogenase enzymes, which oxidize and produce H2 in nature. In this application, which is relevant to water-splitting devices, we looked into whether a sequential or concerted mechanism was more preferable for nickel-based catalysts with pendant amines. We then continued this investigation to find faster catalysts for H2 oxidation and H2 reduction using more flexible amines with nickel centers. From these studies of PCET reactions, we found that theoretical investigations can aid in the analysis of experimental results and provide predictions for future experiments and in some cases help to reanalyze experimental interpretation.

ISBN: 9781303451058Subjects--Topical Terms:

1021807
Chemistry, General.

Proton-coupled electron transfer reactions: Electrochemical method development and applications.
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245 1 0 $a Proton-coupled electron transfer reactions: Electrochemical method development and applications.
300 $a 266 p.
500 $a Source: Dissertation Abstracts International, Volume: 74-12(E), Section: B.
500 $a Adviser: Sharon Hamines-Schiffer.
502 $a Thesis (Ph.D.)--The Pennsylvania State University, 2013.
520 $a Proton-coupled electron transfer (PCET) reactions involve the transfer of single or multiple electrons and protons in sequential or concerted fashion. PCET reactions are important in biological systems such as photosynthesis and respirations, and in chemical systems, such as electrochemistry and catalysis. The applications studied here are relevant to systems such as artificial photosynthesis and water-splitting devices. Of central importance to PCET reactions is the donor-acceptor distance and effective frequency. The first application, which models proton relays that occur in fuel cells, artificial photosynthesis and enzyme reactions, illustrates the importance of the donor-acceptor distance in the case of a single and a double proton transfer. In the second application, we investigate electrocatalysts inspired by hydrogenase enzymes, which oxidize and produce H2 in nature. In this application, which is relevant to water-splitting devices, we looked into whether a sequential or concerted mechanism was more preferable for nickel-based catalysts with pendant amines. We then continued this investigation to find faster catalysts for H2 oxidation and H2 reduction using more flexible amines with nickel centers. From these studies of PCET reactions, we found that theoretical investigations can aid in the analysis of experimental results and provide predictions for future experiments and in some cases help to reanalyze experimental interpretation.
590 $a School code: 0176.
650 4 $a Chemistry, General. $3 1021807
650 4 $a Chemistry, Physical. $3 560527
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710 2 $a The Pennsylvania State University. $b Chemistry. $3 2094196
773 0 $t Dissertation Abstracts International $g 74-12B(E).
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793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3573774