東華大學圖書館 |

語系: 繁體中文

說明(常見問題)

回圖書館首頁

手機版館藏查詢

登入

回首頁

切換: 標籤 | MARC模式 | ISBD

Experimental and Computational Studi...

Mendez-Hernandez, Dalvin D.

FindBook

Google Book

Amazon

博客來

Experimental and Computational Studies on the Design of Dyes for Water-splitting Dye-sensitized Photoelectrochemical Tandem Cells.

紀錄類型:	書目-語言資料,印刷品 : Monograph/item
正題名/作者:	Experimental and Computational Studies on the Design of Dyes for Water-splitting Dye-sensitized Photoelectrochemical Tandem Cells./
作者:	Mendez-Hernandez, Dalvin D.
面頁冊數:	124 p.
附註:	Source: Dissertation Abstracts International, Volume: 75-08(E), Section: B.
Contained By:	Dissertation Abstracts International75-08B(E).
標題:	Chemistry, General. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3619696
ISBN:	9781303891380

Experimental and Computational Studies on the Design of Dyes for Water-splitting Dye-sensitized Photoelectrochemical Tandem Cells.
Mendez-Hernandez, Dalvin D.

Experimental and Computational Studies on the Design of Dyes for Water-splitting Dye-sensitized Photoelectrochemical Tandem Cells. - 124 p.

Source: Dissertation Abstracts International, Volume: 75-08(E), Section: B.

Thesis (Ph.D.)--Arizona State University, 2014.

Solar energy is a promising alternative for addressing the world's current and future energy requirements in a sustainable way. Because solar irradiation is intermittent, it is necessary to store this energy in the form of a fuel so it can be used when required. The light-driven splitting of water into oxygen and hydrogen (a useful chemical fuel) is a fascinating theoretical and experimental challenge that is worth pursuing because the advance of the knowledge that it implies and the availability of water and sunlight. Inspired by natural photosynthesis and building on previous work from our laboratory, this dissertation focuses on the development of water-splitting dye-sensitized photoelectrochemical tandem cells (WSDSPETCs). The design, synthesis, and characterization of high-potential porphyrins and metal-free phthalocyanines with phosphonic anchoring groups are reported. Photocurrents measured for WSDSPETCs made with some of these dyes co-adsorbed with molecular or colloidal catalysts on TiO2 electrodes are reported as well. To guide in the design of new molecules we have used computational quantum chemistry extensively. Linear correlations between calculated frontier molecular orbital energies and redox potentials were built and tested at multiple levels of theory (from semi-empirical methods to density functional theory). Strong correlations (with r2 values > 0.99) with very good predictive abilities (rmsd < 50 mV) were found when using density functional theory (DFT) combined with a continuum solvent model. DFT was also used to aid in the elucidation of the mechanism of the thermal relaxation observed for the charge-separated state of a molecular triad that mimics the photo-induced proton coupled electron transfer of the tyrosine-histidine redox relay in the reaction center of Photosystem II. It was found that the inclusion of explicit solvent molecules, hydrogen bonded to specific sites within the molecular triad, was essential to explain the observed thermal relaxation. These results are relevant for both advancing the knowledge about natural photosynthesis and for the future design of new molecules for WSDSPETCs.

ISBN: 9781303891380Subjects--Topical Terms:

1021807
Chemistry, General.

Experimental and Computational Studies on the Design of Dyes for Water-splitting Dye-sensitized Photoelectrochemical Tandem Cells.
LDR:03148nam a2200301 4500 001 1962615
005 20140819094519.5
008 150210s2014 ||||||||||||||||| ||eng d
020 $a 9781303891380
035 $a (MiAaPQ)AAI3619696
035 $a AAI3619696
040 $a MiAaPQ $c MiAaPQ
100 1 $a Mendez-Hernandez, Dalvin D. $3 2098712
245 1 0 $a Experimental and Computational Studies on the Design of Dyes for Water-splitting Dye-sensitized Photoelectrochemical Tandem Cells.
300 $a 124 p.
500 $a Source: Dissertation Abstracts International, Volume: 75-08(E), Section: B.
500 $a Advisers: Ana L. Moore; Vladimiro Mujica.
502 $a Thesis (Ph.D.)--Arizona State University, 2014.
520 $a Solar energy is a promising alternative for addressing the world's current and future energy requirements in a sustainable way. Because solar irradiation is intermittent, it is necessary to store this energy in the form of a fuel so it can be used when required. The light-driven splitting of water into oxygen and hydrogen (a useful chemical fuel) is a fascinating theoretical and experimental challenge that is worth pursuing because the advance of the knowledge that it implies and the availability of water and sunlight. Inspired by natural photosynthesis and building on previous work from our laboratory, this dissertation focuses on the development of water-splitting dye-sensitized photoelectrochemical tandem cells (WSDSPETCs). The design, synthesis, and characterization of high-potential porphyrins and metal-free phthalocyanines with phosphonic anchoring groups are reported. Photocurrents measured for WSDSPETCs made with some of these dyes co-adsorbed with molecular or colloidal catalysts on TiO2 electrodes are reported as well. To guide in the design of new molecules we have used computational quantum chemistry extensively. Linear correlations between calculated frontier molecular orbital energies and redox potentials were built and tested at multiple levels of theory (from semi-empirical methods to density functional theory). Strong correlations (with r2 values > 0.99) with very good predictive abilities (rmsd < 50 mV) were found when using density functional theory (DFT) combined with a continuum solvent model. DFT was also used to aid in the elucidation of the mechanism of the thermal relaxation observed for the charge-separated state of a molecular triad that mimics the photo-induced proton coupled electron transfer of the tyrosine-histidine redox relay in the reaction center of Photosystem II. It was found that the inclusion of explicit solvent molecules, hydrogen bonded to specific sites within the molecular triad, was essential to explain the observed thermal relaxation. These results are relevant for both advancing the knowledge about natural photosynthesis and for the future design of new molecules for WSDSPETCs.
590 $a School code: 0010.
650 4 $a Chemistry, General. $3 1021807
650 4 $a Energy. $3 876794
650 4 $a Chemistry, Organic. $3 516206
650 4 $a Chemistry, Inorganic. $3 517253
690 $a 0485
690 $a 0791
690 $a 0490
690 $a 0488
710 2 $a Arizona State University. $b Chemistry. $3 2096519
773 0 $t Dissertation Abstracts International $g 75-08B(E).
790 $a 0010
791 $a Ph.D.
792 $a 2014
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3619696